Rapid detection device and method for three-dimensional space and time distribution of defects in materials and devices
By deeply coaxially coupling laser scanning confocal microscopy and ultrafast transient absorption spectroscopy, the problem of rapid detection of the three-dimensional spatial and temporal distribution of defects in materials and devices has been solved, realizing four-dimensional detection with high resolution and high temporal resolution, which is suitable for non-destructive testing of various physical samples and devices.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Filing Date
- 2025-12-22
- Publication Date
- 2026-04-03
AI Technical Summary
Existing technologies struggle to achieve rapid, non-destructive, and high-precision detection of the three-dimensional spatial and temporal distribution of defects in materials and devices, especially in the face of insufficient resolution and long detection times.
By employing laser scanning confocal microscopy and ultrafast transient absorption spectroscopy depth coaxial coupling technology, combined with a laser module, beam splitting module, frequency conversion module, supercontinuum spectrum generation module, optical delay line module, laser scanning confocal microscopy module and data processing unit, four-dimensional spatiotemporal distribution detection of defects in materials and devices can be achieved.
It enables rapid, non-destructive, and high-precision four-dimensional spatiotemporal detection of defects in materials and devices, providing key technical support for material performance optimization and reliability improvement. It also has flexible functional expansion capabilities and is suitable for the detection of samples and devices in different physical states.
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Abstract
Description
Technical Field
[0001] This invention relates to a rapid monitoring method for the four-dimensional spatiotemporal distribution of defects in materials and devices using ultrafast spectroscopy and micro / nano imaging technology. Specifically, it is a device and method for rapid, non-destructive, and high-precision detection of the four-dimensional spatiotemporal distribution of structure, energy level, and defects in materials and devices by deeply coupling ultrafast transient absorption spectroscopy (fs-TA) with confocal laser scanning microscopy (CLSM), belonging to the field of materials testing. Background Technology
[0002] Materials research and development is a core pillar of human civilization's progress, reshaping life and development patterns in all aspects, from basic survival to technological breakthroughs. Materials testing and characterization technology is the "core support" of materials research and development, permeating the entire process and directly determining research efficiency, reliability of results, and industrialization success rate. The distribution of structure, energy levels, and defects in materials and devices directly affects their performance and reliability during research and production. Materials testing technology has significant limitations, primarily including insufficient resolution, long testing times, and the ability to provide only two-dimensional information on the sample surface or cross-section, making it difficult to comprehensively reflect the three-dimensional spatial distribution of defects, thus failing to meet the precise monitoring needs of research and production for the three-dimensional spatial distribution of defects.
[0003] Laser scanning confocal microscopy focuses a laser beam onto a focal plane of a sample, combining this with scanning galvanometer technology. The scanning system performs point-by-point scanning and continuous optical slicing, then collects fluorescence signals from the focal plane using a confocal pinhole, achieving spatially selective excitation and detection. This results in high-resolution three-dimensional (xyz) images of material defects, exhibiting high spatial resolution. Ultrafast transient absorption (UTB) is a pump-probe technique that uses optical pumping pulses to excite the sample to an excited state, followed by probe pulses to monitor the relaxation process as the excited state returns to the ground state. This allows for separate excitation and detection of the sample. Ultrafast UTB offers high temporal resolution (t) and can be used to study the electronic, exciton, and vibrational dynamics of materials after photoexcitation, revealing ultrafast processes such as relaxation, charge transfer, energy transfer, and charge separation in the excited state.
[0004] Laser confocal scanning microscopy excels in high-resolution spatial imaging, providing zero- to three-dimensional images of sample structures and pinpointing the spatial locations of features such as defects or charge carriers. Ultrafast transient absorption spectroscopy, on the other hand, is adept at probing ultrafast dynamic processes, revealing the evolution of excited states in the femtosecond to nanosecond timescales and demonstrating the timing and specific mechanisms of excited-state processes. These two techniques are complementary; their combined use can achieve four-dimensional (xyzt) spatiotemporal detection of defects and energy levels in materials and devices, establishing quantitative correlations between material-device performance and addressing the core problem of existing technologies' inability to simultaneously detect both spatial and temporal dimensions. Summary of the Invention
[0005] This invention provides a rapid detection device and method for the three-dimensional spatial and temporal distribution of defects in materials and devices based on laser scanning confocal microscopy and ultrafast transient absorption spectroscopy depth coaxial coupling technology, providing key technical support for material research and development, performance optimization and reliability improvement.
[0006] A rapid detection device for the three-dimensional spatial and temporal distribution of defects in materials and devices includes core functional modules, specifically comprising: a laser module, a beam splitting module, a frequency conversion module, a supercontinuum spectrum generation module, an optical delay line module, a laser scanning confocal microscope module, a spectral detection module, and a data processing unit.
[0007] The laser module is an ultrafast pulsed laser with adjustable pulse width, repetition rate, and center wavelength. Its output spectrum's center wavelength and laser intensity can be continuously adjusted (10 nm to 30 μm) or fixed, with a frequency adjustment range covering 0.1 to 10 μm. 15 With a time resolution of ≥1 fs, it can synchronously match the ground state absorption band and defect state absorption band of metal, semiconductor and insulator materials and devices, adapt to the dynamic processes of samples in different states such as gas, liquid, solid and plasma, and can completely cover the evolution process of carrier excitation, relaxation, recombination and defect trapping on the full time scale and three-dimensional spatial scale.
[0008] The core function of the beam splitting module is to achieve precise proportional beam splitting, branch switching, and multi-path collaborative adaptation, adapting to the transmission requirements of pump light and probe light under different imaging modes. It includes three independent beam splitting units (beam splitting module 1, beam splitting module 2, and beam splitting module 3). Specifically: beam splitting module 1 is located behind the laser module and splits the fundamental frequency light into two core branches according to a preset ratio. One beam is connected to the frequency conversion module to generate pump light, and the other beam is connected to the optical delay line module to generate probe light. Beam splitting module 2 is connected behind the frequency conversion module, receives the frequency-modulated pump light, and splits it into two paths. One path can be connected in series to the laser scanning confocal microscope module as the incident light source, and the other path is modulated by a chopper to directly irradiate the sample under test. Beam splitting module 3 is connected behind the supercontinuum spectrum generation module, receives the broadband probe light, and splits it into two paths. One path is connected to the laser scanning confocal microscope module as the probe light source, and the other path is connected to the blackbody module to achieve the absorption of redundant beams.
[0009] The frequency conversion module can perform secondary frequency modulation on the fundamental frequency light, with a frequency adjustment range covering 0.1~10. 15 The frequency conversion module adopts a switchable dual-station configuration: a global frequency modulation unit is set before the beam splitting module 1 (corresponding to...). Figure 10 Alternatively, an independent frequency modulation unit can be set up after the beam splitter module 1 (corresponding to...). Figure 11 ).
[0010] The core function of the supercontinuum spectrum generation module is to extend the incident light into a broadband probe light with high coherence and wide wavelength coverage (10 nm to 30 μm).
[0011] The core function of the optical delay line module is to precisely control the optical path length of the probe light branch. By changing the beam transmission path length, the propagation time of the probe light can be precisely adjusted, so that the time difference between the probe light and the pump light reaching the sample under test can be continuously adjusted, with a time resolution of ≥1 fs.
[0012] The laser scanning confocal microscope module can selectively operate independently from the pump-probe branch of the ultrafast transient absorption spectrum, possessing high precision and a wide detection range, and includes three structural forms. When operating independently, it can achieve defect detection relying solely on its own configured light source, optical lens assembly, scanning galvanometer, high-precision stage, and matching spectral detection module. Its depth range (z-axis) is 0~1 m, its lateral range (X / Y-axis) is 0~1 m, and its depth and lateral scanning step accuracy is ≥0.1 nm, with a spatial resolution of ≥0.1 nm, meeting the requirements for large-area, high-precision detection. The three structural forms include: a laser scanning confocal microscope with simultaneous reflection and transmission detection, a laser scanning confocal microscope with reflection detection, and a laser scanning confocal microscope with transmission detection, as detailed below:
[0013] (1) A laser scanning confocal microscope with simultaneous reflection and transmission detection: Its structure includes: a light source, a scanning galvanometer, a dichroic mirror, two sets of optical lens assemblies (optical lens, focusing pinhole and optical lens), a sample, a spectrometer 2 for collecting the reflected light signals PL and TRPL of the sample, and a matching imaging detector 2, as well as a spectrometer 2 for collecting the transmitted light signals PL and TRPL of the sample. The spectrometer 3 and the matching imaging detector 3 are connected as follows: a symmetrical optical path coupling structure for synchronous acquisition of transmission and reflection signals is constructed with the sample under test as the core. A set of "optical lens, focusing pinhole, and optical lens" linkage coupling combination structure is provided on the front and rear sides of the sample, respectively. The outer side of the optical lens assembly on the front side of the sample passes through a dichroic mirror via an optical path and then connects to the PL and TRPL spectrometers 2 and the corresponding imaging detector 2 via a focusing pinhole. The outer side of the optical lens assembly on the rear side of the sample is directly connected to the PL and TRPL spectrometers 3 and the corresponding imaging detector 3 via an optical path. The light source is connected to the dichroic mirror through a scanning galvanometer module. Its working principle is as follows: the light source emits incident light, and the beam deflection is precisely controlled by the scanning galvanometer. After being rotated and reflected by a dichroic mirror, the light is then focused by an optical lens, filtered by a focusing pinhole, and then focused again by another optical lens. By adjusting the lens position or the height of the high-precision stage, the probe light is finally precisely focused on the designated position on the sample. The reflected signal generated after the sample is excited propagates in the reverse direction along the original incident light path, passes through an optical lens, a focusing pinhole, and another optical lens, and then passes through a dichroic mirror before being detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2. The transmitted signal generated after the sample is excited passes through the sample and is transmitted by a combination of optical lenses, a focusing pinhole, and another optical lens behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 for detection and recording, thus achieving synchronous acquisition of reflected and transmitted signals.
[0014] (2) Laser scanning confocal microscope with reflective detection operation: Compared with the first dual detection module, its structure is composed of removing the optical lens assembly, PL and TRPL spectrometers 3 and imaging detector 3 on the back side of the sample, while retaining the other parts as in the first module; Compared with the first dual detection module, its connection method is different in that there is no optical lens, focusing pinhole and optical lens combination structure on the back side of the sample, and there is no PL and TRPL spectrometers 3 and corresponding imaging detector 3, while the other parts are connected to each other as in the first module; Compared with the first dual detection mode, its working mode does not collect the transmission signal generated after the sample is excited, but collects the reflection signal generated after the sample is excited and propagates in the reverse direction along the original incident light path, passing through the optical lens, focusing pinhole and optical lens in sequence, and then passing through the dichroic mirror and being detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detector 2.
[0015] (3) Laser scanning confocal microscope with transmission detection operation: Compared with the first dual detection module, its structure is composed of removing the optical lens assembly, dichroic mirror, PL and TRPL spectrometers 2 and imaging detector 2 on the front side of the sample, while retaining the other parts as in the first module; Compared with the first dual detection module, its connection method is different in that there is no optical lens, focusing pinhole and optical lens combination structure on the front side of the sample, no dichroic mirror, and no PL and TRPL spectrometers 2 and corresponding imaging detectors 2, while the other parts are connected in the same way as the first module; Compared with the first dual detection mode, its working mode does not collect the reflection signal generated after the sample is excited, but collects the transmission signal generated after the sample is excited. The transmission signal generated after the sample is excited passes through the sample and is transmitted by the optical lens, focusing pinhole and optical lens combination behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 to complete the detection and recording, thereby realizing the acquisition of transmission signal.
[0016] The spectral detection module has a detection range of 100 nm to 1000 μm and includes multiple spectrometers and matching imaging detectors. It is functionally divided to accurately acquire differential absorption signals and fluorescence / infrared / Raman signals, meeting the detection requirements of different operating modes of the device. The specific configuration includes: (1) a TA spectrometer 1 and its corresponding imaging detector 1, whose core function is to receive and record the differential absorption signal of the sample after the detection light passes through the sample under two conditions: pump light excitation and no pump light excitation; (2) a reflective PL and TRPL spectrometer 2 and its imaging detector 2, focusing on signal acquisition along the reflection path; and (3) a transmission PL and TRPL spectrometer 3 and its imaging detector 3, focusing on signal acquisition along the transmission path. The two sets of PL and TRPL spectrometers and their corresponding imaging detector units are used together to receive and record the fluorescence, infrared, and Raman signals generated after the sample is excited by the focused beam, meeting the signal detection requirements of the device under different operating modes.
[0017] The data processing unit is electrically connected to imaging detector 1, imaging detector 2, and imaging detector 3, respectively, and collects signals in the data processing unit. It extracts the spatial coordinates and temporal dynamic evolution information of the material from the four-dimensional data. Through data conversion and analysis, it obtains information on the material's structure and composition, energy levels, charge carriers, optical information, electronic and lattice vibrations, and macroscopic physical information, as detailed below:
[0018] (1) Structural and compositional information: Structural and compositional information is the basic characterization content for defect detection in materials and devices. Its core purpose is to clarify the spatial distribution of defects and the essential composition of materials. It includes structural defects, as well as the composition, valence state, and free radicals of materials. Among them, structural defects are directly obtained by the three-dimensional scanning signal of the laser scanning confocal microscope module. The defect location in the three-dimensional space of xyz is accurately located by utilizing the difference in PL and TRPL intensity between the defect area and the normal area, and the difference in relaxation rate of the TA differential absorption signal. The composition of materials needs to be indirectly calculated by matching with the characteristic emission peak of the PL spectrum, the characteristic scattering peak of the Raman spectrum, or the characteristic absorption peak of the infrared spectrum with the industry standard spectral library. The valence state of elements is derived by the Raman peak shift and the splitting phenomenon of the infrared absorption peak. It is obtained by combining quantum chemical calculation and analysis with the difference in chemical bond vibration frequency caused by the change of valence state. Free radicals are identified by the absorption peak of characteristic functional groups in the infrared spectrum and their type is determined by the spectral analysis.
[0019] (2) Energy level information: Energy level information focuses on the characterization of the electronic energy state of materials and devices, with the core being the accurate identification of energy level defects and the quantification of related energy parameters. This includes energy level defects (including deep and shallow energy level defects), band gap, Fermi level, electronic density of states, and energy level position. Among them, the energy level defects (including deep and shallow energy level defects) are calculated by combining the relaxation time of the TA signal and TRPL fluorescence lifetime data with the band gap formula. Shallow energy level defects correspond to short relaxation times in the picosecond range, while deep energy level defects correspond to long relaxation times in the nanosecond range. The band gap is directly calculated by reading the PL emission peak. The Fermi level is calculated by combining the TA absorption edge analysis with the formula. The electronic density of states is derived from the TA spectral absorption coefficient distribution based on the Kramers-Kronig relationship. The energy level position is determined by converting the valence band top and conduction band bottom energies with the defect energy level offset.
[0020] (3) Carrier Information: Carrier information revolves around the motion characteristics and mechanisms of carriers such as electrons and holes in materials, with the core being the identification of carrier recombination centers and the determination of key dynamic parameters. This includes carrier recombination centers, as well as carrier lifetime, carrier concentration, carrier mobility, and carrier mean free path. Among these, carrier recombination centers (associated with structural defects and energy level defects) are indirectly determined through multi-exponential fitting of TRPL decay curves, with different decay time constants corresponding to different types of recombination centers. Carrier lifetime is obtained by fitting TRPL single-exponential or multi-exponential decay curves and extracting characteristic decay times. Carrier concentration is calculated from the intensity of the TA differential absorption signal. Carrier mobility is obtained by calculating the diffusion coefficient using the carrier diffusion distance. The carrier mean free path is indirectly calculated based on carrier mobility and thermal velocity.
[0021] (4) Optical Information: Optical information mainly characterizes the absorption, emission, and response characteristics of materials and devices to light, directly reflecting the light-to-conversion potential and optical performance of the materials. This includes the fluorescence absorption, fluorescence emission, variable excitation characteristics, and carrier recombination efficiency of the materials. Among them, the fluorescence absorption and emission characteristics are directly obtained through PL spectroscopy. By reading the absorption peak, emission peak position (wavelength), and peak intensity in the spectrum, the optical response range and luminescence characteristics of the materials can be determined. Variable excitation characteristics are obtained through direct testing. By adjusting the excitation power and repetition frequency of the laser module, the PL intensity change curves under different conditions are recorded, and its linear growth or saturation characteristics are analyzed. The carrier recombination efficiency is calculated by the correlation formula between PL quantum yield and fluorescence lifetime, or by the ratio of calibrated PL intensity to excitation light intensity.
[0022] (5) Electronic and lattice vibration information: Electronic and lattice vibration information focuses on the characterization of the microscopic motion state of materials, with the core being the analysis of phonon distribution and electron spin characteristics. This includes the phonon distribution and electron spin of the material; the phonon distribution state is directly obtained through Raman spectroscopy, and the distribution of phonons is determined by reading the characteristic peak intensity ratio of different phonon modes in the Raman spectrum; the electron spin characteristics are based on the spin splitting signal of the Raman peak or the spin relaxation time of the TA signal, and the electron spin state can be analyzed by combining quantum mechanical models.
[0023] (6) Macroscopic physical information: Macroscopic physical information characterizes the overall physical properties of materials and devices, and is directly related to their performance and reliability in practical application scenarios. This includes properties such as the material's work function, temperature field, dielectric constant, polarization characteristics, and conductivity. Specifically, the temperature field distribution is directly obtained through the infrared spectroscopy module. Based on the infrared signal intensity distribution, the three-dimensional temperature distribution of the sample is directly mapped using the fourth power relationship between blackbody radiation intensity and temperature. The work function is derived from the maximum kinetic energy of photoelectrons combined with the photon energy of the laser. The dielectric constant is derived from the refractive index change derived from the TA signal. The polarization characteristics are calculated by converting the polarization-induced absorption change with the calibration curve. The conductivity is derived from carrier concentration and mobility based on Ohm's law.
[0024] The overall optical path connection sequence of the rapid detection device is as follows: The optical path after the laser module outputs light is connected to beam splitting module 1. Beam splitting module 1 can split into two beams. The optical path after one beam is connected to a frequency conversion module, which generates pump light after frequency adjustment. The pump light generated after the frequency conversion module is connected to beam splitting module 2. The optical path after the other beam from beam splitting module 1 is connected to an optical delay line module. The optical path after the optical delay line module is connected to a supercontinuum spectrum generation module, allowing the other beam from beam splitting module 1 to change its optical path and generate broadband probe light through the supercontinuum spectrum generation module. The broadband probe light generated after the supercontinuum spectrum generation module is connected to beam splitting module 3. The output light from beam splitting module 3 can be split into two beam paths. The optical path after one beam path... The optical path is connected to the blackbody module, and the optical path following the other optical path is connected to the laser scanning confocal microscope module, which can be used as the light source for the laser scanning confocal microscope module. That is, the probe light branch enters the laser scanning confocal microscope module through the beam splitter module 3 as a light source or is absorbed by the blackbody. The output light from the beam splitter module 2 can be divided into two optical paths. The optical path following one optical path is connected to the laser scanning confocal microscope module, which can also be used as the light source for the laser scanning confocal microscope module. The optical path following the other optical path is connected to the chopper and the sample to be tested in the laser scanning confocal microscope module in sequence. That is, the output light from the beam splitter module 2 enters the laser scanning confocal microscope module as a light source for the laser scanning confocal microscope module, or directly illuminates the sample to be tested through the chopper.
[0025] The rapid detection device of the present invention possesses flexible functional expansion capabilities, and can be further integrated with an infrared spectroscopy module and a Raman spectroscopy module. This architecture supports synchronous or time-division acquisition of transient absorption signals, infrared absorption signals, and Raman scattering signals. The laser module's wide wavelength range of 10 nm to 30 μm is compatible with the spectral detection module's high sensitivity response of 100 nm to 1000 μm, covering both the mid-infrared to far-infrared band required for infrared spectroscopy and matching the precise capture requirements of Raman spectroscopy for characteristic scattering peaks.
[0026] A rapid detection method for the three-dimensional spatial and temporal distribution of defects in materials and devices based on laser scanning confocal microscopy and ultrafast transient absorption spectroscopy depth coaxial coupling technology is a multimodal testing method with core functions, specifically including: (1) a rapid detection method based on a laser scanning confocal microscopy and ultrafast transient absorption integrated system with synchronous operation of reflective and transmissive detection, including TA imaging mode and PL and TRPL imaging modes; (2) a rapid detection method based on a laser scanning confocal microscopy and ultrafast transient absorption integrated system with reflective detection operation, including TA imaging mode and PL and TRPL imaging modes; (3) a rapid detection method based on a laser scanning confocal microscopy and ultrafast transient absorption integrated system with quasi-transmissive detection operation, including TA imaging mode and PL and TRPL imaging modes, as follows:
[0027] (1) A method for rapid detection using a laser scanning confocal microscope that integrates reflective and transmissive detection with an ultrafast transient absorption system, which is divided into two imaging modes:
[0028] The first type of TA imaging mode specifically includes the following steps (corresponding to...) Figure 2 ):
[0029] S1: Start the laser module and output fundamental frequency light. Based on the characteristics of the ground state absorption band and defect state absorption band of the sample under test, precisely adjust the pulse width, repetition frequency and center wavelength to ensure that the laser can effectively excite the sample to generate defect-correlated excited states.
[0030] S2: The fundamental frequency beam is split into two beams by the beam splitting module 1 according to a preset ratio. One beam is sent to the frequency conversion module for secondary frequency modulation and then used as pump light. The other beam enters the optical delay line module. The time difference between the beam and the pump light is adjusted by precisely controlling the optical path difference. Then, the broadband probe light is generated by the supercontinuum spectrum generation module.
[0031] S3: The pump light is selected by the beam splitting module 2 and periodically modulated by the chopper before directly irradiating the designated area of the sample to be tested, so that the pump light alternately irradiates the sample at a fixed frequency, forming a periodic state switching of "excited-unexcited".
[0032] S4: The probe light is selected and connected to the laser scanning confocal microscope module via the beam splitter module 3 as the incident light source; the beam deflection angle is precisely controlled by the scanning galvanometer to achieve point-by-point scanning of the target area in the xy plane of the sample; after being reflected by the dichroic mirror, it is then converged by the optical lens, filtered by the focusing pinhole to remove stray light, and then converged again by the optical lens, finally precisely focusing the probe light on the sample surface and different depth positions inside; by adjusting the lens position or the height of the high-precision stage, continuous focusing in the sample depth direction (z) is achieved, completing point-by-point coverage in three-dimensional space;
[0033] S5: The focused probe light and pump light are precisely superimposed at a designated position on the sample. The pump light periodically excites the sample in time through a chopper, causing ground-state carriers to absorb photon energy (electrons and holes) and transition from the ground state to the excited / defect state, thus changing the energy state of the sample. The probe light continuously changes its path length through the optical delay line module, realizing a full-time domain scan of the probe light relative to the arrival time of the pump light (covering the entire process of carrier excitation, defect trapping, and recombination). Broadband light is generated through the supercontinuum spectroscopy generation module. When it acts on the sample, it is selectively absorbed by the excited / defect state carriers in the sample by the pump light, carrying the state information of the sample and completely capturing the dynamic process of the interaction between carriers and defects in the time dimension (t).
[0034] S6: The TA spectrometer and imaging detector 1 simultaneously acquire the differential absorption signal of the probe light (reflection / transmission) after the sample is subjected to the "pump light excited state" and "no pump light ground state". This signal directly reflects the concentration of charge carriers (electrons and holes) in the excited state of the sample at different time points (t). By completely recording the temporal differential signal of each pixel in the xyz three-dimensional space, a four-dimensional dataset containing "spatial three-dimensional (xyz) + temporal one-dimensional (t)" is finally constructed to realize the synchronous characterization of the spatial distribution and temporal evolution of defects.
[0035] The second type of PL and TRPL imaging modes specifically includes the following steps (corresponding to...) Figure 3 ):
[0036] S1: Start the laser module and output fundamental frequency light. Based on the characteristics of the ground state absorption band and defect state absorption band of the sample under test, precisely adjust the pulse width, repetition frequency and center wavelength to ensure that the laser can effectively excite the sample to generate defect-correlated excited states.
[0037] S2: The fundamental frequency beam is split into two beams by the beam splitting module 1. One beam is frequency-modulated by the frequency conversion module and used as pump light. The other beam enters the optical delay line module to control the time difference with the pump light, and then the probe light is generated by the supercontinuum spectrum generation module.
[0038] S3: The pump light is selected and connected to the laser scanning confocal microscope module via the beam splitter module 2 as the incident light source; the beam deflection angle is adjusted by the scanning galvanometer to achieve point-by-point scanning of the target area of the sample in the xy plane; after being reflected by the dichroic mirror, it is then focused onto the target area of the sample in the xy plane after being converged by the optical lens and filtered by the focusing pinhole; by adjusting the lens position or the height of the high-precision stage, precise focusing in the depth direction (z) of the sample is achieved, completing point-by-point coverage in three-dimensional space;
[0039] S4: The fluorescence, infrared, and Raman signals generated after the sample is excited propagate in the reverse direction along the original incident light path, passing through an optical lens, a focusing pinhole, and another optical lens in sequence, before passing through a dichroic mirror and being detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2; the transmitted signals pass through the sample and are transmitted by a combination of optical lenses, a focusing pinhole, and another optical lens behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 for detection and recording. The two sets of detection units synchronously collect signals and signal attenuation to construct a zero-to-three-dimensional (xyz) dataset.
[0040] (2) The second type of reflective detection method uses a laser scanning confocal microscope and an ultrafast transient absorption integrated system for rapid detection, which is divided into two imaging modes:
[0041] The first type of TA imaging method specifically includes the following steps (corresponding to...) Figure 5 ):
[0042] S1 to S6: Steps S1 to S6 of the TA imaging mode are completely consistent with those of the first type of transmission / reflection dual-detection structure.
[0043] The second PL and TRPL imaging method specifically includes the following steps (corresponding to...) Figure 6 ):
[0044] S1 to S3: Steps S1 to S3 of the PL and TRPL imaging modes of the first type of transmission / reflection dual-detection structure are completely consistent.
[0045] S4: After the sample is excited, it only produces fluorescence, infrared and Raman signals in the reflection direction. The signal propagates in the reverse direction along the original incident light path, passes through the optical lens, focusing pinhole and optical lens in sequence, and then passes through the dichroic mirror. The PL and TRPL spectrometers 2 and their corresponding imaging detectors 2 complete the detection and recording. By collecting the reflected signal and the signal attenuation, a zero-to-three-dimensional (xyz) dataset is constructed.
[0046] (3) The third type of transmission detection method uses a laser scanning confocal microscope and an ultrafast transient absorption integrated system for rapid detection, which is divided into two imaging modes:
[0047] The first type of TA imaging method specifically includes the following steps (corresponding to...) Figure 8 ):
[0048] S1 to S6: Steps S1 to S6 of the TA imaging mode are completely consistent with those of the first type of transmission / reflection dual-detection structure.
[0049] The second PL and TRPL imaging method specifically includes the following steps (corresponding to...) Figure 9 ):
[0050] S1-S3: Steps S1-S3 of the PL and TRPL imaging modes of the first type of transmission / reflection dual-detection structure are completely consistent.
[0051] S4: After the sample is excited, it only produces fluorescence, infrared and Raman signals in the transmission direction. After passing through the sample, the signal is transmitted to the PL and TRPL spectrometers 3 and imaging detector 3 through the optical lens, focusing pinhole and optical lens combination behind the sample to complete the detection and recording (no reflection signal acquisition); by collecting the transmission signal and signal attenuation, a zero to three-dimensional (xyz) dataset is constructed.
[0052] The PL and TRPL imaging methods protected by this invention can be deeply coupled with ultrafast transient absorption spectroscopy to achieve four-dimensional (xyzt) spatiotemporal detection, or they can be implemented independently using only a laser scanning confocal microscope module to obtain zero- to three-dimensional distribution information of material defects. When the laser scanning confocal microscope module can operate independently of the pump-detector branch of the ultrafast transient absorption spectroscopy, it can also achieve four sub-modes of zero-dimensional to two-dimensional photoluminescence (0D to 2D PL), three-dimensional photoluminescence (3D PL), zero-dimensional to two-dimensional time-resolved photoluminescence (0D to 2D TRPL), and three-dimensional time-resolved photoluminescence (3D TRPL) using only its own light source, optical lens assembly, scanning galvanometer, high-precision stage, and spectral detection module (PL and TRPL spectrometer 2 and corresponding imaging detector 2, PL and TRPL spectrometer 3 and corresponding imaging detector 3), completing the spatial distribution detection of defects in materials and devices. This independent operation mode falls within the technical scope protected by this invention. Specifically:
[0053] 1. A 0D to 2D PL imaging mode based on confocal microscopy, comprising the following steps:
[0054] S1: Sample and objective configuration: Provide an objective group including at least a low-power objective and a high-power oil immersion objective; when the high-power oil immersion objective is selected, apply immersion oil between the front end of the objective and the sample coverslip to ensure that the sample surface is fully wetted by the immersion oil;
[0055] S2: Excitation light configuration: Turn on the tunable laser source, whose excitation wavelength range covers 10 nm to 30 μm. After selecting the objective lens, adjust the laser wavelength to the optimal excitation wavelength of the target sample.
[0056] S3: Detection optical path configuration: Select the spectrometer and the corresponding imaging detector, and set its receiving wavelength range to the optimal excitation wavelength, specifically, it can be arbitrarily adjusted within the range of 100 nm to 1000 μm;
[0057] S4: Focusing: By controlling the high-precision stage with an accuracy better than 0.1 nm to move along the Z-axis, the positive focal plane is found until the intensity of the detected fluorescence signal reaches a local maximum, and the signal-to-noise ratio is optimized by adjusting the laser power intensity;
[0058] S5: Image acquisition: By adjusting the beam deflection angle with a scanning galvanometer, point-by-point scanning of the target area in the xy plane of the sample is achieved, obtaining the 0D to 2D PL intensity distribution map of the sample.
[0059] 2. A 3D PL imaging method based on confocal microscopy, comprising the following steps:
[0060] S1: Based on the 0D to 2D PL imaging modes of the confocal microscope, S1 to S4, the sample is adjusted to the positive focus position;
[0061] S2: Set the Z-axis range for 3D scanning: By controlling a high-precision stage with an accuracy better than 0.1 nm, move the stage unidirectionally along the Z-axis until the sample is completely out of focus, and mark it as the starting point of the 3D scan in the operation interface; then move the stage in the opposite direction, passing through the positive focus position and continuing to move in the opposite direction to the completely out of focus position, and mark it as the ending point of the 3D scan.
[0062] S3: Set the layer scan parameters: In the 3D settings window, set the number of slices to be collected between the start point and the end point. The Z-axis step size between slices is fixed and adjustable within the range of 0.1 nm to 1 m.
[0063] S4: The fluorescence, infrared, and Raman signals generated after the sample is excited propagate in the reverse direction along the original incident light path, passing through an optical lens, a focusing pinhole, and another optical lens in sequence, before passing through a dichroic mirror and being detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2; the transmitted signals pass through the sample and are transmitted by a combination of optical lenses, a focusing pinhole, and another optical lens behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 for detection and recording. The two sets of detection units synchronously collect signals and signal attenuation to construct a zero-to-three-dimensional (xyz) dataset.
[0064] S4: 3D Image Acquisition: The beam deflection angle is adjusted by the scanning galvanometer to achieve point-by-point scanning of the target area in the xy plane of the sample; by adjusting the lens position or the height of the high-precision stage, the sample depth direction (z) is precisely focused to complete point-by-point coverage in three-dimensional space; the system automatically performs 3D scanning and imaging according to the set number of slices and step size, and synthesizes the images of each layer to obtain the 3D PL distribution map of the sample.
[0065] 3. A 0D to 2D TRPL imaging method based on confocal microscopy, comprising the following steps:
[0066] S1: Based on the 0D to 2D PL imaging modes of the confocal microscope, S1 to S4, the sample is adjusted to the positive focus position;
[0067] S2: Time-resolved parameter settings: Turn on the laser, the excitation wavelength is arbitrarily adjustable within the range of 10 nm to 30 μm, and the repetition frequency is between 0.1 and 10. 15 The frequency can be adjusted arbitrarily within the Hz range, and a suitable repetition frequency can be set according to the sample fluorescence lifetime.
[0068] S3: Image acquisition: The beam deflection angle is adjusted by the scanning galvanometer to achieve point-by-point scanning of the target area of the sample in the xy plane, and the fluorescence decay curve of each pixel is recorded to obtain the 0D to 2D PL fluorescence lifetime distribution map of the sample in the selected area.
[0069] 4. A 3D TRPL imaging method based on confocal microscopy, comprising the following steps:
[0070] S1: Based on the 0D to 2D PL imaging modes of the confocal microscope, S1 to S4, the sample is adjusted to the positive focus position;
[0071] S2: Set the Z-axis range for 3D scanning: Move the high-precision stage with an accuracy better than 0.1 nm along the Z-axis until the sample is completely out of focus, and mark it as the starting point of the 3D scan in the operation interface; then move the stage in the opposite direction, passing through the positive focus position and continuing to move in the opposite direction to the completely out of focus position, and mark it as the ending point of the 3D scan.
[0072] S3: Time resolution parameter settings: In 3D scanning mode, select to switch to a pulsed laser. The excitation wavelength range of the pulsed laser is 10 nm to 30 μm, and the pulse repetition frequency is 0.1~10 μm per trigger. 15 Adjustable within the Hz range, allowing you to set a suitable repetition frequency based on the sample fluorescence lifetime;
[0073] S4: Set the layer scan parameters: In the 3D settings window, set the number of slices to be collected between the start point and the end point. The Z-axis step size between slices is fixed and adjustable within the range of 0.1 nm to 1 m.
[0074] S5: 3D Image Acquisition: The beam deflection angle is adjusted by the scanning galvanometer to achieve point-by-point scanning of the target area in the xy plane of the sample; by adjusting the lens position or the height of the high-precision stage, the sample depth direction (z) is precisely focused to complete point-by-point coverage in three-dimensional space; the system automatically performs 3D scanning according to the set number of slices and step size, records the fluorescence decay curve of each 3D pixel, and finally synthesizes the 3D TRPL distribution map of the sample.
[0075] The materials include one or more of metals, semiconductors, and insulating materials, and their physical states include one or more of gaseous, liquid, solid, and plasma states, as well as heterogeneous materials formed by the combination of the above materials.
[0076] The devices include, but are not limited to, the following types and are adaptable to defect detection under various physical conditions: metal-based devices: metal interconnect structures, metal thin-film sensors; semiconductor-based devices: solar cells, photodetectors, light-emitting diodes, chips; insulator-based devices: dielectric capacitors, insulating coatings, etc. They are suitable for defect distribution detection and performance correlation analysis of the above devices.
[0077] Compared with existing technologies, the rapid monitoring method for the four-dimensional spatiotemporal distribution of defects in materials and devices provided by this invention has the following advantages:
[0078] 1. Full-dimensional characterization: Achieve four-dimensional detection of "three-dimensional space and one-dimensional time", establish quantitative structure-property relationship between defects and device performance, and provide four-dimensional comprehensive characterization of materials through "spatial snapshots" and "temporal snapshots".
[0079] 2. High resolution and fast detection synergy: Combining confocal and super-resolution technologies, it takes into account both nanometer-level spatial resolution and femtosecond-level temporal resolution to meet the needs of large-area, multi-dimensional, high-precision and fast detection.
[0080] 3. Non-destructive testing: It adopts adjustable power ultrafast laser excitation, which avoids thermal damage and maintains the original state of the sample, avoiding the destructive defects of techniques such as electron microscopy. It is especially suitable for guiding material design and process iteration in the research and development stage. Attached Figure Description
[0081] To more clearly illustrate the technical solutions of the embodiments of the present invention, the accompanying drawings used in the embodiments will be briefly introduced below. It should be understood that the following drawings only show some embodiments of the present invention and should not be regarded as a limitation on the scope. For those skilled in the art, other related drawings can be obtained based on these drawings without creative effort.
[0082] Figure 1 This is a schematic diagram of the optical path of a laser scanning confocal microscope and an ultrafast transient absorption integrated system that operates simultaneously with reflective and transmissive detection.
[0083] Figure 2 This is a schematic diagram of the imaging optical path of a laser scanning confocal microscope and an ultrafast transient absorption integrated system that integrates reflective and transmissive detection.
[0084] Figure 3This is a schematic diagram of the optical path of the laser scanning confocal microscope and the ultrafast transient absorption integrated system PL and TRPL, which operate simultaneously with reflective and transmissive detection.
[0085] Figure 4 This is a schematic diagram of the optical path of a laser scanning confocal microscope and an ultrafast transient absorption integrated system operating with reflective detection.
[0086] Figure 5 This is a schematic diagram of the optical path of a laser scanning confocal microscope and an ultrafast transient absorption integrated system (TA) operating with reflective detection.
[0087] Figure 6 This is a schematic diagram of the optical path of the PL and TRPL integrated system of a laser scanning confocal microscope and an ultrafast transient absorption system operating in a reflective detection mode.
[0088] Figure 7 This is a schematic diagram of the optical path of a laser scanning confocal microscope and an ultrafast transient absorption integrated system operating in a transmission detection mode.
[0089] Figure 8 This is a schematic diagram of the optical path of a laser scanning confocal microscope and an ultrafast transient absorption integrated system (TA) operating in transmission detection mode.
[0090] Figure 9 This is a schematic diagram of the optical path of the laser scanning confocal microscope and the ultrafast transient absorption integrated system PL and TRPL, which operate in a transmission detection mode.
[0091] Figure 10 This is a schematic diagram of an independent frequency modulation unit set up in the branch after the beam splitting module 1 in the frequency conversion module.
[0092] Figure 11 This is a schematic diagram of a global frequency modulation unit set up in front of the beam splitter module 1 in the frequency conversion module.
[0093] Figure 12 It is a two-dimensional PL image based on the independent operation mode of the confocal microscope module.
[0094] Figure 13 It is a 3D PL image based on the independent operation mode of the confocal microscope module.
[0095] Figure 14 These are two-dimensional TRPL images based on the independent operation mode of the confocal microscope module.
[0096] Figure 15 These are three-dimensional TRPL images based on the independent operation mode of the confocal microscope module. Detailed Implementation
[0097] The following specific embodiments and accompanying drawings illustrate the implementation of the present invention. Those skilled in the art can easily understand other advantages and effects of the present invention from the content disclosed in this specification. It should be understood that these embodiments are for illustrative purposes only and are not intended to limit the scope of the invention. Furthermore, it should be understood that after reading the teachings of this invention, those skilled in the art can make various modifications or alterations to the invention, and these equivalent forms also fall within the scope defined by the appended claims.
[0098] The present invention generally includes the following steps:
[0099] S1: Construct a coupling detection system, which includes a laser module, a beam splitting module, a frequency conversion module, a probe light generation module, an optical delay line module, a blackbody absorption module, a chopper, a confocal scanning module, a spectral detection module, and a data processing unit;
[0100] S2: Fix the sample on the sample stage, adjust the flatness of the sample stage so that the sample detection surface is parallel to the scanning plane, focus and position the sample through the high numerical aperture objective lens of the confocal scanning module, start the laser source, and split the laser into a pump light branch and a probe light branch through the beam splitting module to ensure that the two beams are coaxially coupled.
[0101] The laser in the S3 pump light branch is focused on the sample to be detected after the energy and frequency parameters are adjusted by the pump light modulation module, exciting the sample to generate carrier excited state or particle active state; the laser in the probe light branch is converted into broadband probe light by the probe light generation module, and after the time delay with the pump light is precisely controlled by the optical delay line, it is focused on the same detection area with the pump light in the same line to avoid spatial displacement error.
[0102] S4: Drives the "scanning galvanometer" and links it with the "focusing pinhole" to focus the light spot, enabling it to scan point-by-point along the sample's xy plane. Simultaneously, by adjusting the objective lens focal length, continuous optical slicing along the z-axis is achieved. The user sets the number of scanning layers along the sample thickness direction (z-axis) and sets the horizontal (x / y-axis) scanning step size and vertical (z-axis) interlayer spacing for each layer. The spectral detection module synchronously acquires the transient absorption signal of each spatial pixel at different time delays, ultimately achieving three-dimensional imaging of defects in the material.
[0103] S5: The data processing unit performs noise reduction, feature extraction, and three-dimensional reconstruction on the acquired signals, generates a 0-3D spatial (xyz) defect distribution map of the sample and corresponding carrier dynamics curves, constructs a four-dimensional (xyzt) spatiotemporal distribution dataset of defects, and combines energy level feature analysis to achieve integrated characterization of structure-energy level-defect. The detection process can achieve real-time or near-real-time measurement.
[0104] Example 1
[0105] This embodiment details the specific implementation method of the TA imaging mode for a laser scanning confocal microscope and an ultrafast transient absorption integrated system that integrates reflection and transmission detection simultaneously. Figure 2 This system enables precise four-dimensional characterization of defects in materials and devices, encompassing three-dimensional space (x, y, z) and one-dimensional time (t). Its core modules include a laser module, beam splitter module, pump light modulation module, probe light generation module, optical delay line module, blackbody absorption module, chopper, confocal scanning module, spectral detection module, and data processing unit. The specific steps are as follows:
[0106] (1) Sample preparation: Select a semiconductor material sample and fix it on a high-precision stage. Adjust the stage to be horizontal to ensure that the sample surface is perpendicular to the optical axis of the objective lens.
[0107] (2) Laser parameter adjustment: Start the laser module and output the fundamental frequency light. According to the characteristics of the ground state absorption band and defect state absorption band of the sample under test, precisely adjust the pulse width, repetition frequency and center wavelength to ensure that the laser can effectively excite the sample to generate defect-related excited states.
[0108] (3) Beam splitting and pump light modulation: The fundamental frequency beam is split into two beams by the beam splitting module 1 at a preset ratio. One beam is sent to the frequency conversion module for secondary frequency modulation and then used as the pump light. The other beam enters the optical delay line module. The time difference between the two beams relative to the pump light and the sample arrival time is adjusted by precisely controlling the optical path difference. Then, the broadband probe light is generated by the supercontinuum spectrum generation module. At the same time, the pump light is selected by the beam splitting module 2 and periodically modulated by the chopper before directly irradiating the designated area of the sample to be tested. The pump light irradiates the sample alternately at a fixed frequency, forming a periodic state switching of "excited-unexcited".
[0109] (4) Probe beam focusing and three-dimensional scanning: After being selected by the beam splitting module 3, the broadband probe beam is connected to the laser scanning confocal microscope module as the incident light source; the beam deflection angle is precisely controlled by the scanning galvanometer to achieve point-by-point scanning of the target area of the sample in the xy plane; after being reflected by the dichroic mirror, it is then converged by the optical lens, filtered by the focusing pinhole to remove stray light, and then converged again by the optical lens, finally accurately focusing the probe beam on the sample surface and different depth positions inside; by adjusting the lens position or the height of the high-precision stage, continuous focusing in the sample depth direction (z) is achieved, and point-by-point coverage of the three-dimensional space is completed;
[0110] (5) Time-domain scanning and signal interaction: The focused probe light and pump light are precisely superimposed at the designated position of the sample. The pump light periodically excites the sample in time through the chopper, causing the ground state carriers to absorb photon energy (electrons and holes) and transition from the ground state to the excited state / defect state, thus causing a change in the energy state of the sample. The probe light continuously changes the probe optical path through the optical delay line module to achieve full time-domain scanning of the probe light relative to the arrival time of the pump light (covering the entire process of carrier excitation, defect trapping, and recombination). Broadband light is generated through the supercontinuum spectroscopy generation module. When it acts on the sample, it is selectively absorbed by the excited state / defect state carriers in the sample by the pump light, carrying the state information of the sample and completely capturing the dynamic process of the interaction between carriers and defects in the time dimension (t).
[0111] (6) Signal acquisition and construction of four-dimensional dataset: TA spectrometer 1 and imaging detector 1 synchronously acquire the differential absorption signal of the probe light (reflection / transmission dual path) after the sample is treated under the conditions of "pump light excited state" and "no pump light ground state"; the signal directly reflects the concentration of charge carriers (electrons and holes) in the excited state of the sample at different time points (t). By completely recording the time domain differential signal of each pixel in the xyz three-dimensional space, a four-dimensional dataset containing three spatial dimensions (xyz) and one temporal dimension (t) is finally constructed to realize the synchronous characterization of the spatial distribution and temporal evolution of defects.
[0112] Example 2
[0113] This embodiment details the specific implementation methods of PL and TRPL imaging modes for a laser scanning confocal microscope and ultrafast transient absorption integrated system that integrates reflection and transmission detection simultaneously. Figure 3 By simultaneously acquiring reflected and transmitted signals along two paths, this method achieves accurate characterization of the three-dimensional (xyz) distribution of defects and carrier dynamics in materials and devices. The core module of the system used in this embodiment is the same as that in Embodiment 1. The specific steps are as follows:
[0114] (1) Sample preparation: Select a semiconductor material sample and fix it on a high-precision stage. Adjust the stage to be horizontal to ensure that the sample surface is perpendicular to the optical axis of the objective lens.
[0115] (2) Laser parameter adjustment: Start the laser module and output the fundamental frequency light. According to the characteristics of the ground state absorption band and defect state absorption band of the sample under test, precisely adjust the pulse width, repetition frequency and center wavelength to ensure that the laser can effectively excite the sample to generate defect-related excited states.
[0116] (3) Beam splitting and pump light focusing: The fundamental frequency beam is split into two beams by the beam splitting module 1. One beam is frequency-modulated by the frequency conversion module and used as the pump light. The other beam enters the optical delay line module to control the time difference with the pump light, and then generates the probe light by the supercontinuum spectrum generation module. At the same time, the pump light is selected by the beam splitting module 2 and connected to the laser scanning confocal microscope module as the incident light source. The beam deflection angle is adjusted by the scanning galvanometer to realize the point-by-point scanning of the target area of the sample in the xy plane. After being reflected by the dichroic mirror, it is focused on the target area of the sample in the xy plane after being converged by the optical lens and filtered by the focusing pinhole. By adjusting the lens position or the height of the high-precision stage, the precise focusing and three-dimensional spatial coverage of the sample in the depth direction are completed.
[0117] (4) Dual-path signal acquisition and dataset construction: After the sample is excited, the fluorescence, infrared and Raman signals generated are reflected and propagated in the reverse direction along the original incident light path. After passing through the optical lens, focusing pinhole and optical lens in sequence, they pass through the dichroic mirror and are detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2. The generated transmission signal passes through the sample and is transmitted by the combination of the optical lens, focusing pinhole and optical lens behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 to complete the detection and recording. The two sets of detection units collect signals and signal attenuation simultaneously to construct a zero-to-three-dimensional (xyz) dataset to realize the correlation characterization between defect spatial distribution and carrier lifetime.
[0118] Example 3
[0119] This embodiment details the specific implementation of the TA imaging mode for a laser scanning confocal microscope and ultrafast transient absorption integrated system operating with reflective detection (corresponding to...). Figure 5 This embodiment achieves accurate four-dimensional characterization of defects in materials and devices, encompassing three-dimensional (xyz) space and one-dimensional (t) time. The core modules of the system used in this embodiment are identical to those in Embodiment 1, with the key difference being the confocal scanning module: only the reflective detection structure is retained, while the optical lens on the back of the sample, the focusing pinhole, the optical lens, the transmission PL and TRPL spectrometers 3, and the imaging detector 3 are removed. The settings and parameters of the remaining modules are the same as in Embodiment 1. The specific steps—laser parameter adjustment, beam splitting and modulation, probe light focusing and three-dimensional scanning, time-domain scanning, and signal acquisition—are completely consistent with Embodiment 1. The difference lies in the signal acquisition: only the differential absorption signal of the probe light is acquired through the reflection path, and a four-dimensional dataset is constructed based on the reflection signal through the data processing unit.
[0120] Example 4
[0121] This embodiment details the specific implementation methods of PL and TRPL imaging modes for a laser scanning confocal microscope and ultrafast transient absorption integrated system operating with reflective detection (corresponding to...). Figure 6 By acquiring reflected signals, this embodiment achieves accurate characterization of the three-dimensional (xyz) distribution of defects and carrier dynamics in materials and devices. The core modules of the system used in this embodiment are the same as those in Embodiment 3. The specific steps of laser parameter adjustment, beam splitting and modulation, probe light focusing and three-dimensional scanning, time-domain scanning and signal acquisition are completely consistent with those in Embodiment 2. The difference lies in the signal acquisition. Only fluorescence, infrared and Raman signals in the reflection direction are acquired after sample excitation to construct a zero-to-three-dimensional (xyz) dataset.
[0122] Example 5
[0123] This embodiment details the specific implementation of the TA imaging mode for a laser scanning confocal microscope and ultrafast transient absorption integrated system operating in transmission-mode detection (corresponding to...). Figure 8 This embodiment achieves accurate four-dimensional characterization of defects in materials and devices, encompassing three-dimensional (xyz) space and one-dimensional (t) time. The core modules of the system used in this embodiment are identical to those in Embodiment 1, with the key difference being the confocal scanning module: the front optical lens, focusing pinhole, optical lens, dichroic mirror, reflective PL and TRPL spectrometers 2, and imaging detector 2 are removed. The settings and parameters of the remaining modules are the same as in Embodiment 1. The specific steps—laser parameter adjustment, beam splitting and modulation, probe light focusing and three-dimensional scanning, time-domain scanning, and signal acquisition—are completely consistent with Embodiment 1. The difference lies in signal acquisition; only the differential absorption signal of the probe light is acquired through the transmission path, and a four-dimensional dataset is constructed based on the transmission signal by the data processing unit.
[0124] Example 6
[0125] This embodiment details the specific implementation methods of PL and TRPL imaging modes for a laser scanning confocal microscope and ultrafast transient absorption integrated system operating with transmission detection (corresponding to...). Figure 9 By acquiring transmission signals, this embodiment achieves accurate characterization of the three-dimensional (xyz) distribution of defects and carrier dynamics in materials and devices. The core modules of the system used in this embodiment are the same as those in Embodiment 5. The specific steps of laser parameter adjustment, beam splitting and modulation, probe light focusing and three-dimensional scanning, time-domain scanning and signal acquisition are completely consistent with those in Embodiment 2. The difference lies in the signal acquisition. Only fluorescence, infrared and Raman signals in the transmission direction are acquired after sample excitation, thus reducing the construction of a zero-to-three-dimensional (xyz) dataset.
[0126] Example 7
[0127] This embodiment provides a method for detecting the spatial distribution of defects using only a laser scanning confocal microscope module. It eliminates the need for a pump-probe branch coupled with ultrafast transient absorption spectroscopy. Through PL and TRP imaging modes, it achieves accurate characterization of the zero- to three-dimensional spatial distribution of defects. This embodiment utilizes only the laser scanning confocal microscope module and its supporting components.
[0128] (1) Zero-to-two-dimensional PL imaging based on laser scanning confocal microscopy:
[0129] The laser scanning confocal microscope module light source is turned on and adjusted to the optimal excitation wavelength of the target sample. The beam deflection angle is controlled by the scanning galvanometer to achieve point-by-point scanning of the target region of the sample in the xy plane. After reflection by the dichroic mirror, the light is then focused onto the target region of the sample in the xy plane after being converged by optical lenses and filtered by a focusing pinhole. By adjusting the lens position or the height of the high-precision stage, the fluorescence, infrared, and Raman signals generated after the sample is excited are reflected and propagated in the reverse direction along the original incident light path. After passing through optical lenses, focusing pinholes, and optical lenses, the light passes through the dichroic mirror and is detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2. The generated transmitted signal passes through the sample and is transmitted by the optical lenses, focusing pinholes, and optical lens combination behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 for detection and recording. The two sets of detection units simultaneously collect signals and signal attenuation to construct a zero-to-three-dimensional (xyz) dataset, thus obtaining the zero-to-two-dimensional photoluminescence intensity distribution map of the sample within a specified range (corresponding to...). Figure 12 ).
[0130] (2) Three-dimensional photoluminescence (PL) imaging method based on laser scanning confocal microscopy: Based on the zero-to-two-dimensional PL imaging settings, a specified depth range to be acquired is selected, and the sample is scanned and photographed layer by layer to finally obtain the three-dimensional photoluminescence intensity distribution map of the sample (corresponding to...). Figure 13 ).
[0131] (3) A zero-to-two-dimensional TRPL imaging method based on laser scanning confocal microscopy: Based on the 2DPL imaging settings, the lens position or high-precision stage height is adjusted to focus to a specified depth of the sample; then, a suitable repetition frequency is set according to the fluorescence lifetime of the sample, and two-dimensional scanning is performed to record the fluorescence decay curve of each pixel, thereby obtaining the zero-to-two-dimensional fluorescence lifetime distribution map of the sample in the selected area (corresponding to Figure 14 ).
[0132] (4) A three-dimensional TRPL imaging method based on laser scanning confocal microscopy (corresponding to) Figure 15Based on the zero-to-two-dimensional PL imaging settings, a specified depth range for acquisition is selected, and an appropriate repetition frequency of the light source is set according to the sample fluorescence lifetime. Layer-by-layer scanning and imaging of the sample are performed, recording the fluorescence decay curve of each three-dimensional pixel. Finally, a three-dimensional fluorescence lifetime distribution map of the sample is synthesized (corresponding to...). Figure 15 ).
[0133] This embodiment demonstrates that the PL / TRPL imaging method protected by this invention can be realized using only a laser scanning confocal microscope module. Its detection accuracy, non-destructive properties, and multi-parameter resolution capabilities are consistent with the coupling mode, and it belongs to the technical solution of this invention.
[0134] Figure 1 This is a schematic diagram of the laser scanning confocal microscope and ultrafast transient absorption integrated system that operates synchronously with reflective and transmissive detection in Examples 1 and 2. Its optical path layout is built around "pump-detection dual-branch coordination and synchronous acquisition of transmission and reflection signals". The system is provided with an initial laser signal by an ultrafast laser source. The ultrafast laser is precisely divided into pump light and detector light branches by a beam splitting module. The laser scanning confocal microscope module is connected in series to realize the acquisition of transmitted light and reflected light.
[0135] Figure 2 This is a schematic diagram of the TA imaging optical path of the laser scanning confocal microscope and ultrafast transient absorption integrated system that operates synchronously with reflective and transmissive detection in Example 1. The pump light and probe light branches are connected in series with the laser scanning confocal microscope optical path to achieve transmissive or reflective TA imaging.
[0136] Figure 3 This is a schematic diagram of the optical path of the laser scanning confocal microscope and the ultrafast transient absorption integrated system PL and TRPL in Example 2, where the reflective and transmissive detection operate synchronously. The pump light branch of the optical path is connected in series with the laser scanning confocal microscope optical path to realize reflective and transmissive PL and TRPL imaging.
[0137] Figure 4 This is a schematic diagram of the laser scanning confocal microscope and ultrafast transient absorption integrated system operating with reflective detection in Examples 3 and 4. It provides the system with an initial laser signal through an ultrafast laser source, and uses a beam splitting module to accurately split the ultrafast laser into pump light and probe light branches. The laser scanning confocal microscope module is connected in series to realize the acquisition of reflected light.
[0138] Figure 5 This is a schematic diagram of the optical path of the laser scanning confocal microscope and ultrafast transient absorption integrated system (TA) in Example 3, where the pump light and probe light branches are connected in series in the laser scanning confocal microscope optical path to achieve transmission or reflection TA imaging.
[0139] Figure 6This is a schematic diagram of the optical path of the laser scanning confocal microscope and ultrafast transient absorption integrated system PL and TRPL in Example 4, which operates with reflective detection. The pump light branch of the optical path is connected in series with the laser scanning confocal microscope optical path to achieve reflective PL and TRPL imaging.
[0140] Figure 7 This is a schematic diagram of the optical path of the laser scanning confocal microscope and ultrafast transient absorption integrated system in the transmission detection operation of Examples 5 and 6. It provides the initial laser signal to the system through an ultrafast laser source, and uses a beam splitting module to accurately split the ultrafast laser into pump light and probe light branches. The laser scanning confocal microscope module is connected in series to realize the acquisition of reflected light.
[0141] Figure 8 This is a schematic diagram of the optical path of the laser scanning confocal microscope and ultrafast transient absorption integrated system (TA) in Example 5, where the pump light and probe light branches are connected in series in the laser scanning confocal microscope optical path to achieve transmission or reflection TA imaging.
[0142] Figure 9 This is a schematic diagram of the optical path of the laser scanning confocal microscope and ultrafast transient absorption integrated system PL and TRPL in Example 6, which is a transmission-type detection operation. The pump light branch of the optical path is connected in series with the laser scanning confocal microscope optical path to realize transmission-type PL and TRPL imaging.
[0143] Figure 10 This is a schematic diagram of the frequency conversion module in the optical path system of embodiments 1, 2, 3, 4, 5 and 6, where an independent frequency modulation unit is set up in the branch after the beam splitting module 1.
[0144] Figure 11 This is a schematic diagram of a global frequency modulation unit set in front of the beam splitting module 1 in the frequency conversion module of the optical path system of embodiments 1, 2, 3, 4, 5 and 6.
[0145] Figure 12 This is a two-dimensional PL imaging image based on the independent operation mode of the confocal microscope module in Example 7.
[0146] Figure 13 This is a three-dimensional PL imaging image based on the independent operation mode of the confocal microscope module in Example 7.
[0147] Figure 14 This is a two-dimensional TRPL imaging image based on the independent operation mode of the confocal microscope module in Example 7.
[0148] Figure 15 This is a three-dimensional TRPL imaging image based on the independent operation mode of the confocal microscope module in Example 7.
[0149] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and are not intended to limit the scope of protection of the present invention. Although the present invention has been described in detail with reference to preferred embodiments, it is not limited to those listed in the embodiments. All changes, modifications, substitutions and variations made to these embodiments should be included within the scope of protection of the present invention.
Claims
1. A rapid detection device for the three-dimensional spatial and temporal distribution of defects in materials and devices, characterized in that, The core functional modules include: laser module, beam splitting module, frequency conversion module, supercontinuum spectrum generation module, optical delay line module, laser scanning confocal microscope module, spectral detection module, and data processing unit.
2. A rapid detection device for the three-dimensional spatial and temporal distribution of defects in materials and devices according to claim 1, characterized in that, The laser module is an ultrafast pulsed laser with adjustable pulse width, repetition rate, and center wavelength. Its output spectrum's center wavelength and laser intensity can be continuously adjusted (10 nm to 30 μm) or fixed in mode, with a frequency adjustment range covering 0.1~10 nm. 15 Hz, with a time resolution of ≥1 fs; it can synchronously match the ground state absorption band and defect state absorption band of metal, semiconductor and insulating materials and devices, adapt to the dynamic process of samples in different states such as gas, liquid, solid and plasma, and can completely cover the evolution process of carrier excitation, relaxation, recombination and defect trapping in the whole time scale and three-dimensional spatial scale. The core function of the beam splitting module is to achieve precise proportional beam splitting, branch switching, and multi-path collaborative adaptation, adapting to the transmission requirements of pump light and probe light under different imaging modes. It includes three independent beam splitting units (beam splitting module 1, beam splitting module 2, and beam splitting module 3). Specifically: beam splitting module 1 is located behind the laser module and splits the fundamental frequency light into two core branches according to a preset ratio. One beam is connected to the frequency conversion module to generate pump light, and the other beam is connected to the optical delay line module to generate probe light. Beam splitting module 2 is connected behind the frequency conversion module and receives the frequency-modulated pump light and splits it into two paths. One path can be connected in series to the laser scanning confocal microscope module as the incident light source, and the other path is directly used to illuminate the sample under test after being modulated by a chopper. Beam splitting module 3 is connected behind the supercontinuum spectrum generation module and receives the broadband probe light and splits it into two paths. One path is connected to the laser scanning confocal microscope module as the probe light source, and the other path is connected to the blackbody module to achieve the absorption of redundant beams. The frequency conversion module can perform secondary frequency modulation on the fundamental frequency light, with a frequency adjustment range covering 0.1~10. 15 Hz, the frequency conversion module adopts a switchable dual-station configuration: a global frequency modulation unit is set in front of the beam splitter module 1, or a branch independent frequency modulation unit is set in the rear of the beam splitter module 1; The core function of the supercontinuum spectrum generation module is to extend the incident light into a broadband probe light with high coherence and a wide wavelength range (10 nm to 30 μm). The core function of the optical delay line module is to precisely control the optical path length of the probe light branch. By changing the beam transmission path length, the propagation time of the probe light can be precisely adjusted, so that the time difference between the probe light and the pump light reaching the sample under test can be continuously adjusted, with a time resolution of ≥1 fs. The laser scanning confocal microscope module can selectively operate independently from the pump-probe branch of the ultrafast transient absorption spectrum, possessing high precision and a wide detection range, and includes three structural forms. When operating independently, it can achieve defect detection relying solely on its own configured light source, optical lens assembly, scanning galvanometer, high-precision stage, and matching spectral detection module. Its depth range (z-axis) is 0~1 m, its lateral range (X / Y-axis) is 0~1 m, and its depth and lateral scanning step accuracy is ≥0.1 nm, with a spatial resolution of ≥0.1 nm, meeting the requirements for large-area, high-precision detection. The three structural forms include: a laser scanning confocal microscope with simultaneous reflection and transmission detection, a laser scanning confocal microscope with reflection detection, and a laser scanning confocal microscope with transmission detection, as detailed below: (1) The first dual-detection module structure, a laser scanning confocal microscope with synchronous operation of reflection and transmission detection, comprises: a light source, a scanning galvanometer, a dichroic mirror, two sets of optical lens assemblies (optical lens, focusing pinhole, and optical lens), a sample, a spectrometer 2 for collecting the reflected light signal PL and TRPL of the sample and an adapted imaging detector 2, and a spectrometer 3 for collecting the transmitted light signal PL and TRPL of the sample and an adapted imaging detector 3; the two sets of optical lens assemblies are connected in sequence by pipes: an optical lens, a focusing pinhole, and an optical lens; the connection method is: with the sample to be tested as the core, a symmetrical optical path coupling structure for synchronous acquisition of transmission and reflection signals is constructed on both sides of the sample, and a set of "optical lens, focusing pinhole, and optical lens" is provided on the front and back sides of the sample to be tested, respectively. The optical lens assembly is a linked and coupled combination structure. The outer side of the optical lens assembly on the front side of the sample passes through a dichroic mirror via an optical path, and then connects to the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2 via a focusing pinhole. The outer side of the optical lens assembly on the rear side of the sample is directly connected to the PL and TRPL spectrometers 3 and their corresponding imaging detectors 3 via an optical path. The light source is connected to the dichroic mirror via a scanning galvanometer module. Its working principle is as follows: the incident light emitted by the light source is precisely deflected by the scanning galvanometer, then reflected by the dichroic mirror, and then sequentially converged by the optical lens, filtered by the focusing pinhole to remove stray light, and then re-converged by the optical lens. By adjusting the lens position or the height of the high-precision stage, the probe light is precisely focused on the designated position of the sample. The reflected signal generated after the sample is excited propagates in the reverse direction along the original incident light path, passes through the optical lens, focusing pinhole, and optical lens in sequence, and then passes through the dichroic mirror before being detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2. The transmitted signal generated after the sample is excited passes through the sample and is transmitted by the optical lens, focusing pinhole, and optical lens combination behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 to complete the detection and recording, realizing the synchronous acquisition of reflected and transmitted signals. (2) The second type of laser scanning confocal microscope with reflective detection operation: Compared with the first type of dual detection module, its structure is composed of removing the optical lens assembly, PL and TRPL spectrometers 3 and imaging detector 3 on the back side of the sample, while retaining the other parts in the same manner as the dual detection module; Compared with the first type of dual detection module, its connection method is different in that there is no optical lens, focusing pinhole and optical lens combination structure on the back side of the sample, and there is no PL and TRPL spectrometers 3 and corresponding imaging detector 3, while the other parts are connected in the same manner as the first module; Compared with the first type of dual detection mode, its working mode does not collect the transmission signal generated after the sample is excited, but collects the reflection signal generated after the sample is excited and propagates in the reverse direction along the original incident light path, passing through the optical lens, focusing pinhole and optical lens in sequence, and then passing through the dichroic mirror and being detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detector 2; (3) Laser scanning confocal microscope with transmission detection operation: Compared with the first dual detection module, its structure is composed of removing the optical lens assembly, dichroic mirror, PL and TRPL spectrometer 2 and imaging detector 2 on the front side of the sample, while retaining the other parts as the first module; Compared with the first dual detection module, its connection method is different in that there is no optical lens, focusing pinhole and optical lens combination structure on the front side of the sample, no dichroic mirror, and no PL and TRPL spectrometer 2 and corresponding imaging detector 2, while the other parts are connected in the same way as the first module; Compared with the first dual detection mode, its working mode does not collect the reflection signal generated after the sample is excited, but collects the transmission signal generated after the sample is excited. The transmission signal generated after the sample is excited passes through the sample and is transmitted by the optical lens, focusing pinhole and optical lens combination behind the sample to another set of PL and TRPL spectrometer 3 and imaging detector 3 to complete the detection and recording, thereby realizing the acquisition of transmission signal; The spectral detection module has a detection range of 100 nm to 1000 μm and includes multiple spectrometers and matching imaging detectors. It is divided into functional groups to accurately acquire differential absorption signals and fluorescence / infrared / Raman signals to meet the detection requirements of different working modes of the device. The specific configuration includes: (1) TA spectrometer 1 and corresponding imaging detector 1, whose core function is to receive and record the differential absorption signal of the sample after the detection light passes through the sample in two states: pump light excitation and no pump light excitation; (2) reflective PL and TRPL spectrometers 2 and imaging detector 2, which focus on signal acquisition of the reflection path; (3) transmission PL and TRPL spectrometers 3 and imaging detector 3, which focus on signal acquisition of the transmission path. The above two sets of PL and TRPL spectrometers and corresponding imaging detector units are used together to receive and record the fluorescence, infrared and Raman signals generated after the sample is excited by the focused beam to meet the signal detection requirements of the device in different working modes. The data processing unit is electrically connected to imaging detector 1, imaging detector 2 and imaging detector 3 respectively, and collects signals in the data processing unit to extract four-dimensional data of the material's spatial coordinates and time dynamic evolution information.
3. A rapid detection device for the three-dimensional spatial and temporal distribution of defects in materials and devices according to claim 2, characterized in that, After extracting the spatial coordinates and temporal dynamic evolution information of the material from the data processing unit, further data transformation and analysis can yield one or more of the following: material structure and composition information, energy level information, charge carrier information, optical information, electronic and lattice vibration information, and macroscopic physical information, as detailed below: (1) Structural and compositional information: Structural and compositional information is the basic characterization content for defect detection in materials and devices. Its core purpose is to clarify the spatial distribution of defects and the essential composition of materials. It includes structural defects, as well as the composition, valence state, and free radicals of materials. Among them, structural defects are directly obtained through the three-dimensional scanning signal of the laser scanning confocal microscope module. The defect location in the three-dimensional space of xyz is accurately located by utilizing the difference in PL and TRPL intensity between the defect area and the normal area, and the difference in relaxation rate of the TA differential absorption signal. The composition of materials needs to be indirectly calculated by matching with the characteristic emission peak of the PL spectrum, the characteristic scattering peak of the Raman spectrum, or the characteristic absorption peak of the infrared spectrum with the industry standard spectral library. The valence state of elements is derived by the Raman peak shift and the splitting phenomenon of the infrared absorption peak. It is obtained by combining quantum chemical calculation analysis with the difference in chemical bond vibration frequency caused by the change of valence state. Free radicals are identified by the absorption peak of the characteristic functional group in the infrared spectrum and their type is determined by the spectral analysis. (2) Energy level information: Energy level information focuses on the characterization of the electronic energy state of materials and devices, with the core being the accurate identification of energy level defects and the quantification of related energy parameters. This includes energy level defects (including deep and shallow energy level defects), band gap, Fermi level, electronic density of states, and energy level position. Among them, the energy level defects (including deep and shallow energy level defects) are calculated by combining the relaxation time of the TA signal and TRPL fluorescence lifetime data with the band gap formula. Shallow energy level defects correspond to short relaxation times in the picosecond range, while deep energy level defects correspond to long relaxation times in the nanosecond range. The band gap is directly calculated by reading the PL emission peak. The Fermi level is calculated by combining the TA absorption edge analysis with the formula. The electronic density of states is derived from the TA spectral absorption coefficient distribution based on the Kramers-Kronig relationship. The energy level position is determined by converting the valence band top and conduction band bottom energies with the defect energy level offset. (3) Carrier Information: Carrier information revolves around the motion characteristics and mechanisms of carriers such as electrons and holes in materials, with the core being the identification of carrier recombination centers and the determination of key dynamic parameters. This includes carrier recombination centers, as well as carrier lifetime, carrier concentration, carrier mobility, and carrier mean free path. Among these, carrier recombination centers (associated with structural defects and energy level defects) are indirectly determined through multi-exponential fitting of TRPL decay curves, with different decay time constants corresponding to different types of recombination centers. Carrier lifetime is obtained by fitting TRPL single-exponential or multi-exponential decay curves and extracting characteristic decay times. Carrier concentration is calculated from the intensity of the TA differential absorption signal. Carrier mobility is obtained by calculating the diffusion coefficient using the carrier diffusion distance. The carrier mean free path is indirectly calculated based on carrier mobility and thermal velocity. (4) Optical Information: Optical information mainly characterizes the absorption, emission, and response characteristics of materials and devices to light, directly reflecting the light-to-conversion potential and optical performance of the materials. This includes the fluorescence absorption, fluorescence emission, variable excitation characteristics, and carrier recombination efficiency of the materials. Among them, the fluorescence absorption and emission characteristics are directly obtained through PL spectroscopy. By reading the absorption peak, emission peak position (wavelength), and peak intensity in the spectrum, the optical response range and luminescence characteristics of the materials can be determined. Variable excitation characteristics are obtained through direct testing. By adjusting the excitation power and repetition frequency of the laser module, the PL intensity change curves under different conditions are recorded, and its linear growth or saturation characteristics are analyzed. The carrier recombination efficiency is calculated by the correlation formula between PL quantum yield and fluorescence lifetime, or by the ratio of calibrated PL intensity to excitation light intensity. (5) Electronic and lattice vibration information: Electronic and lattice vibration information focuses on the characterization of the microscopic motion state of materials, with the core being the analysis of phonon distribution and electron spin characteristics. This includes the phonon distribution and electron spin of the material; the phonon distribution state is directly obtained through Raman spectroscopy, and the distribution of phonons is determined by reading the characteristic peak intensity ratio of different phonon modes in the Raman spectrum; the electron spin characteristics are based on the spin splitting signal of the Raman peak or the spin relaxation time of the TA signal, and the electron spin state can be analyzed by combining quantum mechanical models; (6) Macroscopic physical information: Macroscopic physical information characterizes the overall physical properties of materials and devices, and is directly related to their performance and reliability in practical application scenarios. This includes properties such as the material's work function, temperature field, dielectric constant, polarization characteristics, and conductivity. Specifically, the temperature field distribution is directly obtained through the infrared spectroscopy module. Based on the infrared signal intensity distribution, the three-dimensional temperature distribution of the sample is directly mapped using the fourth power relationship between blackbody radiation intensity and temperature. The work function is derived from the maximum kinetic energy of photoelectrons combined with the photon energy of the laser. The dielectric constant is derived from the refractive index change derived from the TA signal. The polarization characteristics are calculated by converting the polarization-induced absorption change with the calibration curve. The conductivity is derived from carrier concentration and mobility based on Ohm's law.
4. A rapid detection device for the three-dimensional spatial and temporal distribution of defects in materials and devices according to claim 2, characterized in that, The overall optical path connection sequence of the rapid detection device is as follows: The optical path following the laser module output light is connected to beam splitting module 1. Beam splitting module 1 can split into two beams. The optical path following one beam is connected to a frequency conversion module, which generates pump light after frequency adjustment. The pump light generated after the frequency conversion module is connected to beam splitting module 2. The optical path following the other beam from beam splitting module 1 is connected to an optical delay line module. The optical path following the optical delay line module is connected to a supercontinuum spectrum generation module, allowing the other beam from beam splitting module 1 to change its optical path and generate broadband probe light through the supercontinuum spectrum generation module. The broadband probe light generated after the supercontinuum spectrum generation module is connected to beam splitting module 3. The output light from beam splitting module 3 can be split into two beam paths. The optical path following one beam path is connected to… The first beam is connected to a blackbody module, and the second beam path is connected to a laser scanning confocal microscope module. It can be used as the light source for the laser scanning confocal microscope module. That is, the probe light branch enters the laser scanning confocal microscope module through the beam splitter module 3 as a light source or is absorbed by the blackbody. The output light from the beam splitter module 2 can be divided into two beam paths. The second beam path is connected to the laser scanning confocal microscope module and can also be used as the light source for the laser scanning confocal microscope module. The third beam path is connected to the chopper and the sample to be tested in the laser scanning confocal microscope module. That is, the output light from the beam splitter module 2 enters the laser scanning confocal microscope module as a light source or directly irradiates the sample to be tested after passing through the chopper.
5. A rapid detection device for the three-dimensional spatial and temporal distribution of defects in materials and devices according to claim 1, characterized in that, The rapid detection device has been functionally expanded by further integrating an infrared spectroscopy module and a Raman spectroscopy module. It supports synchronous or time-division acquisition of transient absorption signals, infrared absorption signals, and Raman scattering signals. The wide wavelength range of the laser module (10 nm to 30 μm) is compatible with the high sensitivity response of the spectral detection module (100 nm to 1000 μm), which can cover the mid-infrared to far-infrared band required by infrared spectroscopy and also meet the requirements of Raman spectroscopy for accurate capture of characteristic scattering peaks.
6. A method for rapid testing of materials and devices using the rapid testing device according to any one of claims 1-5, characterized in that, This is a multimodal testing method with core functions based on laser scanning confocal microscopy and ultrafast transient absorption spectroscopy with deep coaxial coupling. Specifically, it includes: (1) a rapid detection method based on a laser scanning confocal microscope and an ultrafast transient absorption integrated system operating simultaneously with reflective and transmissive detection, including TA imaging mode and PL and TRPL imaging modes; (2) a rapid detection method based on a laser scanning confocal microscope and an ultrafast transient absorption integrated system operating with reflective detection, including TA imaging mode and PL and TRPL imaging modes; (3) a rapid detection method based on a laser scanning confocal microscope and an ultrafast transient absorption integrated system operating with quasi-transmissive detection, including TA imaging mode and PL and TRPL imaging modes, as follows: (1) A method for rapid detection using a laser scanning confocal microscope that integrates reflective and transmissive detection with an ultrafast transient absorption system, which is divided into two imaging modes: The first type of TA imaging mode specifically includes the following steps: S1: Start the laser module and output fundamental frequency light. Based on the characteristics of the ground state absorption band and defect state absorption band of the sample under test, precisely adjust the pulse width, repetition frequency and center wavelength to ensure that the laser can effectively excite the sample to generate defect-correlated excited states. S2: The fundamental frequency beam is split into two beams by the beam splitting module 1 according to a preset ratio. One beam is sent to the frequency conversion module for secondary frequency modulation and then used as pump light. The other beam enters the optical delay line module. The time difference between the beam and the pump light is adjusted by precisely controlling the optical path difference. Then, the broadband probe light is generated by the supercontinuum spectrum generation module. S3: The pump light is selected by the beam splitting module 2 and periodically modulated by the chopper before directly irradiating the designated area of the sample to be tested, so that the pump light alternately irradiates the sample at a fixed frequency, forming a periodic state switching of "excited-unexcited". S4: The probe light is selected and connected to the laser scanning confocal microscope module via the beam splitter module 3 as the incident light source; the beam deflection angle is precisely controlled by the scanning galvanometer to achieve point-by-point scanning of the target area in the xy plane of the sample; after being reflected by the dichroic mirror, it is then converged by the optical lens, filtered by the focusing pinhole to remove stray light, and then converged again by the optical lens, finally precisely focusing the probe light on the sample surface and different depth positions inside; by adjusting the lens position or the height of the high-precision stage, continuous focusing in the sample depth direction (z) is achieved, completing point-by-point coverage in three-dimensional space; S5: The focused probe light and pump light are precisely superimposed at a designated position on the sample. The pump light periodically excites the sample in time through a chopper, causing ground-state carriers to absorb photon energy (electrons and holes) and transition from the ground state to the excited / defect state, thus changing the energy state of the sample. The probe light continuously changes its path length through the optical delay line module, realizing a full-time domain scan of the probe light relative to the arrival time of the pump light (covering the entire process of carrier excitation, defect trapping, and recombination). Broadband light is generated through the supercontinuum spectroscopy generation module. When it acts on the sample, it is selectively absorbed by the excited / defect state carriers in the sample by the pump light, carrying the state information of the sample and completely capturing the dynamic process of the interaction between carriers and defects in the time dimension (t). S6: The TA spectrometer and imaging detector 1 simultaneously acquire the differential absorption signal of the probe light (reflection / transmission) after the sample is subjected to "pump light excited state" and "no pump light ground state"; this signal directly reflects the concentration of charge carriers (electrons and holes) in the excited state of the sample at different time points (t). By completely recording the temporal differential signal of each pixel in the xyz three-dimensional space, a four-dimensional dataset containing "spatial three-dimensional (xyz) + temporal one-dimensional (t)" is finally constructed to realize the synchronous characterization of the spatial distribution and temporal evolution of defects. The second type of PL and TRPL imaging mode specifically includes the following steps: S1: Start the laser module and output fundamental frequency light. Based on the characteristics of the ground state absorption band and defect state absorption band of the sample under test, precisely adjust the pulse width, repetition frequency and center wavelength to ensure that the laser can effectively excite the sample to generate defect-correlated excited states. S2: The fundamental frequency beam is split into two beams by the beam splitting module 1. One beam is frequency-modulated by the frequency conversion module and used as pump light. The other beam enters the optical delay line module to control the time difference with the pump light, and then the probe light is generated by the supercontinuum spectrum generation module. S3: The pump light is selected and connected to the laser scanning confocal microscope module via the beam splitter module 2 as the incident light source; the beam deflection angle is adjusted by the scanning galvanometer to achieve point-by-point scanning of the target area of the sample in the xy plane; after being reflected by the dichroic mirror, it is then focused onto the target area of the sample in the xy plane after being converged by the optical lens and filtered by the focusing pinhole; by adjusting the lens position or the height of the high-precision stage, precise focusing in the depth direction (z) of the sample is achieved, completing point-by-point coverage in three-dimensional space; S4: The fluorescence, infrared, and Raman signals generated after the sample is excited propagate in the reverse direction along the original incident light path, passing through an optical lens, a focusing pinhole, and another optical lens in sequence, before passing through a dichroic mirror and being detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2; the transmitted signals pass through the sample and are transmitted by a combination of optical lenses, a focusing pinhole, and another optical lens behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 for detection and recording. The two sets of detection units synchronously collect signals and signal attenuation to construct a zero-to-three-dimensional (xyz) dataset; (2) The second type of reflective detection method uses a laser scanning confocal microscope and an ultrafast transient absorption integrated system for rapid detection, which is divided into two imaging modes: The first type of TA imaging method specifically includes the following steps: S1 to S6: Steps S1 to S6 of the TA imaging mode of the first type of transmission / reflection dual-detection structure are completely consistent; The second PL and TRPL imaging method specifically includes the following steps: S1 to S3: Steps S1 to S3 of the PL and TRPL imaging modes of the first type of transmission / reflection dual-detection structure are completely consistent; S4: After the sample is excited, it only produces fluorescence, infrared and Raman signals in the reflected direction. The signal propagates in the reverse direction along the original incident light path, passes through the optical lens, focusing pinhole and optical lens in sequence, and then passes through the dichroic mirror. The PL and TRPL spectrometers 2 and their corresponding imaging detectors 2 complete the detection and recording. By collecting the reflected signal and the signal attenuation, a zero-to-three-dimensional (xyz) dataset is constructed. (3) The third type of transmission detection method uses a laser scanning confocal microscope and an ultrafast transient absorption integrated system for rapid detection, which is divided into two imaging modes: The first type of TA imaging method specifically includes the following steps: S1 to S6: Steps S1 to S6 of the TA imaging mode of the first type of transmission / reflection dual-detection structure are completely consistent; The second PL and TRPL imaging method specifically includes the following steps: S1-S3: The steps S1-S3 of the PL and TRPL imaging modes of the first type of transmission / reflection dual-detection structure are completely consistent; S4: After the sample is excited, it only produces fluorescence, infrared and Raman signals in the transmission direction. After passing through the sample, the signal is transmitted to the PL and TRPL spectrometers 3 and imaging detector 3 through the optical lens, focusing pinhole and optical lens combination behind the sample to complete the detection and recording (no reflection signal acquisition); by collecting the transmission signal and signal attenuation, a zero to three-dimensional (xyz) dataset is constructed.
7. The method of claim 6, characterized in that, The laser scanning confocal microscope module can focus the excitation light onto the sample surface or at a specified depth within the sample, with a depth range (z-axis) of 0~1 m and a lateral range (X / Y-axis) of 0~1 m. The depth and lateral scanning step accuracy is less than or equal to 1 nm, preferably 0.1 nm, and the spatial resolution is ≥0.1 nm. This meets the requirements for large-area, high-precision, and rapid detection.
8. The method of claim 6, characterized in that, The material includes one or more of metals, semiconductors, insulating materials, etc., and its physical state range includes one or more of gaseous, liquid, solid and plasma states, as well as heterogeneous materials formed by the combination of the above materials. The devices include, but are not limited to, the following types and are adapted to defect detection under various physical conditions: metal-based devices: metal interconnect structures, metal thin-film sensors; semiconductor-based devices: solar cells, photodetectors, light-emitting diodes, chips; insulator-based devices: dielectric capacitors, insulating coatings, etc. This method is applicable to defect distribution detection and performance correlation analysis of the aforementioned devices.
9. A laser scanning confocal microscope, characterized in that, It features three structural forms, each capable of defect detection relying solely on its own configured light source, optical lens assembly, scanning galvanometer, high-precision stage, and matching spectral detection module. These three forms include: a laser scanning confocal microscope with simultaneous reflective and transmissive detection, a laser scanning confocal microscope with reflective detection, and a laser scanning confocal microscope with transmissive detection, as detailed below: (1) The first dual-detection module structure, a laser scanning confocal microscope with synchronous operation of reflection and transmission detection, comprises: a light source, a scanning galvanometer, a dichroic mirror, two sets of optical lens assemblies (optical lens, focusing pinhole, and optical lens), a sample, a spectrometer 2 for collecting the reflected light signal PL and TRPL of the sample and an adapted imaging detector 2, and a spectrometer 3 for collecting the transmitted light signal PL and TRPL of the sample and an adapted imaging detector 3; the two sets of optical lens assemblies are connected in sequence by pipes: an optical lens, a focusing pinhole, and an optical lens; the connection method is: with the sample to be tested as the core, a symmetrical optical path coupling structure for synchronous acquisition of transmission and reflection signals is constructed on both sides of the sample, and a set of "optical lens, focusing pinhole, and optical lens" is provided on the front and back sides of the sample to be tested, respectively. The optical lens assembly is a linked and coupled combination structure. The outer side of the optical lens assembly on the front side of the sample passes through a dichroic mirror via an optical path, and then directly connects to the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2 via a focusing pinhole. The outer side of the optical lens assembly on the rear side of the sample passes through an optical path directly connects to the PL and TRPL spectrometers 3 and their corresponding imaging detectors 3. The light source is connected to the dichroic mirror via a scanning galvanometer module. Its working principle is as follows: the incident light emitted by the light source is precisely deflected by the scanning galvanometer, then reflected by the dichroic mirror, and then sequentially converged by the optical lens, filtered by the focusing pinhole to remove stray light, and then re-converged by the optical lens. By adjusting the lens position or the height of the high-precision stage, the probe light is precisely focused onto a designated position on the sample. The reflected signal generated after the sample is excited propagates in the reverse direction along the original incident light path, passing through an optical lens, a focusing pinhole, and another optical lens in sequence, before passing through a dichroic mirror and being detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2. The transmitted signal generated after the sample is excited passes through the sample and is transmitted by a combination of optical lenses, a focusing pinhole, and another optical lens behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 for detection and recording, thus achieving synchronous acquisition of reflected and transmitted signals. (2) The second type of laser scanning confocal microscope with reflective detection operation: Compared with the first type of dual detection module, its structure is composed of removing the optical lens assembly, PL and TRPL spectrometers 3 and imaging detector 3 on the back side of the sample, while retaining the other parts in the same manner as the dual detection module; Compared with the first type of dual detection module, its connection method is different in that there is no optical lens, focusing pinhole and optical lens combination structure on the back side of the sample, and there is no PL and TRPL spectrometers 3 and corresponding imaging detector 3, while the other parts are connected in the same manner as the first module; Compared with the first type of dual detection mode, its working mode does not collect the transmission signal generated after the sample is excited, but collects the reflection signal generated after the sample is excited and propagates in the reverse direction along the original incident light path, passing through the optical lens, focusing pinhole and optical lens in sequence, and then passing through the dichroic mirror and being detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detector 2; (3) Laser scanning confocal microscope with transmission detection operation: Compared with the first dual detection module, its structure is composed of removing the optical lens assembly, dichroic mirror, PL and TRPL spectrometers 2 and imaging detector 2 on the front side of the sample, while retaining the other parts as in the first module; Compared with the first dual detection module, its connection method is different in that there is no optical lens, focusing pinhole and optical lens combination structure on the front side of the sample, no dichroic mirror, and no PL and TRPL spectrometers 2 and corresponding imaging detectors 2, while the other parts are connected in the same way as the first module; Compared with the first dual detection mode, its working mode does not collect the reflection signal generated after the sample is excited, but collects the transmission signal generated after the sample is excited. The transmission signal generated after the sample is excited passes through the sample and is transmitted by the optical lens, focusing pinhole and optical lens combination behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 to complete the detection and recording, thereby realizing the acquisition of transmission signal.
10. The laser scanning confocal microscope imaging method according to claim 9, characterized in that, By utilizing its own light source, optical lens assembly, scanning galvanometer, high-precision stage, and spectral detection module (PL and TRPL spectrometers 2 and corresponding imaging detectors 2, PL and TRPL spectrometers 3 and corresponding imaging detectors 3), four sub-modes are achieved: zero-dimensional to two-dimensional photoluminescence (0D to 2DPL), three-dimensional photoluminescence (3DPL), zero-dimensional to two-dimensional time-resolved photoluminescence (0D to 2D TRPL), and three-dimensional time-resolved photoluminescence (3D TRPL). This enables the spatial distribution detection of defects in materials and devices, specifically including the following: (1) A 0D to 2D PL imaging mode based on confocal microscopy, comprising the following steps: S1: Sample and objective configuration: Provide an objective group including at least a low-power objective and a high-power oil immersion objective; when the high-power oil immersion objective is selected, apply immersion oil between the front end of the objective and the sample coverslip to ensure that the sample surface is fully wetted by the immersion oil; S2: Excitation light configuration: Turn on the tunable laser source, whose excitation wavelength range covers 10 nm to 30 μm. After selecting the objective lens, adjust the laser wavelength to the optimal excitation wavelength of the target sample. S3: Detection optical path configuration: Select the spectrometer and the corresponding imaging detector, and set its receiving wavelength range to the optimal excitation wavelength, specifically, it can be arbitrarily adjusted within the range of 100 nm to 1000 μm; S4: Focusing: By controlling the high-precision stage with an accuracy better than 0.1 nm to move along the Z-axis, the positive focal plane is found until the intensity of the detected fluorescence signal reaches a local maximum, and the signal-to-noise ratio is optimized by adjusting the laser power intensity; S5: Image acquisition: By adjusting the beam deflection angle with a scanning galvanometer, point-by-point scanning of the target area in the xy plane of the sample is achieved, and the 0D to 2D PL intensity distribution map of the sample is obtained; (2). A 3D PL imaging method based on confocal microscopy, comprising the following steps: S1: Based on the 0D to 2D PL imaging modes of the confocal microscope, S1 to S4, the sample is adjusted to the positive focus position; S2: Set the Z-axis range for 3D scanning: By controlling a high-precision stage with an accuracy better than 0.1 nm, move the stage unidirectionally along the Z-axis until the sample is completely out of focus, and mark it as the starting point of the 3D scan in the operation interface; then move the stage in the opposite direction, passing through the positive focus position and continuing to move in the opposite direction to the completely out of focus position, and mark it as the ending point of the 3D scan. S3: Set the layer scan parameters: In the 3D settings window, set the number of slices to be collected between the start point and the end point. The Z-axis step size between slices is fixed and adjustable within the range of 0.1 nm to 1 m. S4: The fluorescence, infrared, and Raman signals generated after the sample is excited propagate in the reverse direction along the original incident light path, passing through an optical lens, a focusing pinhole, and another optical lens in sequence, before passing through a dichroic mirror and being detected and recorded by the PL and TRPL spectrometers 2 and their corresponding imaging detectors 2; the transmitted signals pass through the sample and are transmitted by a combination of optical lenses, a focusing pinhole, and another optical lens behind the sample to another set of PL and TRPL spectrometers 3 and imaging detectors 3 for detection and recording. The two sets of detection units synchronously collect signals and signal attenuation to construct a zero-to-three-dimensional (xyz) dataset; S4: 3D Image Acquisition: The beam deflection angle is adjusted by the scanning galvanometer to achieve point-by-point scanning of the target area of the sample in the xy plane; by adjusting the lens position or the height of the high-precision stage, the sample depth direction (z) is precisely focused to complete point-by-point coverage in three-dimensional space; the system automatically performs 3D scanning and imaging according to the set number of slices and step size, and synthesizes the images of each layer to obtain the 3D PL distribution map of the sample; (3) A 0D to 2D TRPL imaging method based on confocal microscopy, comprising the following steps: S1: Based on the 0D to 2D PL imaging modes of the confocal microscope, S1 to S4, the sample is adjusted to the positive focus position; S2: Time-resolved parameter settings: Turn on the laser, the excitation wavelength is arbitrarily adjustable within the range of 10 nm to 30 μm, and the repetition frequency is between 0.1 and 10. 15 The frequency can be adjusted arbitrarily within the Hz range, and a suitable repetition frequency can be set according to the sample fluorescence lifetime. S3: Image acquisition: The beam deflection angle is adjusted by the scanning galvanometer to achieve point-by-point scanning of the target area of the sample in the xy plane, and the fluorescence decay curve of each pixel is recorded to obtain the 0D to 2D PL fluorescence lifetime distribution map of the sample in the selected area. (4) A 3D TRPL imaging method based on confocal microscopy, comprising the following steps: S1: Based on the 0D to 2D PL imaging modes of the confocal microscope, S1 to S4, the sample is adjusted to the positive focus position; S2: Set the Z-axis range for 3D scanning: Move the high-precision stage with an accuracy better than 0.1 nm along the Z-axis until the sample is completely out of focus, and mark it as the starting point of the 3D scan in the operation interface; then move the stage in the opposite direction, passing through the positive focus position and continuing to move in the opposite direction to the completely out of focus position, and mark it as the ending point of the 3D scan. S3: Time resolution parameter settings: In 3D scanning mode, select to switch to a pulsed laser. The excitation wavelength range of the pulsed laser is 10 nm to 30 μm, and the pulse repetition frequency is 0.1~10 μm per trigger. 15 Adjustable within the Hz range, allowing you to set a suitable repetition frequency based on the sample fluorescence lifetime; S4: Set the layer scan parameters: In the 3D settings window, set the number of slices to be collected between the start point and the end point. The Z-axis step size between slices is fixed and adjustable within the range of 0.1 nm to 1 m. S5: 3D Image Acquisition: The beam deflection angle is adjusted by the scanning galvanometer to achieve point-by-point scanning of the target area in the xy plane of the sample; by adjusting the lens position or the height of the high-precision stage, the sample depth direction (z) is precisely focused to complete point-by-point coverage in three-dimensional space; the system automatically performs 3D scanning according to the set number of slices and step size, records the fluorescence decay curve of each 3D pixel, and finally synthesizes the 3D TRPL distribution map of the sample.