CN109813654B - Time-resolved measurement device for second harmonic generation of material surface states - Google Patents
Time-resolved measurement device for second harmonic generation of material surface states Download PDFInfo
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Abstract
本发明实施例提供一种材料表面态二次谐波产生的时间分辨测量装置，包括：反射谱系统和计算机；反射谱系统用于从反射光谱中分离获得二次谐波信号以及与探测光同频率的反射信号；计算机用于处理同频率的反射信号以及二次谐波信号，获取具有中心对称晶体结构材料的动力学过程；其中，同频率的反射信号用于反映材料的体态特征，二次谐波信号用于反映材料的表面态特征。本发明实施例通过利用同频率的反射信号反映材料的体态特征，以及利用二次谐波信号反映的材料的表面态特征等原理，从而能够研究或观察具有中心对称晶体结构材料的各种相互作用的动力学过程。
An embodiment of the present invention provides a time-resolved measurement device for generating second harmonics of a surface state of a material, including: a reflection spectrum system and a computer; the reflection spectrum system is used to separate and obtain the second harmonic signal from the reflection spectrum and the same as the detection light. The reflected signal of the same frequency; the computer is used to process the reflected signal of the same frequency and the second harmonic signal, and obtain the dynamic process of the material with the centrosymmetric crystal structure; wherein, the reflected signal of the same frequency is used to reflect the physical characteristics of the material, and the secondary Harmonic signals are used to reflect the surface state characteristics of materials. In the embodiments of the present invention, various interactions of materials with centrosymmetric crystal structures can be studied or observed by using the reflected signals of the same frequency to reflect the body state characteristics of materials, and using the second harmonic signals to reflect the surface state characteristics of materials. dynamic process.
Description
Technical Field
The embodiment of the invention relates to the technical field of ultrafast laser, in particular to a time resolution measuring device for generating material surface state second harmonic.
Background
In order to study the electronic structure, electron-electron and electron-phonon interaction in the material, the prior art generally adopts conventional static means, such as neutron scattering, photoelectron spectroscopy, infrared spectroscopy and raman spectroscopy. Although the above method can effectively detect static electron and phonon structure of material, it is unable to detect and operate electronic structure of transient non-equilibrium state in real time, and unable to observe relaxation process of interaction between electrons and respective degree of freedom in time domain.
Disclosure of Invention
In order to solve the above problems, embodiments of the present invention provide a time-resolved measurement apparatus for material surface state second harmonic generation that overcomes or at least partially solves the above problems.
The embodiment of the invention provides a time resolution measuring device for generating material surface state second harmonic, which comprises: a reflective system and a computer; the reflection spectrum system is used for separating and obtaining a second harmonic signal and a reflection signal with the same frequency as the detection light from the reflection spectrum; wherein, the reflection spectrum is output to the reflection spectrum system after the time-resolved ultrafast pump detection spectrometer irradiates the material with the centrosymmetric crystal structure by the detection light; the computer is used for processing the reflection signal and the second harmonic signal with the same frequency to obtain the dynamic process of the material with the centrosymmetric crystal structure; the reflection signals with the same frequency are used for reflecting the volume state characteristics of the material, and the second harmonic signals are used for reflecting the surface state characteristics of the material.
According to the time-resolved measurement device for generating the material surface state second harmonic, disclosed by the embodiment of the invention, the dynamic processes of various interactions of the material with the centrosymmetric crystal structure can be researched or observed by using the principles of reflecting the material bulk state characteristics by using the reflection signals with the same frequency, reflecting the material surface state characteristics by using the second harmonic signals and the like, and the relaxation processes of the interactions between electrons and the respective degrees of freedom in the time domain are observed.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below. It is obvious that the drawings in the following description are only some embodiments of the invention, and that for a person skilled in the art, other drawings can be derived from these without inventive effort.
Fig. 1 is a schematic structural diagram of a time-resolved measurement apparatus for generating a second harmonic of a material surface state according to an embodiment of the present invention;
FIG. 2 is a schematic structural diagram of a time-resolved measurement apparatus for generating second harmonic in a surface state of a material according to another embodiment of the present invention;
in the figure, 1: a femtosecond laser source; 2: a beam splitter; 3: a delay line; 4: a second reflector; 5: an optical chopper; 6: a first reflector; 7: a second focusing lens; 8: a third focusing lens; 9: a sample; 10: a first focusing lens; 11: a beam splitter prism; 12: a polarizing plate; 13: an infrared detector; 14: a photomultiplier tube; 15: a phase-locked amplifier; 16: a computer; 17: a reflectance spectrum system; 18: a time-resolved ultrafast pump detection spectrometer.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are some embodiments, but not all embodiments, of the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Fig. 1 is a time-resolved measurement apparatus for generating second harmonic of material surface state according to an embodiment of the present invention, referring to fig. 1, the apparatus includes: a reflectance spectrum system 17 and a computer 16;
the reflection spectrum system 17 is used for separating and obtaining a second harmonic signal and a reflection signal with the same frequency as the detection light from the reflection spectrum; wherein, the reflection spectrum is output to the reflection spectrum system 17 after the time-resolved ultrafast pump detection spectrometer 18 irradiates the material with the centrosymmetric crystal structure by the detection light.
Specifically, the time-resolved ultrafast pump detection spectrometer 18 is based on the ultrafast pump-detection time-resolved technique, and outputs the obtained reflectance spectrum to the reflectance spectrum system 17 after irradiating a sample having a centrosymmetric crystal structure material with detection light. Wherein the near infrared detection light in the time-resolved ultrafast pump detection spectrometer 18 interacts with a sample of high-temperature superconducting material with a centrosymmetric crystal structure, and due to the non-centrosymmetry of the surface state structure of the sample, the second-order nonlinear polarizability tensor χ of the surface state(2)Not equal to 0, and second harmonic information is generated. Therefore, the reflection spectrum system 17 can separate and obtain the second harmonic signal and the reflection signal having the same frequency as the detection light from the reflection spectrum. Wherein, there is a center pairA sample of the material with the crystal structure is called as a strongly-associated bulk material with a flat and smooth surface and good reflectivity.
The computer 16 is used for processing the reflection signal and the second harmonic signal with the same frequency to obtain a dynamic process of the material with the centrosymmetric crystal structure; the reflection signals with the same frequency are used for reflecting the volume state characteristics of the material, and the second harmonic signals are used for reflecting the surface state characteristics of the material.
Specifically, the ultrafast laser applied in the time-resolved ultrafast pump detection spectrometer 18 is in a near-infrared band, and the penetration depth in the material is in a micron order; thus, on the one hand, the interaction information carried by the co-frequency reflected light is mainly determined by the bulk structure of the material having a centrosymmetric crystal structure. On the other hand, the interaction information carried by the second harmonic signal is entirely determined by the surface state structure. By combining the two aspects, the body state characteristics can be reflected by utilizing the reflection signals with the same frequency, the surface state characteristics can be reflected by utilizing the second harmonic signals, and the like, so that the dynamic processes of various interactions of the material with the centrosymmetric crystal structure can be researched, the dynamic processes of various coupling actions can be known through ultrafast time-resolved spectral measurement, and the transient properties of the interactions in the surface state and the body state can be distinguished. Therefore, based on the above principle, the computer 16 can process the reflected signal and the second harmonic signal with the same frequency to obtain the dynamic process of the material with the centrosymmetric crystal structure.
According to the time-resolved measurement device for generating the material surface state second harmonic, disclosed by the embodiment of the invention, the dynamic processes of various interactions of the material with the centrosymmetric crystal structure can be researched or observed by using the principles of reflecting the material bulk state characteristics by using the reflection signals with the same frequency, reflecting the material surface state characteristics by using the second harmonic signals and the like, and the relaxation processes of the interactions between electrons and the respective degrees of freedom in the time domain are observed.
Referring to fig. 2, based on the content of the above embodiment, as an alternative embodiment, the reflectance spectrum system 17 includes: a first focusing lens 10, a beam splitter prism 11, a polarizing plate 12, an infrared detector 13 and a photomultiplier tube 14; the first focusing lens 10 is used for focusing the reflection spectrum to the beam splitter prism 11; the beam splitter prism 11 is used for separating the reflected signal with the same frequency and the second harmonic signal in the reflected spectrum; the infrared detector 13 is used for receiving the reflected signals with the same frequency and outputting the reflected signals with the same frequency to the computer 16; the polarizing plate 12 is used for changing the polarization of the second harmonic signal; the photomultiplier 14 is configured to receive the second harmonic signal whose polarization has been changed by the polarizer 12 and output the second harmonic signal to the computer 16.
In particular, the reflectance spectroscopy system 17 is used to separate the second harmonic, detect the second harmonic, and the light of the same frequency. After the beam splitter prism 11 separates and obtains the reflection signal and the second harmonic signal with the same frequency, the reflection signal with the same frequency is input to the infrared detector 13 (that is, the infrared detector 13 receives the transient reflectivity signal of the near infrared on the surface of the sample 9), and the infrared detector 13 further outputs the reflection signal with the same frequency to the computer 16. The second harmonic signal passes through the polarizer 12 and the photomultiplier 14 in sequence, and the photomultiplier 14 collects and detects the second harmonic signal and further outputs the second harmonic signal to the computer 16. The computer 16 processes the near infrared reflected signals and the second harmonic signals in the reflected spectrum.
Based on the above description of the embodiments, as an alternative embodiment, the time-resolved ultrafast pumping detection spectrometer 18 includes: the device comprises a femtosecond laser light source 1, a beam splitter 2, a pump light system and a detection light system; the femtosecond laser light source 1 is used for generating femtosecond pulse laser and sending the femtosecond pulse laser to the beam splitter 2; the beam splitter 2 is used for splitting the femtosecond pulse laser into pump light and probe light, sending the pump light to the pump light system, and sending the probe light to the probe light system; the pump light system is used for optically modulating the pump light and focusing the modulated pump light to the surface of the material with the centrosymmetric crystal structure; the detection optical system is used for delaying the detection light and focusing the processed detection light on the surface of the material with the centrosymmetric crystal structure.
The femtosecond laser source 1 can be a titanium-sapphire femtosecond laser, and the light source can provide femtosecond pulse laser with the wavelength of 800nm and the repetition frequency of 1KHz and transmit the femtosecond pulse laser to the beam splitter 2. The beam splitter 2 can split the femtosecond pulse laser into two beams of light, which are the pump light and the probe light, respectively.
Based on the content of the foregoing embodiments, as an alternative embodiment, the pumping light system includes: an optical chopper 5, a first reflecting mirror 6, and a second focusing lens 7; the optical chopper 5 is used for optically modulating the pump light and sending the modulated pump light to the first reflector 6; the first reflector 6 is used for reflecting the pump light to the second focusing lens 7; the second focusing lens 7 is used to focus the pump light onto the surface of the material with a centrosymmetric crystal structure.
Specifically, in the pump light system, the pump light is focused on the surface of the sample 9 after passing through the optical chopper 5, the first reflecting mirror 6, and the second focusing lens 7. The pump light can excite sample 9, causing the properties of sample 9 to change, and observing the kinetics of the sample. Wherein, the spot diameter of the pump light is 0.3-0.6 mm, and can be preferably 0.4 mm.
Based on the content of the above embodiments, as an alternative embodiment, the probe light system includes: a delay line 3, a second mirror 4, and a third focusing lens 8; the delay line 3 is used for performing time delay processing on the detection light and sending the detection light after the time delay processing to the second reflecting mirror 4; the second reflecting mirror 4 is used for reflecting the detection light to the third focusing lens 8; the third focusing lens 8 is used to focus the probe light onto the surface of the material having a centrosymmetric crystal structure.
The delay line 3 can be arranged on the optical path of the detection light, and the optical path difference between the pump light and the detection light on the delay line 3 is controlled by using the electric displacement table, so that the time delay between the two beams of light is realized. The delay line 3 can include two-sided high-reflection mirrors, the two-sided high-reflection mirrors are arranged at 90 degrees, the detection light and the two-sided high-reflection mirrors form an angle of 45 degrees, and therefore when the electric displacement table moves, the incident light is always parallel to the reflected light. The delayed probe light is focused on the sample 9 via the second reflecting mirror 4 and the third focusing lens 8.
Based on the content of the above embodiment, as an alternative embodiment, the light spot of the pumping light irradiated to the surface of the material with the centrosymmetric crystal structure is completely overlapped with the light spot of the probe light irradiated to the surface of the material with the centrosymmetric crystal structure.
Based on the above disclosure of the embodiments, as an alternative embodiment, the time-resolved measurement apparatus for material surface state second harmonic generation further includes: a lock-in amplifier 15; the optical chopper 5 is used for transmitting the modulated pump light to the lock-in amplifier 15; the infrared detector 13 is used for sending the reflected signal with the same frequency to the phase-locked amplifier 15; the lock-in amplifier 15 is configured to identify the reflection signal with the same frequency by using the pump light as a reference signal, and amplify and output the identified reflection signal with the same frequency to the computer 16.
Specifically, the optical chopper 5 can modulate a pump light of 1KHz at a frequency of 420Hz, and the modulated electric signal is input to the lock-in amplifier 15 as a reference signal. The lock-in amplifier 15 also receives the near-infrared transient reflectivity signal (i.e. the same-frequency reflection signal) of the surface of the sample 9 input by the infrared detector 13, and identifies and amplifies the same-frequency reflection signal and outputs the same to the computer 16.
In summary, the time-resolved measurement apparatus for generating the material surface state second harmonic according to the embodiment of the present invention selects near/mid infrared light as a pump and near infrared light as a probe based on the ultrafast time-resolved pump-probe principle. Firstly, pumping light excites an electronic system to be in a non-equilibrium transient state; then the detection light and the material have a centrosymmetric body structure and a non-centrosymmetric surface structure, and generate linear and nonlinear interaction to generate light with the same frequency (with body state information) and second harmonic (with surface state information); then, separating out the light with the same frequency and the second harmonic from the reflected spectrum by using a beam splitter prism; and finally, detecting the light with the same frequency by using an infrared detector and a phase-locked amplifier, and detecting the second harmonic by using a photomultiplier, thereby realizing the research on the centrosymmetric body state and the non-centrosymmetric surface state of the material.
Finally, it should be noted that: the above examples are only intended to illustrate the technical solution of the present invention, but not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some technical features may be equivalently replaced; and such modifications or substitutions do not depart from the spirit and scope of the corresponding technical solutions of the embodiments of the present invention.
Claims (6)
1. A time-resolved measurement device for the generation of second harmonics of a material surface state, comprising: a reflective system and a computer;
the reflection spectrum system is used for separating and obtaining a second harmonic signal and a reflection signal with the same frequency as the detection light from the reflection spectrum; the reflection spectrum is output to the reflection spectrum system after the time-resolved ultrafast pump detection spectrometer irradiates a material with a centrosymmetric crystal structure through the detection light;
the computer is used for processing the reflection signal with the same frequency and the second harmonic signal to obtain a dynamic process of the material with the centrosymmetric crystal structure; wherein the reflection signal with the same frequency is used for reflecting the posture characteristic of the material, and the second harmonic signal is used for reflecting the surface posture characteristic of the material;
the reflectance spectrum system comprises: the device comprises a first focusing lens, a beam splitter prism, a polaroid, an infrared detector and a photomultiplier;
the first focusing lens is used for focusing the reflection spectrum to the beam splitter prism;
the beam splitting prism is used for separating the reflection signal with the same frequency in the reflection spectrum and the second harmonic signal;
the infrared detector is used for receiving the reflection signals with the same frequency and outputting the reflection signals with the same frequency to the computer;
the polaroid is used for changing the polarization of the second harmonic signal;
the photomultiplier is used for receiving the second harmonic signal after polarization is changed by the polaroid and outputting the second harmonic signal to the computer.
2. The apparatus of claim 1, wherein the time-resolved ultrafast pumped probe spectrometer comprises: the device comprises a femtosecond laser light source, a beam splitter, a pump light system and a detection light system;
the femtosecond laser light source is used for generating femtosecond pulse laser and sending the femtosecond pulse laser to the beam splitter;
the beam splitter is used for splitting the femtosecond pulse laser into pumping light and detection light, sending the pumping light to the pumping light system and sending the detection light to the detection light system;
the pump light system is used for optically modulating the pump light and focusing the modulated pump light to the surface of the material with the centrosymmetric crystal structure;
the detection light system is used for delaying the detection light and focusing the processed detection light to the surface of the material with the centrosymmetric crystal structure.
3. The apparatus of claim 2, wherein the pump light system comprises: an optical chopper, a first reflector and a second focusing lens;
the optical chopper is used for optically modulating the pump light and sending the modulated pump light to the first reflecting mirror;
the first reflector is used for reflecting the pump light to the second focusing lens;
the second focusing lens is used for focusing the pump light to the surface of the material with the centrosymmetric crystal structure.
4. The apparatus of claim 2, wherein the probe light system comprises: a delay line, a second reflecting mirror and a third focusing lens;
the delay line is used for carrying out time delay processing on the detection light and sending the detection light after the time delay processing to the second reflecting mirror;
the second reflecting mirror is used for reflecting the detection light to the third focusing lens;
the third focusing lens is used for focusing the detection light to the surface of the material with the central symmetry crystal structure.
5. The apparatus of claim 2, wherein the spot of the pump light impinging on the surface of the material having a centrosymmetric crystal structure is completely coincident with the spot of the probe light impinging on the surface of the material having a centrosymmetric crystal structure.
6. The apparatus of claim 3, further comprising: a phase-locked amplifier;
the optical chopper is used for transmitting the modulated pump light to the lock-in amplifier;
the infrared detector is used for sending the reflection signal with the same frequency to the phase-locked amplifier;
the phase-locked amplifier is used for identifying the reflection signal with the same frequency by taking the pump light as a reference signal and amplifying and outputting the identified reflection signal with the same frequency to the computer.
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