CN111307756A - Frequency-adjustable ultrafast time resolution transient reflection spectrometer - Google Patents

Frequency-adjustable ultrafast time resolution transient reflection spectrometer Download PDF

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CN111307756A
CN111307756A CN201911138096.7A CN201911138096A CN111307756A CN 111307756 A CN111307756 A CN 111307756A CN 201911138096 A CN201911138096 A CN 201911138096A CN 111307756 A CN111307756 A CN 111307756A
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聂需辰
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Nanjing University of Aeronautics and Astronautics
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    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/17Systems in which incident light is modified in accordance with the properties of the material investigated
    • G01N21/25Colour; Spectral properties, i.e. comparison of effect of material on the light at two or more different wavelengths or wavelength bands
    • G01N21/31Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry
    • G01N21/39Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry using tunable lasers
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/17Systems in which incident light is modified in accordance with the properties of the material investigated
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/17Systems in which incident light is modified in accordance with the properties of the material investigated
    • G01N21/1717Systems in which incident light is modified in accordance with the properties of the material investigated with a modulation of one or more physical properties of the sample during the optical investigation, e.g. electro-reflectance
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/17Systems in which incident light is modified in accordance with the properties of the material investigated
    • G01N21/55Specular reflectivity
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    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/17Systems in which incident light is modified in accordance with the properties of the material investigated
    • G01N21/1717Systems in which incident light is modified in accordance with the properties of the material investigated with a modulation of one or more physical properties of the sample during the optical investigation, e.g. electro-reflectance
    • G01N2021/1725Modulation of properties by light, e.g. photoreflectance
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/17Systems in which incident light is modified in accordance with the properties of the material investigated
    • G01N2021/1789Time resolved

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Abstract

The invention discloses a variable-frequency ultrafast time resolution transient reflection spectrometer, which comprises: the device comprises a titanium gem femtosecond laser device, a beam splitting unit, a pumping light path, a detection light path, a light spot monitoring unit and a signal detection processing unit. The beam splitting unit divides a laser beam output by the titanium-sapphire femtosecond laser device into a pumping light part and a detection light part, the pumping light path performs frequency modulation processing on a first beam of pulse laser to obtain the pumping light with a preset wavelength, and the detection light path performs delay processing on a second beam of pulse laser to obtain the detection light; after the pump light and the detection light are irradiated on the same position of the sample to be detected in sequence, the reflected light signal generated by the detection light is received and processed by the signal detection and processing unit, and the transient reflectivity change condition of the sample to be detected can be determined. The invention can realize multi-wavelength excitation, provides great help for understanding the transient reflectivity change condition of the sample to be detected under the excitation of different frequencies of light, and further can research the ultrafast dynamic process in the sample to be detected under the excitation of different frequencies of light.

Description

Frequency-adjustable ultrafast time resolution transient reflection spectrometer
Technical Field
The invention belongs to the technical field of ultrafast lasers, and particularly relates to a frequency-adjustable ultrafast time-resolved transient reflection spectrometer.
Background
In recent decades, with the rapid development of ultrashort pulse laser technology, ultrafast spectroscopy technology has been widely applied to various fields of condensed state physics, such as traditional physical systems of metals and semiconductors, and strongly associated electronic systems of iron-based high temperature superconductors, Mott insulators, copper oxide high temperature superconductors, and the like, and has become an important experimental means for studying the ultrafast dynamic process of quasi-particles in non-equilibrium state.
Traditional experimental means, usually using external electric field to drive the movement of conductive electrons to measure transport or tunneling properties, such as scanning tunneling microscope, or using external electromagnetic field, pressure or temperature variation to induce electrons to transit between different energy levels and then observe their light absorption/emission spectra and photoelectron spectra, such as resonance inelastic X-ray scattering, resonance soft X-ray scattering and angle-resolved photoelectron spectra, however, these external excitations are either extremely weak or applied for a time much longer than the characteristic time of interaction between the degrees of freedom inside the system, so that the substance is in quasi-equilibrium state, where the interactions between the degrees of freedom such as charge, orbit, lattice and spin are entangled with each other in the frequency domain, and the kinetic processes such as generation, migration and recombination of photo-excited carriers are often in picosecond order, the traditional static observation means can not capture the inherent ultra-fast kinetic process at all, and is difficult to independently research.
Because electrons, crystal lattices, spin dynamics and the like have different characteristic action time, a substance can be excited by femtosecond strong laser pulses to generate an ultrafast nonequilibrium state, and then ultrafast dynamic processes of respective degrees of freedom are researched in a time domain by using a transient reflection spectrometer.
However, different ultrafast kinetic processes of different materials, such as high temperature superconductivity, charge density waves, metal-insulator transition, etc., correspond to different characteristic energy scales, and thus excitation with excitation light of different energies is required. However, at present, there is no ultrafast time-resolved transient reflection spectrometer with adjustable frequency, which is used to perform deep research on different physical properties of different materials, such as ferromagnetism, superconductivity, electron-phonon coupling and other charge/spin order equalities, and therefore, it is urgently needed to provide an ultrafast time-resolved transient reflection spectrometer with adjustable frequency, which is used to perform research on different physical processes.
Disclosure of Invention
The invention provides a frequency-adjustable ultrafast time resolution transient reflection spectrometer, which aims to solve the problems in the prior art.
In order to achieve the purpose, the invention adopts the technical scheme that:
a frequency-adjustable ultrafast time-resolved transient reflection spectrometer comprises a titanium gem femtosecond laser device, a beam splitting unit, a pumping light path, a detection light path, a light spot monitoring unit and a signal detection processing unit;
the titanium gem femtosecond laser device is used for generating femtosecond pulse laser;
the beam splitting unit is used for splitting the femtosecond pulse laser into a first pulse laser and a second pulse laser;
the pumping light path is used for carrying out frequency modulation processing on the first pulse laser to obtain pumping light with a preset wavelength and adjusting the polarization direction of the first pulse laser;
the detection light path is used for delaying the second pulse laser and then using the second pulse laser as detection light;
after the pumping light vertically irradiates the sample to be detected, the probe light irradiates the same position of the sample to be detected at a preset angle,
the light spot monitoring unit is used for monitoring the accurate positions and the contact ratio of the pumping light spots and the detection light spots on the sample to be detected in real time;
the signal detection processing unit is used for receiving and processing a reflected light signal obtained after the detection light irradiates the sample to be detected, and determining and recording the transient reflectivity change of the sample to be detected.
Further, the beam splitting unit divides the femtosecond pulse laser into a first pulse laser and a second pulse laser at a splitting ratio of 8: 2.
Further, the pumping light path comprises a frequency modulation unit, an optical chopper, a first reflector, a first lambda/2 wave plate and a first focusing lens;
the frequency modulation unit is used for adjusting the frequency of the first pulse laser based on an Optical Parametric Oscillation (OPO) technology and transmitting the frequency-modulated first pulse laser to an optical chopper;
the optical chopper is used for optically modulating the first pulse laser, transmitting the modulated first pulse laser to the first reflector and outputting a modulated electric signal serving as a reference signal to a computer;
the first reflector reflects the first pulse laser passing through the optical chopper to the first lambda/2 wave plate;
the first lambda/2 wave plate is used for adjusting the polarization direction of the first pulse laser;
the first focusing lens is used for vertically focusing the pump light after frequency modulation processing to the surface of the sample.
Further, the detection light path comprises an electric displacement table, a second reflecting mirror and a second focusing lens;
the electric displacement table is used for accurately changing the optical path of the second pulse laser so as to realize time delay relative to the first pulse laser;
the second reflector reflects the delayed second pulse laser to a second focusing mirror;
the second focusing lens is used for focusing the detection light after the delay processing to the surface of the sample to be detected at a preset angle.
The signal detection processing unit comprises a second lambda/2 wave plate, a photoelectric detector and a signal processing unit;
the second lambda/2 wave plate is used for adjusting the polarization direction of the reflected light to be vertical to the polarization direction of the pump light;
and the photoelectric detector is used for receiving the reflected light signal and transmitting the reflected light signal to the signal processing unit, and determining the transient reflectivity change of the sample to be detected.
Furthermore, the sample to be detected is suitable for two-dimensional or bulk materials with smooth surfaces and good reflection performance, such as semiconductors, superconductors, topological insulators and the like.
Preferably, the titanium gemstone femtosecond laser device generates femtosecond pulse laser with the frequency of 1kHz, the pulse width of 35 fs and the wavelength of 800 nm.
Preferably, the pumping optical path performs frequency modulation processing on the first pulse laser to obtain pumping light with a preset wavelength of 400 nm.
Preferably, the optical chopper optically modulates the first pulse laser with a frequency of 450Hz to a frequency of 1kHz, the frequency of the modulated first pulse laser is changed to 450Hz, and the modulated electric signal is used as a reference signal
Preferably, the step precision of the motorized displacement stage is 1 μm, corresponding to a time resolution of 6.67 fs.
Compared with the prior art, the invention has the following beneficial effects:
the laser comprises a titanium gem femtosecond laser device, a beam splitting unit, a pumping light path, a detection light path, a light spot monitoring unit and a signal detection processing unit. Performing frequency modulation processing on the first pulse laser through a pumping light path to obtain pumping light with a preset wavelength, and performing delay processing on the second pulse laser through a detection light path to obtain detection light; after the pump light and the detection light irradiate the sample to be detected in sequence, the reflected light signal generated by the detection light is received by the signal detection processing unit, and the transient reflectivity change of the sample to be detected can be determined. The ultrafast time-resolved reflection spectrometer provided by the embodiment of the invention can realize multi-wavelength detection, provides very beneficial help for understanding the transient reflectivity change condition of the sample to be detected under the irradiation of pump light with different frequencies, and further can research the ultrafast dynamic process in the sample to be detected under the excitation of light with different frequencies.
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FIG. 1 is a schematic block diagram of the present invention;
fig. 2 is a schematic diagram of the complete structure of the present invention.
Detailed Description
The present invention will be further described with reference to the following examples.
As shown in fig. 1, an ultrafast time-resolved transient reflection spectrometer with frequency modulation provided by an embodiment of the present invention includes: the device comprises a titanium gem femtosecond laser device 1, a beam splitting unit 2, a pumping light path 3, a detection light path 4, a light spot monitoring unit 5 and a signal detection processing unit 6. Wherein, the titanium gem femtosecond laser device 1 is used for generating femtosecond pulse laser; the beam splitting unit 2 is used for splitting the femtosecond pulse laser into a first pulse laser and a second pulse laser; the pumping light path 3 is used for performing frequency modulation processing on the first pulse laser to obtain pumping light with a preset wavelength and adjusting the polarization direction of the first pulse laser; the detection light path 4 is used for delaying the second pulse laser and then taking the second pulse laser as detection light; after the pumping light vertically irradiates a sample to be detected, the detection light irradiates the same position of the sample to be detected at a preset angle, and the light spot monitoring unit 6 is used for monitoring the accurate position and the contact ratio of the pumping light spot and the detection light spot on the sample in real time; the signal detection processing unit 7 is used for receiving and processing a reflected light signal obtained after the detection light irradiates the sample to be detected, and determining the transient reflectivity change of the sample to be detected.
Specifically, in the embodiment of the present invention, the titanium sapphire femtosecond laser device 1 is adopted to generate femtosecond pulse laser, the frequency of which can be 1kHz, the pulse width of which can be 35 fs, and the wavelength of which can be 800 nm.
The femtosecond pulse laser generated by the titanium gem femtosecond laser device 1 generates a first pulse laser and a second pulse laser through the beam splitting unit 2, wherein the first pulse laser is used for generating pump light with preset wavelength, and the second pulse laser is used as detection light. The method for generating the pump light with the preset wavelength may be as follows: the first pulse laser passes through the pumping light path 3, and the first pulse laser is subjected to frequency doubling, difference frequency or sum frequency treatment and the like through the pumping light path 3, so that pumping light with a preset wavelength can be obtained. For example, a titanium-sapphire femtosecond laser device 1 is used to generate femtosecond pulse laser with a wavelength of 800 nm, the wavelengths of the first pulse laser and the second pulse laser obtained by the beam splitting unit 2 are both 800 nm, and the pump light with a preset wavelength of 400nm can be obtained after the first pulse laser is frequency-doubled by a pump light path 3.
The sample to be detected adopted in the embodiment of the invention is a body or a two-dimensional material with smooth surface and good reflectivity, and can be a semiconductor, a metal, a high-temperature superconductor, a topological insulator and the like.
The pumping light path 3 is used for performing frequency modulation processing on the first pulse laser to obtain pumping light with a preset wavelength and adjusting the polarization direction of the first pulse laser; the detection light path 4 is used for delaying the second pulse laser and then taking the second pulse laser as detection light; after the pumping light vertically irradiates a sample to be detected, the detection light irradiates the same position of the sample to be detected at a preset angle, and the light spot monitoring unit 6 is used for monitoring the accurate position and the contact ratio of the pumping light spot and the detection light spot on the sample in real time; the signal detection processing unit 7 is used for receiving and processing a reflected light signal obtained after the detection light irradiates the sample to be detected, and determining the transient reflectivity change of the sample to be detected.
After the pump light and the probe light are irradiated on the same position of the sample to be detected in sequence, the signal detection processing unit 7 receives and processes a reflected light signal obtained after the probe light irradiates the sample to be detected, so that the transient reflectivity change of the sample to be detected is determined. In the embodiment of the present invention, only the signal detection processing unit 7 is required to receive the reflected light signal of the detection light, so that the reflected light signal of the pump light is successfully separated from the reflected light signal of the detection light, the pump light is vertically irradiated on the sample to be detected, and the detection light is irradiated on the sample to be detected at the preset angle. Because the two angles irradiated on the sample to be detected are different, the corresponding angles of the reflected light signals are also different, and the separation can be successfully realized.
In the embodiment of the invention, the diameter of the spot focused by the pump light on the sample to be detected is generally twice that of the spot focused by the detection light on the sample to be detected, the area is quadruple, and the signal change caused by the excitation of the pump light on the sample to be detected can be completely detected by the detection light by setting the centers of the spot of the detection light and the spot of the pump light to be completely coincident. In this embodiment, in practical implementation, even if the two concentric light spots do not completely coincide with each other, the detection signal is not lost as long as the pumping light spot covers the detection light spot by the light spot monitoring unit 6.
In the embodiment of the present invention, the signal detection processing unit 7 is configured to receive and process a reflected light signal obtained after the detection light irradiates the sample to be detected, so as to determine a transient reflectivity change of the sample to be detected.
As shown in fig. 2, based on the above embodiments, in the ultrafast time-resolved transient reflection spectrometer with adjustable frequency provided in an embodiment of the present invention, the pump optical path 3 specifically includes: a frequency modulation unit 31, an optical chopper 32, a first mirror 33, a first lambda/2 wave plate 34, a first focusing lens 35. Wherein the first pulse laser passes through the frequency modulation unit 31, the optical chopper 32, the first reflecting mirror 33 and the first lambda/2 wave plate 34 to obtain the pump light. The first focusing lens 35 is used for converging the pump light and enabling the converged pump light to vertically irradiate the sample to be detected.
Specifically, in the embodiment of the present invention, the frequency modulation unit 31 performs frequency modulation on the first pulse laser by using an OPO technique to obtain the pump light with the preset wavelength. The optical chopper 32 is used to optically modulate the first pulse laser light to change the frequency of the first pulse laser light, thereby functioning as a pulse switch. For example, the optical chopper 32 in the embodiment of the present invention optically modulates the first pulse laser light having a frequency of 1kHz at a frequency of 450Hz, the frequency of the modulated first pulse laser light becomes 450Hz, and the modulated electric signal serves as a reference signal. The first pulsed laser light is reflected to the first λ/2 plate 34 via the first mirror 33. The first λ/2 wave plate 34 is used to adjust the polarization direction of the modulated first pulse laser light to be perpendicular to the polarization direction of the probe light. The first mirror 33 is a high-reflection mirror. The focusing lens 35 is used for converging the pump light and enabling the converged pump light to vertically irradiate the sample to be detected.
As shown in fig. 2, on the basis of the foregoing embodiment, the ultrafast time-resolved transient reflection spectrometer with frequency modulation provided in the embodiment of the present invention includes: an electric displacement table 41, a second mirror 42, and a second focusing lens 43. The electric displacement table 41 is used for accurately changing the optical path of the second pulse laser, so as to realize the time delay relative to the first pulse laser, and in the embodiment of the invention, the stepping precision of the electric displacement table is 1 μm, and the corresponding time resolution is 6.67 fs. The second reflecting mirror 42 reflects the second pulse laser light after the time delay to the second focusing mirror 43, and the second focusing lens 43 is used for focusing the detection light after the delay processing to the surface of the sample at a preset angle. Specifically, the probe light is at an angle with respect to the pump light, as long as the reflected signals of the probe light and the pump light can be separated.
As shown in fig. 2, based on the above embodiment, in the ultrafast time-resolved transient reflection spectrometer with adjustable frequency provided in the embodiment of the present invention, after the pump light vertically irradiates the sample 5 to be detected, the probe light irradiates the same position of the sample 5 to be detected at a preset angle, and the light spot monitoring unit 6 is configured to monitor the accurate positions and the coincidence ratio of the pump light spot and the probe light spot on the sample in real time.
As shown in fig. 2, based on the above embodiment, the signal detection processing unit 7 of the ultrafast time-resolved transient reflection spectrometer with adjustable frequency provided in the embodiment of the present invention specifically includes: a second lambda/2 wave plate 71, a photodetector 72, a signal processing unit 73. Wherein the second λ/2 plate 71 is used to adjust the polarization direction of the reflected light to be perpendicular to the polarization direction of the pump light; the photodetector 72 is configured to receive a reflected light signal obtained after the detection light irradiates the sample 5 to be detected and transmit the reflected light signal to the signal processing unit 73, and the signal processing unit 73 is configured to determine and record a transient reflectivity change of the sample to be detected.
The above description is only of the preferred embodiments of the present invention, and it should be noted that: it will be apparent to those skilled in the art that various modifications and adaptations can be made without departing from the principles of the invention and these are intended to be within the scope of the invention.

Claims (5)

1. A frequency-adjustable ultrafast time-resolved transient reflection spectrometer is characterized by comprising a titanium gem femtosecond laser device, a beam splitting unit, a pumping light path, a detection light path, a light spot monitoring unit and a signal detection processing unit;
the titanium gem femtosecond laser device is used for generating femtosecond pulse laser;
the beam splitting unit is used for splitting the femtosecond pulse laser into a first pulse laser and a second pulse laser;
the pumping light path is used for carrying out frequency modulation processing on the first pulse laser to obtain pumping light with a preset wavelength and adjusting the polarization direction of the first pulse laser;
the detection light path is used for delaying the second pulse laser and then using the second pulse laser as detection light;
after the pumping light vertically irradiates the sample to be detected, the probe light irradiates the same position of the sample to be detected at a preset angle,
the light spot monitoring unit is used for monitoring the accurate positions and the contact ratio of the pumping light spots and the detection light spots on the sample to be detected in real time;
the signal detection processing unit is used for receiving and processing a reflected light signal obtained after the detection light irradiates the sample to be detected, and determining and recording the transient reflectivity change of the sample to be detected.
2. The tunable ultrafast time resolved transient reflection spectrometer of claim 1, wherein: the beam splitting unit divides the femtosecond pulse laser into a first pulse laser and a second pulse laser according to a splitting ratio of 8: 2.
3. The tunable ultrafast time resolved transient reflection spectrometer of claim 1, wherein: the pumping light path comprises a frequency modulation unit, an optical chopper, a first reflector, a first lambda/2 wave plate and a first focusing lens;
the frequency modulation unit is used for adjusting the frequency of the first pulse laser based on an Optical Parametric Oscillation (OPO) technology and transmitting the frequency-modulated first pulse laser to an optical chopper;
the optical chopper is used for optically modulating the first pulse laser, transmitting the modulated first pulse laser to the first reflector and outputting a modulated electric signal serving as a reference signal to a computer;
the first reflector reflects the first pulse laser passing through the optical chopper to the first lambda/2 wave plate;
the first lambda/2 wave plate is used for adjusting the polarization direction of the first pulse laser;
the first focusing lens is used for vertically focusing the pump light after frequency modulation processing to the surface of the sample.
4. The tunable ultrafast time resolved transient reflection spectrometer of claim 1, wherein: the detection light path comprises an electric displacement table, a second reflector and a second focusing lens;
the electric displacement table is used for accurately changing the optical path of the second pulse laser so as to realize time delay relative to the first pulse laser;
the second reflector reflects the delayed second pulse laser to a second focusing mirror;
the second focusing lens is used for focusing the detection light after the delay processing to the surface of the sample to be detected at a preset angle.
5. The tunable ultrafast time resolved transient reflection spectrometer of claim 1, wherein: the signal detection processing unit comprises a second lambda/2 wave plate, a photoelectric detector and a signal processing unit;
the second lambda/2 wave plate is used for adjusting the polarization direction of the reflected light to be vertical to the polarization direction of the pump light;
and the photoelectric detector is used for receiving the reflected light signal and transmitting the reflected light signal to the signal processing unit, and determining the transient reflectivity change of the sample to be detected.
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Application publication date: 20200619