Novel nanometer laser sensing mechanism with ultrahigh sensitivity and resolution ratio

Abstract

The invention discloses a sensing mechanism and method based on nano laser, and the method comprises the following steps: (1) selecting and matching a luminescent material which needs to meet the following conditions: the luminescent material is a marker capable of being used for luminescent sensing and also can be used as a gain medium of a nano laser; (2) energy level matching and optimization between all light-emitting molecules used in traditional sensing based on light-emitting signal intensity change as a nano laser gain medium and a surface plasmon structure; (3) obtaining a nano laser signal based on the surface plasmon array and the luminescent material system; and (4) the sensing based on the nano laser signal has higher sensitivity and resolution compared with the traditional sensing based on the intensity change of the light-emitting signal. The intensity of the nano laser in the invention is influenced by the intensity of the luminescent substance. The mechanism is disclosed for the first time, and compared with traditional luminous intensity sensing, nano laser has high sensitivity and resolution due to the ultra-narrow linewidth, and will play an important role in the future optical sensing technology.

Description

Technical Field

[0001] This invention belongs to the fields of nano-optics, analytical chemistry, and biomedicine, and in particular relates to a novel sensing mechanism based on nanolasers, which has ultra-high sensitivity and resolution. Background Technology

[0002] The development of fluorescence sensing technology can be traced back to the 19th century, but it wasn't until the 20th century, with the emergence of fluorescence detection methods and advancements in instrument technology, that fluorescence sensing technology gradually gained widespread application. Early on, fluorescence was primarily observed with the naked eye, but this method had limited sensitivity. In 1928, Jette and West developed the first photoluminometer, ending the era of naked-eye observation. Subsequently, Zworykin and Rajchman's invention of the photomultiplier tube in 1939 further improved the sensitivity and resolution of the luminometer, bringing a significant breakthrough to the development of fluorescence detection methods. However, fluorescence sensing also has significant drawbacks, such as susceptibility to environmental interference, limited selectivity, sensitivity limitations, stability issues, biocompatibility problems, operational complexity, and quantum yield limitations.

[0003] Plasmonic nanolasers utilize nanocavities provided by plasmonic structures as coherent light sources at the nanoscale for optical feedback. We have found that almost all biomarkers used for luminescence analysis can serve as gain media for nanolasers. This means that traditional luminescence-based analytical sensing techniques can be used for sensing and analysis using signals from nanolaser lasing. Importantly, nanolaser signals offer higher sensitivity and resolution. However, this technology has a crucial prerequisite: achieving the nanolaser threshold. In fact, scientists in this field internationally have been working diligently to address the nanolaser threshold problem through various methods. In recent years, continuously pumpable nanolasers at room temperature have been achieved. We have also made significant breakthroughs in this direction, including the development of nanolasers that can be excited by ordinary light sources such as incoherent LEDs through optimization of the nanocavity. This forms the important research foundation for the nanolaser signal sensing proposed in this invention. Summary of the Invention

[0004] In view of the shortcomings pointed out in the background art and the existing research foundation, the present invention provides a new mechanism for ultra-high sensitivity and resolution based on nanolaser sensing, aiming to solve the problems existing in the prior art mentioned in the background art.

[0005] To achieve the above objectives, the technical solution adopted by the present invention is as follows:

[0006] A novel nanolaser sensing mechanism with ultra-high sensitivity and resolution includes the following steps:

[0007] (1) The selection and matching of luminescent materials must meet the following requirements: they must be both a marker that can be used for luminescent sensing and a gain medium for nanolasers.

[0008] (2) Energy level matching and optimization between the luminescent molecules used as nanolaser gain media and surface plasmon structures in all traditional sensing based on changes in luminescent signal intensity;

[0009] (3) Obtaining nanolaser signals based on surface plasmon arrays and luminescent material systems;

[0010] (4) Sensing based on nanolaser signals has higher sensitivity and resolution than traditional sensing based on changes in the intensity of light emission signals.

[0011] Optionally, in step (1), the luminescent molecule can emit light in the range of 190-1000 nm, but there is no strict limitation.

[0012] Optionally, in step (2), the method of using nanolaser gain medium can be spin coating, drop coating, surface self-assembly, specific bonding, surface potential and hydrophilic / hydrophobic adsorption on the surface of plasmonic nanostructure, or using a refractive index matching liquid to attach the gain medium fixed on other substrates to the surface of plasmonic nanostructure.

[0013] Optionally, in steps (2, 3), the surface plasmon array includes a gold and silver nanoarray structure prepared by holographic lithography, nanoimprint lithography, nanosphere lithography, and electron beam and focused ion beam etching methods.

[0014] Optionally, in step (3), the pump source in the nanolaser acquisition can be a continuous laser or a pulsed laser;

[0015] Optionally, in step (3), the range of the acquisition angle in the nanolaser acquisition can be 0-360°;

[0016] Optionally, in steps (3, 4), the properties of the nanolaser signal can be intensity, displacement, full width at half maximum (FWHM), and threshold.

[0017] Alternatively, different detection systems can be developed by changing the luminescent molecules or altering the specific binding mechanism.

[0018] The present invention, employing the above technology, has the following advantages:

[0019] 1. High-precision methods, such as holographic lithography and nanoimprinting, can be used to fabricate different nano-optical cavities to match fluorescent probes with different emission wavelengths, including but not limited to 190-1000nm.

[0020] 2. Surface-deposited metals and semiconductor materials can be bonded to many modification layers, offering a wide range of options. For example, gold can form strong gold-sulfur bonds with substances containing thiol groups.

[0021] 3. The laser signal acquisition is fast and accurate, with an ultra-narrow linewidth and ultra-high intensity. Its sensitivity is higher than that of fluorescence detection and plasmon refractive index detection, enabling rapid detection of trace biomolecules and compounds.

[0022] 4. The self-made nanolaser acquisition system can achieve a wide range of adjustable angle acquisition and can easily tune the emission band of the nanolaser. Attached Figure Description

[0023] Figure 1 These are physical images of the surface plasmon nanostructures provided in Embodiments 1 and 2 of this invention.

[0024] Figure 2 These are scanning electron microscope images of the surface plasmon nanostructures provided in Embodiments 1 and 2 of this invention.

[0025] Figure 3 This is the basis for matching the emission position of the surface plasmon nanoresonator and the gain medium provided in Embodiments 1 and 2 of the present invention, where 1 refers to the emission spectrum of LDS 751 and 2 refers to the resonance peak of the surface plasmon nanoresonator used in this patent.

[0026] Figure 4 This is the nanolaser signal obtained by using LDS-751 as the gain medium to sense the increasing concentration of the gain medium, as provided in Embodiment 1 of the present invention.

[0027] Figure 5 This is a graph showing the change in intensity of a nanolaser signal as a function of concentration when using LDS-751 as the gain medium, as provided in Embodiment 1 of the present invention.

[0028] Figure 6 This is a schematic diagram of the surface mechanism of sensing double-stranded DNA using LDS-751@dsDNA as a gain medium, provided in Embodiment 2 of the present invention. 1 refers to 532nm continuous laser, 2 refers to LDS-751@dsDNA, 3 refers to surface plasmon nanoarray, and 4 refers to the excited nanolaser signal.

[0029] Figure 7 The laser signal sensing double-stranded DNA using LDS-751@dsDNA as the gain medium, as provided in Embodiment 2 of the invention, changes with the concentration of double-stranded DNA; the higher the concentration, the stronger the nanolaser signal.

[0030] Figure 8This is a graph showing the change in laser signal intensity as a function of concentration when using LDS-751@dsDNA as the gain medium to sense double-stranded DNA, as provided in Embodiment 2 of the invention. Detailed Implementation

[0031] To make the objectives, technical solutions, and advantages of this invention clearer, the invention will be further described in detail below with reference to the accompanying drawings and embodiments. It should be understood that the two specific embodiments described herein are merely illustrative and not intended to limit the invention.

[0032] I. The method for sensing changes in gain medium concentration using LDS-751 as the gain medium provided by this invention is as follows: Figure 4 As shown, the detailed steps are as follows:

[0033] (1) Using a silicon wafer as a substrate, a negative photoresist is spin-coated, and a plasmonic nanoarray structure is prepared by ultraviolet holographic lithography and a silver metal layer is deposited.

[0034] (2) Transfer 5 μL of LDS-751 (DMSO) solution onto the nanoarray in (1), cover it with a coverslip, and form a uniform liquid layer with a thickness of 6 μm.

[0035] (3) Nanolaser signals of LDS-751 (DMSO) solutions of different concentrations were acquired using a self-built nanolaser acquisition system, and the intensity versus concentration was plotted for analysis.

[0036] II. A method for sensing double-stranded DNA using LDS-751@dsDNA as a gain medium provided by this invention, as follows: Figure 5 As shown, the detailed steps are as follows:

[0037] (1) Using a silicon wafer as a substrate, a negative photoresist is spin-coated, and a plasmonic nanoarray structure is prepared by ultraviolet holographic lithography and a silver metal layer is deposited.

[0038] (2) Add LDS-751 stock solution to double-stranded DNA solution and incubate at room temperature for 10 min to allow LDS-751 molecules to enter the double-stranded DNA groove for labeling.

[0039] (3) Use a pipette to transfer 5 μL of LDS-751 labeled double-stranded DNA onto the surface of the structure, cover with a coverslip, and form a uniform liquid layer with a thickness of 6 μm.

[0040] (4) The nanolaser signals of LDS-751 labeled double-stranded DNA at different concentrations were collected in a self-built nanolaser acquisition system, and the intensity versus concentration was plotted for analysis.

[0041] In specific implementation examples, plasmon nanostructures with different morphologies can be prepared by changing the exposure conditions of ultraviolet holographic lithography, such as... Figure 2 As shown.

[0042] In specific implementation cases, different analytes can be detected by changing the luminescent material, such as... Figure 3 As shown.

[0043] In specific implementation cases, different microfluidic devices can be added to the surface of the structure to adapt to the requirements of different detection systems, such as... Figure 6 As shown.

[0044] In specific implementation cases, different luminescent material detection systems can be adapted by adding or removing different optical elements and the wavelength of the laser light source.

[0045] refer to Figure 1 and Figure 6 The method of this invention can be used to detect various suitable test objects on a chip of about one square centimeter and on a small detection device.

[0046] The above description is merely a preferred embodiment of the present invention and is not intended to limit the present invention. Any modifications, equivalent substitutions, and improvements made within the spirit and principles of the present invention should be included within the protection scope of the present invention.

Claims

1. A novel nanolaser sensing mechanism with ultra-high sensitivity and resolution, characterized in that, Includes the following steps: (1) The selection and matching of luminescent materials must meet the following requirements: they must be both a marker that can be used for luminescent sensing and a gain medium for nanolasers. (2) Energy level matching and optimization between the luminescent molecules used as nanolaser gain media and surface plasmon structures in all traditional sensing based on changes in luminescent signal intensity; (3) Obtaining nanolaser signals based on surface plasmon arrays and luminescent material systems; (4) Sensing based on nanolaser signals has higher sensitivity and resolution than traditional sensing based on changes in the intensity of light emission signals.

2. The preparation method according to claim 1, characterized in that, In steps (1, 2), the luminescent molecules include, but are not limited to, all conventional luminescent molecules in the 190-1000nm ultraviolet, visible and near-infrared bands.

3. The preparation method according to claim 1, characterized in that, In steps (2, 3), the method of using nanolaser gain medium includes spin coating, drop coating, surface self-assembly, specific bonding, surface potential and hydrophilic / hydrophobic adsorption on the surface of plasmonic nanostructure, and using a refractive index matching solution to attach the gain medium fixed on other substrates to the surface of the plasmonic nanoarray structure.

4. The preparation method according to claim 1, characterized in that, In steps (2, 3), the surface plasmon nanoarray includes gold and silver nanoarray structures prepared by holographic lithography, nanoimprint lithography, nanosphere lithography, and electron beam and focused ion beam etching methods.

5. The preparation method according to claim 1, characterized in that, In step (3), the nanolaser acquisition device used for nanolaser signal acquisition includes a continuous pump source, a filter, a polarizer, and a signal acquisition device.

6. The preparation method according to claim 1, characterized in that, In steps (3, 4), the nanolaser signal includes intensity, displacement, full width at half maximum (FWHM), and threshold, and the sensing of the substance to be tested includes sensing properties such as concentration, structural changes, and dynamic detection.

7. A novel nanolaser sensing mechanism with ultra-high sensitivity and resolution as described in claims 1-6, characterized in that: The process of converting photoluminescence signals into nanolaser signals involves stimulated emission amplification caused by surface plasmon nanooptic resonators, resulting in higher sensitivity than traditional luminescence intensity detection methods. Secondly, the laser signal is only a few nanometers long, which is significantly better than the fluorescence emission peak shape of tens of nanometers, thus providing higher resolution. This is a novel and high-performance sensing technology that will play an important role in fields such as life sciences, biomedicine, food safety, and environmental safety.

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