In-situ online low-temperature high-pressure ultrafast spectroscopy device, system and method thereof

Abstract

The application provides an online in-situ low-temperature high-pressure ultrafast spectroscopy device, a system and a method thereof. The high-pressure device comprises a cold shield with an optical window, a metal ring, a gasket, a first pressurized air bag, a second pressurized air bag, a pressurized metal column, a diamond anvil cell, a first temperature sensor, a second temperature sensor, a heat-conducting base, a cryostat and a gas pressure controller. The online in-situ pressure calibration and imaging system comprises a continuous light laser, the high-pressure device, online in-situ pressure optical components and an online in-situ pressure imaging system. The low-temperature high-pressure ultrafast pump-probe system comprises a femtosecond laser, the online in-situ pressure calibration and imaging system, pump-probe optical components and a pump-probe imaging system. The application realizes temperature regulation at 6-325K under high pressure with double air bag pressure regulation, realizes online in-situ free pressure regulation at low temperature, and realizes continuous regulation with an accuracy of 0.1GPa in the pressure range of 0-80GPa, and realizes online in-situ low-temperature high-pressure ultrafast spectroscopy and ultrafast dynamics measurement.

Description

TECHNICAL FIELD

[0001] The application belongs to the field of ultrafast spectroscopy, and particularly relates to an online in-situ low-temperature high-pressure ultrafast spectroscopy device, a system thereof and a method. BACKGROUND

[0002] Ultrafast spectroscopy technology is an important frontier in non-equilibrium condensed matter physics research. This technology is an important tool for studying ultrafast dynamic processes within condensed matter. It has high resolution and sensitivity, non-destructive, and non-contact characteristics, and therefore has wide application prospects in basic research, material science, industrial production, medical science, and other fields. The most basic ultrafast spectroscopy technology is pump-probe technology. The main principle of this technology is to first irradiate a substance with a pump laser, which pumps the substance into an excited state. After a certain delay, the sample is probed by another laser or other detection means, and information about the sample in the excited state, such as multi-degree of freedom coupling and non-equilibrium state relaxation, is obtained.

[0003] In order to study the properties of matter under different external conditions, such as temperature and pressure control, external temperature and pressure control are important technical means for studying material properties. In pressure control, online in-situ pressure adjustment high-pressure systems are of great significance for high-pressure spectroscopy testing. Online in-situ pressure adjustment means adjusting the pressure in the diamond anvil cell without moving the sample, which avoids the problems of low spectral signal stability and reproducibility caused by moving the diamond anvil cell out of the optical path. Among them, the gas bag in-situ pressure adjustment is a feasible online in-situ pressure adjustment method. Today, high-pressure systems compatible with spectroscopy testing focus on non-low-temperature online in-situ systems and non-gas bag in-situ pressure adjustment high-pressure systems. In non-low-temperature online in-situ systems, temperature control is not compatible, and spectroscopy testing of low-temperature samples cannot be achieved. In non-gas bag in-situ pressure adjustment systems, the pressure needs to be adjusted by compressing the diamond anvil cell with a motor or other means each time, which has low sample pressure control accuracy and affects some spectroscopy tests that are sensitive to the sample point and sample surface morphology, reducing the reliability of experimental data. Therefore, providing a low-temperature gas bag in-situ pressure adjustment high-pressure system compatible with spectroscopy testing and a testing method thereof will help to solve these problems of low-temperature high-pressure sample testing.

[0004] The high-pressure system compatible with the spectrum test is generally in the room temperature environment or uses the non-gasbag in-situ pressure regulating high-pressure technology, and is rarely used for the gasbag in-situ pressure regulating and low-temperature high-pressure and the superfast pumping detection technology. At present, in the existing technology, the low-temperature Brillouin scattering which realizes the in-situ high pressure, the in-situ high-pressure Raman spectrum test, the high-pressure superfast spectrum test which realizes the gasbag pressure regulating at room temperature and the high-pressure low-temperature superfast spectrum test which realizes the in-situ gasbag pressure regulating are partially realized. The gasbag pressure regulating technology compatible with the superfast spectrum test has important significance for the research on the physical properties of the substances at low temperature and high pressure, but there are some problems which are difficult to solve in the current technology, for example, the gasbag pressure regulating device can only be carried out at room temperature, and the pressure regulating at low temperature cannot be realized. For some quantum materials which have special properties at low temperature and high pressure, the superfast spectrum test cannot be carried out. In the high-pressure low-temperature technology using the gasbag pressure regulating, the free pressure increasing and decreasing cannot be realized, and the imaging quality is poor. So far, there is no device which can realize the low-temperature pressure regulating and the free pressure increasing and decreasing of the superfast pumping detection measurement.

[0005] Therefore, the low-temperature system and the gasbag pressure regulating high-pressure system are combined with each other to realize the free temperature regulation and the pressure increasing and decreasing, and are suitable for the superfast pumping detection system, and there are still some challenges, how to make the high-pressure and temperature regulation system compatible with each other, how to realize the free pressure increasing and decreasing regulation in the low-temperature system, how to calibrate the pressure at low temperature, and how to make the superfast pumping detection measurement compatible with each other. For realizing the low-temperature high-pressure superfast pumping detection at the liquid nitrogen and liquid helium temperature, the above problems need to be solved urgently. SUMMARY

[0006] Therefore, the purpose of the present application is to overcome the defects in the prior art, and to provide an online in-situ low-temperature high-pressure superfast spectrum device, a system and a method thereof. The double-gasbag in-situ pressure regulating high-pressure technology which has less influence on the sample point at low temperature is realized, the free pressure increasing and decreasing regulation with higher precision is realized, the pressure calibration method at low-temperature high pressure in the online in-situ low-temperature high-pressure is realized, and the superfast pumping detection experiment at low-temperature high pressure is realized.

[0007] Before the summary of the present application is described, the terms used in the present application are defined as follows:

[0008] The term "OPA" refers to: optical parametric amplifier.

[0009] The term "BBO crystal" refers to: barium borate crystal.

[0010] The term "LBO crystal" refers to: lithium triborate crystal.

[0011] The term "KDP crystal" refers to: potassium dihydrogen phosphate crystal.

[0012] The term "CCD camera" refers to: digital camera with charge-coupled device image sensor.

[0013] The term "CMOS camera" refers to a camera that is usually 10 times less sensitive than a CCD camera.

[0014] The term "Dewar" refers to a container and tool for storing liquefied gas, for low-temperature research, and for protecting crystal elements, etc.

[0015] The term "DAC" refers to a diamond anvil cell.

[0016] The term "on-site in situ" refers to a detection situation in which the sample is not removed from the light path, the sample position is not rotated, and the sample position is fixed. The English is "on-site in situ", that is, the detection is carried out in real time without moving and rotating the detected object in its original environment, so as to avoid the influence of reset error, that is, to avoid the influence of movement, rotation or change of detection environment on the result.

[0017] The term "Ultrafast Spectroscopy" refers to a technology for detecting dynamic changes of matter on an extremely short time scale using ultra-short laser pulses. The English is Ultrafast Spectroscopy, which can capture the physical and chemical changes of matter on an extremely short time scale of picoseconds, femtoseconds, attoseconds, etc.

[0018] The term "high pressure" refers to a working pressure greater than 101.325 kPa in the on-site in situ detection of ultrafast spectroscopy.

[0019] The term "low temperature" refers to a working temperature lower than 25℃ in the on-site in situ detection of ultrafast spectroscopy.

[0020] To achieve the above-mentioned purpose, the first aspect of the present application provides a low-temperature double-gas-bag pressure-regulating high-pressure device, comprising: a cold shield with an optical window, a metal ring, a gasket, a first pressurized gas bag, a second pressurized gas bag, a pressurized metal column, a diamond anvil cell pressure cavity, a first temperature sensor, a second temperature sensor, a heat-conducting base, a cryostat, and a gas pressure controller; wherein:

[0021] The metal ring fixes the gasket, the first pressurized gas bag, the second pressurized gas bag, the pressurized metal column, the diamond anvil cell pressure cavity, and the first temperature sensor on one side of the heat-conducting base;

[0022] The second temperature sensor is independent of the metal ring and is arranged on the other side of the heat-conducting base;

[0023] The heat-conducting base and the cold shield are fixed on the cryostat.

[0024] According to the high-pressure device of the first aspect of the present application, the high-pressure device further comprises a heating coil, and the heating coil is arranged on the same side of the heat-conducting base as the second temperature sensor; wherein,

[0025] The first temperature sensor is located outside the diamond anvil cell;

[0026] The pressurized metal cylinder is located between the gasket and the diamond anvil cell;

[0027] The first pressurized gas pocket and the second pressurized gas pocket are both connected with the gas pressure controller;

[0028] The metal ring comprises a first metal ring and a second metal ring, the first metal ring and the first gasket are preferably connected with the first pressurized gas pocket; and / or

[0029] The gasket comprises a first gasket and a second gasket, the second metal ring and the second gasket are preferably connected with the second pressurized gas pocket.

[0030] The high-pressure device according to the first aspect of the present application, wherein the high-pressure device further comprises a metal housing with another optical window, a vacuum pump for providing a vacuum environment, and a Dewar for providing a low-temperature environment; wherein,

[0031] The cold shield and the heat-conducting pedestal are located in a space composed of the metal housing and the cryostat; and / or

[0032] The vacuum pump is connected with the Dewar on the cryostat;

[0033] Preferably, the low-temperature environment of the high-pressure device is 6-325 K, more preferably 20-315 K, and further preferably 40-300 K;

[0034] Preferably, the high pressure of the high-pressure device is 0-80 GPa, more preferably 5-70 GPa, and further preferably 10-60 GPa;

[0035] Preferably, the diamond anvil in the diamond anvil cell is a shortened diamond anvil; and / or

[0036] Preferably, the Dewar is selected from one or more of the following: a low-temperature liquid nitrogen tank, a liquid nitrogen Dewar, a liquid helium Dewar, more preferably a liquid nitrogen Dewar or a liquid helium Dewar, and most preferably a liquid helium Dewar.

[0037] The second aspect of the present application provides an in-situ online pressure calibration and imaging system, which comprises:

[0038] The high-pressure device with low-temperature double-gas-pocket pressure regulation according to the first aspect;

[0039] A continuous laser;

[0040] An in-situ online pressure calibration optical component; and

[0041] An online in-situ sample topography imaging component;

[0042] The continuous laser emits laser light, which is focused on a ruby of the high-pressure device through an optical path built by the online in-situ pressure calibration optical component, and the optical path guides reflected light to the online in-situ sample topography imaging component to realize detection and calibration of the pressure value in the diamond anvil cell at different temperatures and pressures.

[0043] The online in-situ pressure calibration and imaging system according to the second aspect of the present application, wherein,

[0044] The wavelength of the continuous laser is selected from one or more of 532 nm, 633 nm, and 450 nm, preferably 532 nm or 633 nm, and most preferably 532 nm;

[0045] The online in-situ pressure calibration optical component is selected from one or more of a half-mirror, a mirror, a light source, a relay lens, a fiber coupler, and a long-focus microscope objective; and / or

[0046] The online in-situ sample topography imaging component is selected from one or more of a spectral analyzer, a camera, and a computer host;

[0047] Preferably, the long-focus microscope objective is selected from one or more of a 5x long-focus microscope objective, a 10x long-focus microscope objective, a 20x long-focus microscope objective, and a 50x long-focus microscope objective, more preferably a 10x long-focus microscope objective or a 20x long-focus microscope objective, and most preferably a 20x long-focus microscope objective; and / or

[0048] Preferably, the camera is selected from one or more of a CCD camera, a CMOS camera, and a single-lens reflex camera, more preferably a CCD camera and / or a CMOS camera, and most preferably a CCD camera.

[0049] The third aspect of the present application provides a low-temperature high-pressure ultrafast pumping and detection system, which comprises:

[0050] The online in-situ pressure calibration and imaging system according to the second aspect;

[0051] A femtosecond laser;

[0052] A pumping and detection optical component; and

[0053] A pumping and detection imaging component;

[0054] The femtosecond laser emits femtosecond laser, and the light path built by the pump-probe optical component is divided into two beams of light, which are focused into the low-temperature double-bag pressure-regulating high-pressure device, the light path guides the reflected light into the pump-probe imaging component, and the temperature and pressure of the sample are regulated by the high-pressure device, so that the ultrafast pump-probe of the sample under different temperature and pressure is realized.

[0055] The low-temperature high-pressure ultrafast pump-probe system according to the third aspect of the present application, wherein,

[0056] The pump-probe optical component is selected from one or more of the following: a semi-transmissive and semi-reflective mirror, a delay line, a mirror, a chopper, an OPA, a filter, a focusing lens, a long-focus microscope objective, a light source, a lock-in amplifier, a crystal, a relay lens, and a fiber coupler; and / or

[0057] The pump-probe imaging component is selected from one or more of the following: a CCD camera, a differential probe, a computer host, and a display screen.

[0058] Preferably, the long-focus microscope objective is selected from one or more of the following: a 5-fold long-focus microscope objective, a 10-fold long-focus microscope objective, a 20-fold long-focus microscope objective, and a 50-fold long-focus microscope objective, more preferably selected from one or more of the following: a 5-fold long-focus microscope objective, a 10-fold long-focus microscope objective, and a 20-fold long-focus microscope objective, and most preferably a 10-fold long-focus microscope objective.

[0059] Preferably, the camera is selected from one or more of the following: a CCD camera, a CMOS camera, and a single-lens reflex camera, more preferably a CCD camera and / or a CMOS camera, and most preferably a CCD camera.

[0060] Preferably, the filter is a 400 nm filter and / or an 800 nm filter; and / or

[0061] Preferably, the crystal is selected from one or more of the following: a BBO crystal, an LBO crystal, and a KDP crystal, preferably a BBO crystal or an LBO crystal, and most preferably a BBO crystal.

[0062] The fourth aspect of the present application provides a temperature regulation method under high pressure, which comprises using the low-temperature double-bag pressure-regulating high-pressure device according to the first aspect.

[0063] Preferably, the temperature regulation method comprises the following steps: transferring heat through the heat-conducting base and the diamond anvil cell, monitoring the temperature of the heat-conducting base and the temperature of the sample through two temperature sensors, and regulating the temperature of the low-temperature thermostat by controlling the flow rate of the Dewar and the power of the heating coil to regulate the temperature of the sample under high pressure.

[0064] The fifth aspect of the present application provides a method for in-situ pressure regulation at low temperature, which comprises using:

[0065] the high-pressure device for low-temperature double-bag pressure regulation of the first aspect, or

[0066] the in-situ pressure calibration and imaging system of the second aspect;

[0067] Preferably, the method for in-situ pressure regulation at low temperature comprises the following steps: filling the first pressurized gas bag and the second pressurized gas bag with inert gas through the gas pressure controller, compressing and stretching the diamond anvil cell in the diamond anvil cell to realize free increase or decrease of the hydrostatic pressure provided to the sample, and measuring the pressure in the diamond anvil cell in the cryostat through the in-situ pressure calibration and imaging system to realize in-situ pressure regulation at low temperature.

[0068] The sixth aspect of the present application provides a method for ultrafast spectroscopy pump-probe at low temperature and high pressure, which comprises using:

[0069] the high-pressure device for low-temperature double-bag pressure regulation of the first aspect,

[0070] the in-situ pressure calibration and imaging system of the second aspect, or

[0071] the low-temperature high-pressure ultrafast pump-probe system of the third aspect;

[0072] Preferably, the method for ultrafast spectroscopy pump-probe at low temperature and high pressure comprises the following steps: adjusting the optical path to align the pump-probe laser emitted by the femtosecond laser to the long-focus microscopic objective lens, and then to the sample surface through the optical window of the cold shield in front of the low-temperature double-bag pressure regulation high-pressure device to realize ultrafast pump-probe of the sample at different temperatures and pressures.

[0073] More preferably, the method for ultrafast spectroscopy pump-probe at low temperature and high pressure further comprises the following steps:

[0074] 1) loading the sample into the high-pressure device and placing it into the optical path;

[0075] 2) adjusting the temperature and pressure of the sample, and measuring the calibration pressure through the in-situ pressure calibration and imaging system; and

[0076] 3) performing pump-probe measurement through the low-temperature high-pressure ultrafast pump-probe system.

[0077] According to one preferred embodiment of the present application, the present application provides a low-temperature double-bag pressure-regulated high-pressure device, which comprises a metal shell with an optical window, a metal ring, a gasket, a first pressurized gas bag, a second pressurized gas bag, a pressurized metal column, a shortened diamond anvil cell, a first temperature sensor, a second temperature sensor, a cold shield with an optical window, a heating coil, a heat-conducting base, a gas pressure controller, a cryostat, a vacuum pump, and a liquid nitrogen / liquid helium Dewar; wherein:

[0078] Inside the low-temperature double-bag pressure-regulated high-pressure device, the gasket, the pressurized gas bag, the pressurized metal column, the shortened diamond anvil cell, and the first temperature sensor are fixed on the heat-conducting base by the metal ring, the pressurized metal column is located between the pressurized gas bag and the shortened diamond anvil cell, the pressurized gas bag is connected to the gas pressure controller, and the first temperature sensor is located outside the shortened diamond anvil cell. The cold shield is installed on the heat-conducting base, the second temperature sensor is installed outside the heat-conducting base, the heating coil is installed at the bottom of the heat-conducting base, and the heat-conducting base is installed in the cryostat. The cold shield with an optical window and the heat-conducting base are located in a space composed of the metal shell with an optical window and the cryostat. The vacuum pump and the liquid nitrogen / liquid helium Dewar are connected to the cryostat to provide a high-vacuum and low-temperature environment for the device.

[0079] Preferably, the diamonds of the shortened diamond anvil are selected from one or more of the following: diamonds with a platform mesa diameter of 400 μm, diamonds with a platform mesa diameter of 300 μm, diamonds with a platform mesa diameter of 200 μm, more preferably selected from one or more of the following: diamonds with a platform mesa diameter of 200 μm, diamonds with a platform mesa diameter of 300 μm, and further selected from one or more of the following: diamonds with a platform mesa diameter of 300 μm.

[0080] According to another preferred embodiment of the present application, the present application provides a pressure calibration and imaging system, which comprises the low-temperature double-bag pressure-regulated high-pressure device of the first aspect, a relay lens, a 20-fold long-focus microscope objective, a 532 nm continuous light solid-state laser, a CCD camera, light rays, a spectral analyzer, a half-mirror, and a mirror; wherein:

[0081] A sample cavity is provided in the shortened diamond anvil cell, and the sample is preferably placed at the ruby beside the sample cavity in the shortened diamond anvil cell;

[0082] The light path is built by the mirror and the half-mirror, the 532nm continuous light laser is focused on the ruby in the shortened diamond anvil cell by the 20 times long-focus microscope objective and the relay lens, and the reflected light is guided into the CCD camera and the spectrum analyzer. The sample surface is imaged by the CCD, the sample condition is monitored, and the sample point irradiated by the laser is observed. The pressure in the diamond anvil cell is measured by the displacement of the ruby fluorescence peak caused by temperature and pressure.

[0083] According to still another preferred embodiment of the present application, the present application provides a method for in-situ pressure regulation at low temperature, which comprises the low-temperature double-bag pressure-regulating high-pressure device of the first aspect and the pressure calibration and imaging system of the second aspect.

[0084] The principle of the test method is as follows: according to the device of the first aspect and the second aspect of the present application, the diamond anvil cell is compressed and stretched by filling the pressurized gas bag with high-purity inert gas such as helium / nitrogen through the air pressure controller, so as to freely increase or decrease the hydrostatic pressure provided to the sample. The pressure in the diamond anvil cell in the cryostat is measured by the pressure calibration and imaging system. Finally, the in-situ pressure regulation at low temperature is realized.

[0085] According to still another preferred embodiment of the present application, the present application provides a method for temperature regulation at high pressure, which comprises the low-temperature double-bag pressure-regulating high-pressure device of the first aspect.

[0086] Heat is transferred through the heat-conducting base and the diamond anvil cell pressure cavity, the heat-conducting base and the sample temperature are monitored by two temperature sensors, and the sample temperature is regulated by controlling the flow of liquid nitrogen / liquid helium and the power of the heating coil. Finally, the temperature regulation at high pressure is realized.

[0087] According to still another preferred embodiment of the present application, the present application provides an ultrafast spectroscopy experimental method at low temperature and high pressure, which comprises the low-temperature double-bag pressure-regulating high-pressure device of the first aspect and the pressure calibration and imaging system of the second aspect, and a set of ultrafast pump-probe system.

[0088] The temperature and pressure of the sample are regulated by the low-temperature double-bag pressure-regulating high-pressure device and the pressure calibration and imaging system, the pump-probe laser is aligned to enter the 10 times long-focus microscope objective through light path adjustment, and then enters the sample surface from the optical window in front of the low-temperature double-bag pressure-regulating high-pressure device, so as to realize the ultrafast pump-probe of the sample at different temperatures and pressures.

[0089] Compared with the prior art, the low-temperature high-pressure ultrafast pump-probe system of the present application has the following settings:

[0090] (1) Adding a diamond anvil cell pressure chamber in a cryostat.

[0091] (2) Adding a (double) gas membrane driven online in-situ high pressure pressure regulation in a cryostat.

[0092] (3) A shortened diamond anvil cell high pressure press pressure chamber suitable for a cryostat.

[0093] (4) Installing a heat-conducting base in a cryostat for temperature regulation and detection of heating and cooling of a diamond anvil cell.

[0094] (5) Placing an online in-situ time-resolved ultrafast pump-probe system outside a cryostat.

[0095] (6) Placing an online in-situ high pressure pressure calibration and imaging system outside a cryostat.

[0096] (7) Placing an online in-situ relay lens (Rely lens) confocal imaging monitoring system outside a cryostat.

[0097] The low-temperature high-pressure ultrafast pump-probe system of the present application, as a set of ultrafast pump-probe test experimental system, is used for studying the ultrafast dynamics characteristics of materials under low-temperature high-pressure.

[0098] As a low-temperature spectral measurement system, it is used for various spectral tests at low temperature, and for various instrument processing or material growth at low temperature.

[0099] As a high-pressure system, it is used for various spectral test means and device design with free pressure increasing and decreasing regulation requirements.

[0100] The low-temperature high-pressure ultrafast pump-probe system of the present application realizes online in-situ ultrafast spectral experiment. The sample under the condition of 6-325K and 0-80GPa can be measured by pump-probe ultrafast spectral measurement.

[0101] Compared with the prior art, the online in-situ low-temperature high-pressure ultrafast spectral device, system and method of the present application can have the following beneficial effects, but are not limited to:

[0102] (1) The temperature regulation of 6-325K under high pressure by double gas bag pressure regulation is realized.

[0103] (2) The online in-situ free pressure increasing and decreasing regulation under low temperature is realized, and the pressure is continuously regulated with an accuracy of 0.1GPa in the range of 0-80GPa.

[0104] (3) The online in-situ low-temperature high-pressure ultrafast spectral and ultrafast dynamics measurement is realized. BRIEF DESCRIPTION OF DRAWINGS

[0105] Embodiments of the present application will be described in detail below with reference to the drawings, in which:

[0106] Figure 1 A structural diagram of a high-pressure device with low-temperature double-bag pressure regulation in Example 1 is shown.

[0107] Figure 2 A structural diagram of an in-situ pressure calibration and imaging system in Example 2 is shown.

[0108] Figure 3 A structural diagram of a low-temperature high-pressure ultrafast pump-probe system in Example 3 is shown.

[0109] Figure 4 A structural diagram of a low-temperature high-pressure ultrafast pump-probe system in Example 4 is shown.

[0110] Figure 5 Results of a sample under test in a CCD camera at different temperatures and pressures are shown; wherein, Figure 5 A shows results of a layered iron-based superconducting sample under test at 78K, 25.552GPa; Figure 5 B shows results of a layered iron-based superconducting sample under test at 300K, 2.27GPa.

[0111] Figure 6 A ruby photoluminescence spectrum at a temperature of 13.25K is shown, and by comparing the movement of the photoluminescence spectrum peak position at normal temperature and pressure, the pressure at this time is obtained as 20.81GPa.

[0112] Figure 7 Pump-probe data of an ultrafast spectrum of a layered iron-based superconducting sample at a pressure of 13.7GPa, 8.5K and 20K are shown.

[0113] BRIEF DESCRIPTION OF DRAWINGS

[0114] 2, cold shield with optical window; 1, metal housing with another optical window; 3, first metal ring with first gasket and first pressurized air bag; 4, pressurized metal cylinder; 5, diamond anvil cell; 6, first temperature sensor; 7, sample and ruby; 8, second metal ring with second gasket and second pressurized air bag; 9, second temperature sensor; 10, heating coil; 11, heat conducting pedestal; 12, cryostat; 13, vacuum pump; 14, dewar; 15, air pressure controller; 16, low temperature double air bag pressure regulating high pressure device; 17, relay lens; 18, 20x long focal length microscope objective; 19, first pellicle mirror; 20, second pellicle mirror; 21, fiber coupler; 22, optical spectrum analyzer; 23, first CCD camera; 24, computer host; 25, third pellicle mirror; 26, first mirror; 27, light source; 28, 532nm continuous wave laser; 29, femtosecond laser; 30, fourth pellicle mirror; 31, delay line; 32, second mirror; 33, third mirror; 34, chopper; 35, OPA; 36, 400nm filter; 37, fourth mirror; 38, fifth pellicle mirror; 39, sixth pellicle mirror; 40, seventh pellicle mirror; 41, fifth mirror; 42, 800nm filter; 43, first focusing lens; 44, differential detector; 45, second focusing lens; 46, second CCD camera; 47, 10x long focal length microscope objective; 48, lock-in amplifier; 49, third focusing lens; 50, BBO crystal; 51, fourth focusing lens. DETAILED DESCRIPTION

[0115] The application will be further described in conjunction with the drawings, through specific examples, but it should be understood that these examples are only for more detailed and specific description, and should not be understood as limiting the application in any form.

[0116] This part generally describes the materials and test methods used in the test of the application. Although many materials and operating methods used to achieve the purpose of the application are well known in the art, the application is described as much as possible. It is clear to those skilled in the art that if not specifically described, the materials and operating methods used in the application are well known in the art.

[0117] Example 1

[0118] This example is an exemplary description of the low temperature double air bag pressure regulating high pressure device of the application.

[0119] As Figure 1As shown, the high-pressure device for low-temperature dual-bladder pressure regulation of the present invention includes: a cold screen 2 with an optical window; a metal shell 1 with another optical window; a first metal ring and a first gasket and a first pressurizing airbag 3; a pressurizing metal column 4; a diamond anvil chamber 5; a first temperature sensor 6; a sample and a ruby ​​7; a second metal ring and a second gasket and a second pressurizing airbag 8; a second temperature sensor 9; a heating coil 10; a heat-conducting base 11; a low-temperature thermostat 12; a vacuum pump 13; a Dewar 14; and a pressure controller 15.

[0120] The diamond anvil cell in this embodiment is a shortened diamond anvil cell.

[0121] Inside the high-pressure device with dual-bladder pressure regulation at low temperature, a first gasket, a second gasket, a first pressurizing airbag, a second pressurizing airbag, a pressurizing metal column, a shortened diamond anvil chamber, and a first temperature sensor are fixed in the heat-conducting base by a first metal ring and a second metal ring. The pressurizing metal column is located between the first pressurizing airbag and the diamond anvil chamber. The first and second pressurizing airbags are connected to the pressure controller. The first temperature sensor is located outside the shortened diamond anvil chamber. A cold screen is mounted on the heat-conducting base, and the second temperature sensor is mounted on the outside of the heat-conducting base. The heat-conducting base and the cold screen are fixed inside the cryogenic thermostat. The cold screen with an optical window and the heat-conducting base are located in the space formed by the metal shell with the optical window and the cryogenic thermostat. The vacuum pump and liquid nitrogen / liquid helium Dewar are connected to the cryogenic thermostat to provide a high vacuum and low temperature environment for the device. This embodiment uses a liquid helium Dewar as an example.

[0122] Example 2

[0123] This embodiment is an exemplary description of the online in-situ pressure calibration and imaging system of the present invention.

[0124] like Figure 2 As shown, the pressure calibration and imaging system of the present invention includes: a low-temperature dual-gasbag pressure regulating high-pressure device 16 as described in Example 1, a 532nm continuous light laser 28, an online in-situ pressure calibration optical component, and an online in-situ sample appearance imaging component. The 532nm continuous light laser emits a 532nm laser beam, which is focused onto the ruby ​​of the high-pressure device through an optical path constructed by the online in-situ pressure calibration optical component. The optical path guides the reflected light to the online in-situ sample appearance imaging component, thereby achieving the detection and calibration of the pressure values ​​within the diamond anvil cell under different temperatures and pressures.

[0125] The online in-situ pressure calibration optical component in the embodiment takes a half-transmission half-reflection mirror, a mirror, a light source, a relay lens, a long-focus microscopic objective, and a fiber coupler as examples. The online in-situ sample appearance imaging component takes a CCD camera, a spectrum analyzer, and a computer host as examples. The long-focus microscopic objective takes a 20-fold long-focus microscopic objective as an example, and the CCD camera takes a resolution of 5496*3672 color CCD camera as an example.

[0126] The ruby is placed in the high-pressure device, the 532nm continuous light laser emits 532nm laser, the light path built by the optical component is focused on the ruby, the light path guides the reflected light into the online in-situ sample appearance imaging component, so as to realize the detection and calibration of the pressure value in the diamond anvil cell under different temperatures and pressures.

[0127] The optical path of the embodiment takes the light path of Figure 2 The 532nm laser 28 emits laser light, which is reflected by the third half-transmission half-reflection mirror 25. The light source 27 provides white light, which is reflected by the first mirror 26 and the third half-transmission half-reflection mirror 25, and is focused on the sample to be measured and the ruby 7 through the first half-transmission half-reflection mirror 19, the 20-fold long-focus microscopic objective 18, and the relay lens 17. The reflected light is guided into the first CCD camera 23 and the spectrum analyzer 22. The first CCD camera 23 can be used to image the sample surface, monitor the sample condition, and observe the sample point irradiated by the laser. The spectrum analyzer 22 is used to analyze the ruby fluorescence peak. The light source 27 in the light path provides illumination for the CCD camera to monitor the sample surface. The laser provides laser irradiation for the ruby. The spectrum analyzer is used to analyze the shift of the ruby fluorescence peak under different pressures and temperatures. Finally, the pressure detection is realized.

[0128] Example 3

[0129] The embodiment is an exemplary description of the low-temperature high-pressure ultrafast pumping detection system of the application.

[0130] The low-temperature high-pressure ultrafast pumping detection system of the application comprises the pressure calibration and imaging system described in Embodiment 2, a femtosecond laser 29, a pumping detection optical component, and a pumping detection imaging component. The sample to be measured is placed in the high-pressure device, the femtosecond laser emits femtosecond laser, and the light path built by the pumping detection optical component is focused into the high-pressure device in two beams. The light path guides the reflected light into the pumping detection imaging component. The temperature and pressure of the sample to be measured are adjusted by the high-pressure device and the pressure chamber calibration system, so as to realize the ultrafast pumping detection of the sample under different temperatures and pressures.

[0131] The pump-probe optical components are exemplified by a half-transmission half-reflection mirror, a delay line, a mirror, a chopper, an OPA, a filter, a focusing lens, a long-focus microscope objective, a light source, and a lock-in amplifier. The pump-probe imaging components are exemplified by a CCD camera, a differential detector, and a computer host. The long-focus microscope objective is exemplified by a 10-fold long-focus microscope objective, and the camera is exemplified by a color CCD camera with a resolution of 5496 x 3672.

[0132] The pump-probe optical components are exemplified by a half-transmission half-reflection mirror, a delay line, a mirror, a chopper, an OPA, a filter, a focusing lens, a long-focus microscope objective, a light source, and a lock-in amplifier. The pump-probe imaging components are exemplified by a CCD camera, a differential detector, and a computer host. The long-focus microscope objective is exemplified by a 10-fold long-focus microscope objective, and the camera is exemplified by a color CCD camera with a resolution of 5496 x 3672. Figure 3 The pump-probe optical components are exemplified by a half-transmission half-reflection mirror, a delay line, a mirror, a chopper, an OPA, a filter, a focusing lens, a long-focus microscope objective, a light source, and a lock-in amplifier. The pump-probe imaging components are exemplified by a CCD camera, a differential detector, and a computer host. The long-focus microscope objective is exemplified by a 10-fold long-focus microscope objective, and the camera is exemplified by a color CCD camera with a resolution of 5496 x 3672.

[0133] Example 4

[0134] The pump-probe optical components are exemplified by a half-transmission half-reflection mirror, a delay line, a mirror, a chopper, an OPA, a filter, a focusing lens, a long-focus microscope objective, a light source, and a lock-in amplifier. The pump-probe imaging components are exemplified by a CCD camera, a differential detector, and a computer host. The long-focus microscope objective is exemplified by a 10-fold long-focus microscope objective, and the camera is exemplified by a color CCD camera with a resolution of 5496 x 3672.

[0135] The pump-probe optical components are exemplified by a half-transmission half-reflection mirror, a delay line, a mirror, a chopper, an OPA, a filter, a focusing lens, a long-focus microscope objective, a light source, and a lock-in amplifier. The pump-probe imaging components are exemplified by a CCD camera, a differential detector, and a computer host. The long-focus microscope objective is exemplified by a 10-fold long-focus microscope objective, and the camera is exemplified by a color CCD camera with a resolution of 5496 x 3672.

[0136] The pump-probe optical components are exemplified by a half-transmission half-reflection mirror, a delay line, a mirror, a chopper, an OPA, a filter, a focusing lens, a long-focus microscope objective, a light source, and a lock-in amplifier. The pump-probe imaging components are exemplified by a CCD camera, a differential detector, and a computer host. The long-focus microscope objective is exemplified by a 10-fold long-focus microscope objective, and the camera is exemplified by a color CCD camera with a resolution of 5496 x 3672. Figure 4For example, the light path of the fourth half-transmission half-reflection mirror 30 is divided into two light paths by the fourth half-transmission half-reflection mirror 30. One light path passes through the delay line 31 and is focused on the surface of the sample to be measured by the 10-fold long-focus microscope objective 47. The other light path passes through the chopper 34, the third focusing lens 49, the BBO crystal 50, the fourth focusing lens 51, the 400 nm filter 36, the fourth mirror 37, and is focused on the same point of the sample to be measured by the long-focus microscope objective 47. The reflected light enters the differential detector 44 through the light path. The light source irradiates the surface of the sample to be measured through the light path, and the reflected light enters the second CCD camera 46 through the light path. The pressure calibration and imaging system light path is placed on the right side of the high-pressure device.

[0137] Example 5

[0138] The embodiment is used to illustrate the method for temperature regulation under high pressure of the low-temperature double-bag pressure-regulating high-pressure device of the application.

[0139] According to the low-temperature double-bag pressure-regulating high-pressure device of embodiment 1, heat is transferred from the heat-conducting base to the diamond anvil cell through the heat-conducting base and the two temperature sensors to monitor the temperature of the heat-conducting base and the sample to be measured. The temperature of the sample to be measured is regulated by controlling the flow of liquid nitrogen and liquid helium and the power of the heating coil. Finally, the temperature regulation under high pressure is realized.

[0140] Example 6

[0141] The embodiment is used to illustrate the method for online in-situ pressure regulation at low temperature of the online in-situ pressure calibration and imaging system of the application.

[0142] According to the online in-situ pressure calibration and imaging system of embodiment 2, the diamond anvil cell is compressed and stretched by filling high-purity inert gas helium into the pressurized gas bag through the air pressure controller, so as to freely increase or decrease the hydrostatic pressure provided to the sample to be measured. The pressure in the diamond anvil cell in the cryostat is measured by the pressure calibration and online in-situ sample appearance imaging component. Finally, the online in-situ pressure regulation at low temperature is realized.

[0143] In combination with embodiments 5 and 6, Figure 5 The results of the sample to be measured in the CCD camera under different temperatures and pressures are shown; wherein, Figure 5 A shows the image of the layered iron-based superconducting sample to be measured under 25.552 GPa; Figure 5 B shows the image of the layered iron-based superconducting sample to be measured under 2.27 GPa.

[0144] Figure 6The ruby photoluminescence spectrum at 13.25 K is shown, and the pressure is 20.81 GPa by comparing the movement of the photoluminescence spectrum peak position at normal temperature and pressure.

[0145] Example 7

[0146] This example is used to illustrate the low-temperature in-situ online pumping and detection measurement of the low-temperature high-pressure ultrafast pumping and detection system of the application.

[0147] According to the low-temperature high-pressure ultrafast pumping and detection system of embodiments 3 and 4, the temperature and pressure of the sample are regulated by the high-pressure device of the low-temperature double-bag pressure regulation and the pressure calibration and imaging system, and by adjusting the optical path, the pumping and detection laser is aligned to enter the 10-fold long-focus microscopic objective lens, and then is incident on the sample surface from the optical window of the cold shield in front of the low-temperature double-bag pressure regulation and high-pressure device, so that the ultrafast pumping and detection of the sample at different temperatures and pressures can be realized.

[0148] This example takes a layered iron-based superconducting sample as an example. First, the vacuum pump is opened at 300 K to make the sample chamber a high vacuum environment -5 Pa, and the vacuum degree reaches 10 -5 Pa, and then the sample chamber is cooled, and after reaching the test temperature 20 K, it is kept at 20 K. The pressure of the sample chamber is regulated to 13.7 GPa by the air pressure controller. The pumping and detection test of the sample is carried out. The same steps are taken to carry out the pumping and detection test of the sample at 8.5 K and 13.7 GPa.

[0149] Figure 7 The pumping and detection data of the ultrafast spectrum of the layered iron-based superconducting sample at 8.5 K and 20 K under a pressure of 13.7 GPa are shown.

[0150] Comparative Example

[0151] This comparative example is used to compare the prior art and the low-temperature double-bag pressure regulation high-pressure device, online in-situ pressure calibration and imaging system, and low-temperature high-pressure ultrafast pumping and detection system of the application.

[0152] Comparative example 1: composed of a single-bag high-pressure device, a pressure calibration and imaging system, and an ultrafast pumping and detection system.

[0153] Comparative example 2: composed of a single-bag high-pressure sample chamber and a spectrometer.

[0154] Comparative example 3: includes a laser, a Brillouin optical path system, a vacuum high-pressure sample containing system, a signal acquisition and processing system, and a vacuum high-pressure sample containing system and a cooling system.

[0155] Comparative Example 4: comprising: a laser light source, an objective lens acquisition system, a Raman spectrometer; the main structure of the Raman spectrometer has a slit, a monochromator, a grating and a charge coupled device, there is a laser switching system between the objective lens acquisition system and the Raman spectrometer, and there is a high-voltage system at the end of the objective lens acquisition system.

[0156] As shown in Table 1, compared with the prior art, the low-temperature double-bag pressure regulating high-pressure device, the low-temperature high-pressure ultrafast pumping detection system of the application can realize online in-situ calibration of pressure at low temperature, realize free pressure regulation of double-bag at low temperature, and realize temperature regulation at high pressure, and the device is applied to ultra-pumping detection measurement.

[0157] Table 1 Comparison of prior art and low-temperature double-bag pressure regulating high-pressure device, online in-situ pressure calibration and imaging system, and low-temperature high-pressure ultrafast pumping detection system of the application

[0158]

[0159] Although the effects of some embodiments are shown above, those skilled in the art should understand that according to the concept of the application, the foregoing other embodiments not specifically showing the effects or other technical solutions of the application not shown in the embodiments can also achieve the following technical effects declared in the summary of the application as comparable to the embodiments:

[0160] (1) Temperature regulation at 6-325K under high pressure of double-bag pressure regulating is realized.

[0161] (2) Free pressure regulation at low temperature is realized, and the pressure is continuously regulated in the range of 0-80GPa with an accuracy of 0.1GPa.

[0162] (3) Ultrafast spectroscopy and ultrafast dynamics measurement under online in-situ low temperature and high pressure are realized.

[0163] Although the application has been described to a certain extent, it is obvious that appropriate changes can be made to various conditions without departing from the spirit and scope of the application. It can be understood that the application is not limited to the described embodiments, but is subject to the scope of the claims, which includes equivalent replacements of each factor described.

Claims

1. An online in-situ pressure calibration and imaging system, comprising: The online in-situ pressure calibration and imaging system comprises: a high-pressure device with low-temperature double-bag pressure regulation; a continuous laser; an online in-situ pressure calibration optical component; and an online in-situ sample topography imaging component; wherein the continuous laser emits laser light, which is focused on a ruby in the high-pressure device through an optical path established by the online in-situ pressure calibration optical component, and the optical path guides reflected light to the online in-situ sample topography imaging component to achieve detection and calibration of pressure values in a diamond anvil cell at different temperatures and pressures; and the high-pressure device comprises a cold shield with an optical window, a metal ring, a gasket, a first pressurized gas bag, a second pressurized gas bag, a pressurized metal column, a diamond anvil cell pressure cavity, a first temperature sensor, a second temperature sensor, a heat-conducting base, a cryostat, and a gas pressure controller; wherein the metal ring fixes the gasket, the first pressurized gas bag, the second pressurized gas bag, the pressurized metal column, the diamond anvil cell pressure cavity, and the first temperature sensor on one side of the heat-conducting base; the second temperature sensor is independent of the metal ring and is arranged on the other side of the heat-conducting base; and the heat-conducting base and the cold shield are fixed on the cryostat.

2. The online in-situ pressure calibration and imaging system of claim 1, wherein, The high-pressure device further comprises a heating coil, and the heating coil is arranged on the same side of the heat-conducting base as the second temperature sensor; wherein the first temperature sensor is located outside the diamond anvil cell pressure cavity; the pressurized metal column is located between the gasket and the diamond anvil cell pressure cavity; the first pressurized gas bag and the second pressurized gas bag are connected to the gas pressure controller; and / or the metal ring comprises a first metal ring and a second metal ring, and the gasket comprises a first gasket and a second gasket; the first metal ring and the first gasket are connected to the first pressurized gas bag, and the second metal ring and the second gasket are connected to the second pressurized gas bag.

3. The online in-situ pressure calibration and imaging system of claim 1, wherein, The high-pressure device further comprises a metal shell with another optical window, a vacuum pump for providing a vacuum environment, and a Dewar for providing a low-temperature environment; wherein the cold shield and the heat-conducting base are located in a space composed of the metal shell and the cryostat; and / or the vacuum pump and the Dewar are connected to the cryostat.

4. The online in-situ pressure calibration and imaging system according to claim 3, wherein: the low-temperature environment of the high-pressure device is 6-325 K; the high pressure of the high-pressure device is 0-80 GPa; the diamond anvil in the diamond anvil cell pressure cavity is a shortened diamond anvil; and / or the Dewar is selected from one or more of the following: a low-temperature liquid nitrogen tank, a liquid nitrogen Dewar, and a liquid helium Dewar.

5. The online in-situ pressure calibration and imaging system according to claim 4, wherein: the low-temperature environment of the high-pressure device is 20-315 K; the high pressure of the high-pressure device is 5-70 GPa; and / or the Dewar is a liquid nitrogen Dewar or a liquid helium Dewar.

6. The online in-situ pressure calibration and imaging system according to claim 5, wherein: the low-temperature environment of the high-pressure device is 40-300 K; The high pressure of the high-pressure device is 10-60 GPa; and / or The Dewar is a liquid helium Dewar.

7. The in-situ pressure calibration and imaging system according to any one of claims 1-6, wherein: The wavelength of the continuous laser is selected from one or more of: 532 nm, 633 nm, 450 nm; The in-situ pressure calibration optical components are selected from one or more of: a half-mirror, a mirror, a light source, a relay lens, a fiber coupler, a long-focus microscope objective; and / or The in-situ sample topography imaging components are selected from one or more of: a spectrometer, a camera, a computer host.

8. The online in-situ pressure calibration and imaging system of claim 7, wherein, The wavelength of the continuous laser is 532 nm or 633 nm.

9. The online in-situ pressure calibration and imaging system of claim 8, wherein, The wavelength of the continuous laser is 532 nm.

10. The in-situ pressure calibration and imaging system according to claim 7, wherein: The long-focus microscope objective is selected from one or more of: a 5x long-focus microscope objective, a 10x long-focus microscope objective, a 20x long-focus microscope objective, a 50x long-focus microscope objective; and / or The camera is selected from one or more of: a CCD camera, a CMOS camera, a single-lens reflex camera.

11. The in-situ pressure calibration and imaging system according to claim 10, wherein: The long-focus microscope objective is a 10x long-focus microscope objective or a 20x long-focus microscope objective; and / or The camera is a CCD camera and / or a CMOS camera.

12. The in-situ pressure calibration and imaging system according to claim 11, wherein: The long-focus microscope objective is a 20x long-focus microscope objective; and / or The camera is a CCD camera.

13. A cryogenic high pressure ultrafast pump probe system, characterized in that, The low-temperature high-pressure ultrafast pump-probe system comprises: The in-situ pressure calibration and imaging system according to any one of claims 1-12; a femtosecond laser; pump-probe optical components; and pump-probe imaging components; wherein the femtosecond laser emits femtosecond laser light, the optical path set up by the pump-probe optical components is divided into two beams of light, and the two beams of light are focused together into the low-temperature double-bag pressure-regulated high-pressure device, the optical path guides reflected light into the pump-probe imaging components, and the temperature and pressure of the sample are regulated by the high-pressure device to achieve ultrafast pump-probe of the sample at different temperatures and pressures.

14. The low-temperature high-pressure ultrafast pump-probe system according to claim 13, wherein: The pump-probe optical components are selected from one or more of: a half-mirror, a delay line, a mirror, a chopper, an OPA, a filter, a focusing lens, a long-focus microscope objective, a light source, a lock-in amplifier, a crystal, a relay lens, a fiber coupler; and / or The pump-probe imaging components are selected from one or more of: a CCD camera, a differential detector, a computer host, a display screen.

15. The low-temperature high-pressure ultrafast pump-probe system according to claim 14, wherein: The long-focus microscope objective is selected from one or more of: a 5x long-focus microscope objective, a 10x long-focus microscope objective, a 20x long-focus microscope objective, a 50x long-focus microscope objective; The camera is selected from one or more of: a CCD camera, a CMOS camera, a single-lens reflex camera; The filter is a 400 nm filter and / or an 800 nm filter; and / or The crystal is selected from one or more of: a BBO crystal, a LBO crystal, a KDP crystal.

16. The cryogenic high-pressure ultrafast pump-probe system of claim 15, wherein: The long-focus microscopic objective is selected from one or more of: a 5x long-focus microscopic objective, a 10x long-focus microscopic objective, a 20x long-focus microscopic objective; The camera is a CCD camera and / or a CMOS camera; and / or The crystal is a BBO crystal or a LBO crystal.

17. The cryogenic high-pressure ultrafast pump-probe system of claim 16, wherein: The long-focus microscopic objective is a 10x long-focus microscopic objective; The camera is a CCD camera; and / or The crystal is a BBO crystal.

18. A method for pressure control in-situ online at low temperatures, characterized by, The pressure control method comprises using the in-situ online pressure calibration and imaging system according to any one of claims 1 to 12.

19. The pressure regulating method of claim 18, wherein, The pressure control method comprises the following steps: filling the first pressurized bladder and the second pressurized bladder with inert gas through the gas pressure controller, compressing and stretching the diamond anvil cell in the diamond anvil cell to achieve free increase or decrease of the hydrostatic pressure provided to the sample, and measuring the pressure in the diamond anvil cell in the cryostat through the in-situ online pressure calibration and imaging system to achieve in-situ online pressure control at low temperature.

20. A method of pump-probe spectroscopy at cryogenic high pressure, characterized in that, The pump-probe method comprises using: the in-situ online pressure calibration and imaging system according to any one of claims 1 to 12, or the cryogenic high-pressure ultrafast pump-probe system according to any one of claims 13 to 17.

21. The method of claim 20, wherein, The probe method comprises the following steps: adjusting the optical path so that the pump-probe laser emitted by the femtosecond laser is aligned to enter the long-focus microscopic objective and then enter the optical window of the cold shield in front of the low-temperature double-bladder pressure-regulated high-pressure device to achieve ultrafast pump-probe of the sample at different temperatures and pressures.

22. The method of claim 21, wherein The probe method further comprises the following steps: 1) loading the sample into the high-pressure device and placing it into the optical path; 2) adjusting the temperature and pressure of the sample, and measuring the calibration pressure through the in-situ online pressure calibration and imaging system; and 3) performing pump-probe measurement through the cryogenic high-pressure ultrafast pump-probe system.

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