CN109060767A - A kind of double frequency comb spectrum focusing coherent antistockes Raman spectroscopy detection systems - Google Patents
A kind of double frequency comb spectrum focusing coherent antistockes Raman spectroscopy detection systems Download PDFInfo
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
- G01N21/62—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
- G01N21/63—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light optically excited
- G01N21/65—Raman scattering
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
- G01N21/01—Arrangements or apparatus for facilitating the optical investigation
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
- G01N21/62—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
- G01N21/63—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light optically excited
- G01N21/65—Raman scattering
- G01N2021/653—Coherent methods [CARS]
Abstract
A kind of double frequency comb spectrum focusing coherent antistockes Raman spectroscopy detection systems, including double light comb light source modules, stokes light generation module, micro- focusing and Sample Scan module, sampling trigger module coherent signal detection, acquisition and analysis and processing module etc..Wherein: double light comb light source modules, which contain, to be used as pump light and detects the light source of frequency comb all the way of light and the another way light comb light source as Stokes photogenerated, and there are a small repetition is poor for two-way frequency comb light source；Stokes light generation module realizes that optical frequency deviates using fiber nonlinear effect, obtains stokes light；It samples trigger module and obtains two light comb pulse matching positions using second harmonic generation technique, realize pulse orientation triggering spectra collection.The present invention realizes non-scan rapid wideband and is concerned with anti-stoke Raman spectroscopic detection, has been obviously improved the ability that broadband coherent anti-stokes Raman spectroscopy technology is applied in high dynamic, multicomponent detection analysis.
Description
Technical field
The invention belongs to coherent antistockes Raman spectroscopy detection technology fields, especially a kind of to pass through double frequency comb optics
The mutually spectrum focusing coherent antistockes Raman spectroscopy detection system of scanning, pulse chirp regulation.
Background technique
Coherent antistockes Raman spectroscopy (CARS:Coherent Anti-Stokes Raman Scattering) is visited
Survey technology utilizes Third-order nonlinearity, is able to achieve detectivity more higher than traditional spontaneous Raman process；Meanwhile CARS skill
Art obtains the intrinsic corresponding spectral signal of vibrational-rotational level of measurand molecule, and height can be realized specifically without introducing marking signal
Property detection.The features described above of CARS provides completely new hand for the unmarked imaging exploration in the fields such as physical chemistry, life science
Section.As modern life science on a molecular scale develops the detection of complication system, enough spectral widths are not only needed
To provide sufficient molecular chemistry information, it is also necessary to have sufficiently fast speed of detection to support to the real-time of biochemical kinetics process
Analysis.Narrowband CARS can satisfy requirement on image taking speed, but spectral information is deficient, be simply possible to use in single component analysis；
And the more acquisition speed in the every pixel of several milliseconds of broad band CARS technology.Therefore, the imaging speed of broad band CARS how is improved
Degree realizes that real-time spectrum picture acquisition is one of the main problem of coherent Raman micro-imaging field face.
In existing broad band CARS realization technology, for the resolution capability of spectral preservation itself, whether Fourier becomes
It changes the relevant control CARS technology of CARS technology, pulse, wavelength tuning CARS technology or spectrum and focuses CARS technology, be required to
Impulse phase or frequency modulation(PFM) are realized using external mechanical displacement.Intrinsically, several to the dependence of Mechanical Moving
It is the bottleneck problem place that entire broad band CARS technology realizes high speed micro-imaging at present, greatly limits entire coherent Raman
The micro-imaging technique detection to complex biological system and its dynamic process on a molecular scale.
Particularly, spectrum focuses CARS technology by impulse phase regulation, so that different frequency ingredient exists in femtosecond pulse
Linear array on time, when realizing two pulses with certain time delayed coincidence, only a molecular vibration energy level is excited, i.e. phase
When there is very good energy utilization efficiency, be advantageously implemented height in the excitation that all energy are all used to single level
Sensitive detection.But existing spectrum focuses in CARS technology, and the relative time delay scanning between pulse (is equivalent to the spy of different Raman peaks
Survey) scanning of mechanical displacement platform is still relied on, speed of detection is slow, cannot effectively play spectrum focusing-detection potentiality.
Summary of the invention
In order to overcome the disadvantages of the above prior art, the purpose of the present invention is to provide a kind of double frequency comb spectrum to focus phase
Dry anti stokes raman spectrum detection system is mutually scanned based on double frequency comb optics, without mechanical scanning, detects light
Spectrum width, speed of detection are high.
To achieve the goals above, the technical solution adopted by the present invention is that:
A kind of double frequency comb spectrum focusing coherent antistockes Raman spectroscopy detection systems characterized by comprising
Double light comb light source modules 1 have the first frequency comb light source 1-1 and the second optical frequency of fine difference including repetition rate difference
Comb light source 1-2, pump light and detection light of the output light of the first frequency comb light source 1-1 as detection process；
Stokes light generation module 5, it is non-thread using optical fiber using the output light of the second frequency comb light source 1-2 as input light
Property effect realize optical frequency offset, obtain stokes light；
Micro- focusing and Sample Scan module 9, receive the focusing for closing the pump light and stokes light of beam and anti-stoke
The collection of this light, sample 3-D scanning, obtain coherent antistockes Raman spectroscopy signal；
Coherent signal detection module 11 detects the coherent antistockes Raman spectroscopy signal；
Trigger module 12 is sampled, for positioning pump light in stokes light overlapping region, realizes pulse orientation triggering light
Spectrum acquisition；
Acquisition module 13, acquisition obtain the original spectral data of coherent antistockes Raman spectroscopy signal；
Analysis and processing module 14 carries out spectrum recovering to original spectral data processing.
The central wavelength of double light comb light source modules 1 is in near-infrared, the first frequency comb light source 1-1 and the second optical frequency
Comb the repetition rate f of light source 1-2rWith fine difference, i.e. fr1=fr2+δfr, wherein fr1For the frequency of the first frequency comb light source 1-1
Rate, fr2For the frequency of the second frequency comb light source 1-2, δ frIndicate that the repetition rate of two light sources is poor, value is much smaller than repetition rate
fr。
The output light of the first frequency comb light source 1-1 is successively through the first half-wave plate 2-1 and the first polarization splitting prism 3-
1, transmissive portion, that is, P polarisation introduces linear chrip and the frequency needed for the first optical filter 6-1 leaching through the first dispersion adjustment element 4-1
The chirped pulse of rate range, the output light of the stokes light generation module 5 is through reflecting mirror 7-1 reflection and the second dispersion adjustment
Element 4-2 introduces linear chrip, and the light pulse that two-way introduces linear chrip closes beam by dichroic mirror 8, is then coupled into micro- focusing
With Sample Scan mould 9；
The output light of the second frequency comb light source 1-2 is successively through the second half-wave plate 2-2 and the second polarization splitting prism 3-
2, transmissive portion, that is, P polarisation is input to the first coupling mirror 5-1 after third half-wave plate 2-3；Pass through the second half-wave plate 2-2, second
Polarization splitting prism 3-2, third half-wave plate 2-3 and third optical filter 5-4 adjust the output work of stokes light generation module 5
Rate and output wave-number range.
The sampling trigger module 12 includes the first lens 12-1, nonlinear crystal 12-2, the second lens set gradually
12-3, the 4th optical filter 12-4 and photodetector 12-5 are touched using the second harmonic generation method of two type-Ⅱphase matchings
Send out pulse, process are as follows: part, that is, S that the output light of the first frequency comb light source 1-1 is reflected by the first polarization splitting prism 3-1 is inclined
Light enters the first lens 12-1；The output light of second frequency comb light source 1-2 is by the part reflected the second polarization splitting prism 3-2
S polarisation is adjusted to P polarisation through the 4th half-wave plate 2-4, then is transmitted into the first lens 12-1 through the first polarization splitting prism 3-1,
Nonlinear crystal 12-2 is incident on through the first lens 12-1 convergence and forms second harmonic, then is assembled and the 4th through the second lens 12-3
After optical filter 12-4 leaching, strength signal is obtained by photodetector 12-5 and is used for trigger collection.
The stokes light generation module 5 includes the first coupling mirror 5-1, the nonlinear optical fiber 5-2, second set gradually
The output wave-number range of coupling mirror 5-3 and third optical filter 5-4, output wave-number range and the first frequency comb light source 1-1
Difference matches sample to be tested Raman signal wave number, i.e. wave number difference and sample to be tested Raman peaks beam location is almost the same.
The nonlinear optical fiber 5-2 is photonic crystal fiber or high refractive index nonlinear optical fiber, the anti-stoke that is concerned with
After this raman spectral signal is reflected through reflecting mirror 7-2, the second optical filter 6-2 filters, lens 10 converge, by coherent
Signal detection module 11 detects, and the coherent signal detection module 11 is highly sensitive photodetector.
The first dispersion adjustment element 4-1 and through the second dispersion adjustment element 4-2 make two-way light pulse have it is identical
Chirp coefficient α, light pulse by femtosecond extend at picosecond.
There are repetition rate difference δ f for the light pulse of the two-way introducing linear chripr, make pulse pair with relative delayMutually scanned for interval, with the quick self-scanning characteristic of no moving parts optics, and scan period when
Between be T=1/ δ fr, a given relative delay moment, all energy are all focused on a Raman energy level and are excited
Detection obtains the spectrum point information of corresponding Raman frequency shift, and different relative delays correspond to different Raman frequency shift spectrum points, and effectively
Spectrographic detection interval △ Ω determines there is relational expression by delay interval △ τ
The process to original spectral data processing includes: envelope extraction a) based on low-pass filtering；B) it is based on
The resonance signal phase extraction of expectation maximization and baseline correction and c) intensity correction obtain corresponding with spontaneous Raman spectrum
CARS Raman spectrum.
By the 3-D scanning to the micro- focusing and 9 objective table of Sample Scan module that load sample to be tested, sample is obtained
Raman spectral information on three-dimensional space, realizing has spectral-spatial four-dimensional imaging.
Regulation of the invention refers to intensity and polarization regulation.
Compared with prior art, the beneficial effects of the present invention are:
1. can easily be realized between picosecond pulse pair by the flexible control of repetition rate difference between double frequency comb light sources
The regulation of relative delay step-length and efficiently light pulse optics mutually scans, avoids additional slow mechanical scan table and its control
System has and realizes quick dynamic spectrum detectivity.
It, can be with 2. adjusted using the chirp that the double light comb light source of Gao Zhongying, nonlinear device open up spectrum and dispersion adjustment element
The high-resolution and wide spectrum covering detection of CARS spectrum are realized simultaneously.
Detailed description of the invention
Fig. 1 is double frequency comb coherent anti-stokes Raman spectroscopy detection principle schematic diagrames of the invention.
Fig. 2 is double frequency comb coherent antistockes Raman spectroscopy detection system block diagrams of the invention.
Fig. 3 is that present invention detection coherent anti-stokes Raman spectroscopy restores flow diagram.
Fig. 4 is double frequency comb coherent anti-stokes Raman spectroscopy micro-imaging result diagrams of the invention.
Specific embodiment
The embodiment that the present invention will be described in detail with reference to the accompanying drawings and examples.
The present invention focuses CARS spectrographic detection technology as spectrum in a kind of cleverly method and provides using double frequency comb light sources
Completely new fast-pulse time domain relative delay scan solution.Fig. 1 illustrates realization process of the invention: source from principle
From two column pulses of double frequency comb light sources, a column are used as pump light, repetition fr, another column are as stokes light, repetition fr
+δfr.Because there are a small difference δ f for the repetition rate difference of two column pulsesr, with relative time delay interval δ between two column pulses
fr/fr 2It is gradually staggered, as shown in Figure 1 b.In the process, if pump light and stokes light are the femtosecond of transform limit
Pulse, then CARS process will excite a large amount of Raman energy level to be difficult to directly distinguish simultaneously；If by Dispersion managed, by transform limit
Pulse becomes chirped pulse and the two chirp coefficient α having the same, then at the time of one given, pump light and Stokes
Light focuses on a Raman energy level Ω, as shown in Figure 1a.With the variation of two column interpulse delays, corresponding Raman energy level value hair
Changing, as shown in the figure from Ω1Scan Ω2；When acquisition using with pump light synchronous acquisition mode, then it is available such as Fig. 1 c
Shown in Raman frequency shift and time at mapping relations Wideband Raman spectroscopic data.
Fig. 2 gives double frequency comb coherent antistockes Raman spectroscopy detection system embodiments based on the above principles,
It include: the double light comb light source modules 1 for having the output of fine difference for generating two repetition rate differences；It is produced for stokes light
Raw stokes light generation module 5；It is collected for pump light and stokes light focusing and anti-Stokes light, sample three-dimensional
The micro- focusing and Sample Scan module 9 of scanning；For positioning pump light in the sampling trigger mode of stokes light overlapping region
Block 12；And coherent signal detection module 11, acquisition 13 and analysis and processing module 14；It additionally include light function
Optical component needed for rate, light pulse adjusting etc..
Specifically, the central wavelength of double light comb light source modules 1 is in near-infrared, and its first frequency comb light source 1-1 and
The repetition rate f of two frequency comb light source 1-2rWith fine difference, i.e. fr1=fr2+δfr, wherein fr1For the first frequency comb light source 1-
1 frequency, fr2For the frequency of the second frequency comb light source 1-2, δ frIndicate that the repetition rate of two light sources is poor, value is much smaller than weight
Complex frequency fr。
The output light of first frequency comb light source 1-1 is successively passed through as the pump light and detection light, the output light of detection process
First half-wave plate 2-1 and the first polarization splitting prism 3-1, transmissive portion, that is, P polarisation is through the first dispersion adjustment element 4-1 lead-in
Property chirp, the output light of stokes light generation module 5 introduces linear chrip through the second dispersion adjustment element 4-2, and two-way introduces
The light pulse of linear chrip closes beam by dichroic mirror 8, is then coupled into micro- focusing and Sample Scan mould 9.Wherein the first dispersion tune
It saves element 4-1 and makes two-way light pulse chirp coefficient α having the same through the second dispersion adjustment element 4-2, light pulse is by flying
Second extend at picosecond.
The output light of second frequency comb light source 1-2 is complete successively through the second half-wave plate 2-2 and the second polarization splitting prism 3-2
Full by part, that is, P polarisation the first coupling mirror 5-1 is input to after third half-wave plate 2-3, pass through the second half-wave plate 2-2,
Two polarization splitting prism 3-2, third half-wave plate 2-3 and third optical filter 5-4 adjust the output of stokes light generation module 5
Power and output wave-number range.
First frequency comb light source 1-1 and the second frequency comb light source 1-2 used by the present embodiment is Yb dosed optical fiber
Laser.The repetition rate of laser is locked on rubidium atomic clock by the way that piezoelectric ceramics control chamber is long, realizes the essence of repetition
Really control.The repetition rate of above-mentioned light source is 100MHz, and repetition tunable range is ± 50kHz.Light source output pulse center
Wavelength is about 1060nm, and bandwidth is about 50nm, and pulse width is about 60fs, and pulse energy is about 20nJ.
Stokes light generation module 5 includes the first coupling mirror 5-1 set gradually, nonlinear optical fiber 5-2, the second coupling
The difference of the output wave-number range of mirror 5-3 and third optical filter 5-4, output wave-number range and the first frequency comb light source 1-1
Sample to be tested target Raman signal wave number is matched, i.e. wave number difference and sample to be tested Raman peaks beam location is almost the same.It is non-thread
Property optical fiber 5-2 be photonic crystal fiber or high refractive index nonlinear optical fiber, coherent antistockes Raman spectroscopy signal is through filtering
It after piece 6-2 leaching, is detected by coherent signal detection module 11, coherent signal detection module 11 is
Highly sensitive photodetector.
Sampling trigger module 12 include set gradually the first lens 12-1, nonlinear crystal 12-2, the second lens 12-3,
4th optical filter 12-4 and photodetector 12-5 obtains triggering arteries and veins using the second harmonic generation method of two type-Ⅱphase matchings
Punching, process are as follows: part, that is, S polarisation that the output light of the first frequency comb light source 1-1 is reflected by the first polarization splitting prism 3-1 into
Enter the first lens 12-1, part, that is, S that the output light of the second frequency comb light source 1-2 is reflected by the second polarization splitting prism 3-2 is inclined
Light is adjusted to P polarisation through the 4th half-wave plate 2-4, then is transmitted into the first lens 12-1 through the first polarization splitting prism 3-1, warp
First lens 12-1 convergence is incident on nonlinear crystal 12-2 and forms second harmonic, then assembles and the 4th filter through the second lens 12-3
After mating plate 12-4 leaching, strength signal is obtained by photodetector 12-5 and is used for trigger collection.
The present embodiment is towards the Raman fingerprint region 800-1800cm for being rich in chemical information-1It is detected.In implementation, pass through this
Nonlinear optical fiber in lentor photogenerated module 5 is corresponded near the wavelength frequency displacement to 1260nm of the second frequency comb light source 1-2
Output pulse width is about 80fs.The output power and centre frequency of stokes light can be incident on nonlinear optical by changing
Fine power and polarization direction control, that is, pass through the second half-wave plate 2-2, the second polarization splitting prism 3-2, third half-wave plate 2-3
This power combines to realize with polarization adjustment.In the present embodiment, central wavelength can carry out between 1180nm to 1300nm
It adjusts.
The pulse that above-mentioned first frequency comb light source 1-1 and stokes light generation module 5 export is femtosecond pulse, is needed
Dispersion adjustment element 4-1,4-2 introduce linear chrip, and femtosecond pulse is extended into picosecond pulse.In the present embodiment, it selects high
Refractive index glass SF 57 introduces quadratic phase, and introducing total quadratic phase is 52000fs2, corresponding chirp coefficient α is 3.03 ×
10-6fs-2；After introducing chirp, two pulses become about 2~4 picoseconds of picosecond pulse.In practical application, different length can be matched
57 glass of SF, realize the adjustment target of different chirp coefficients.
The chirped pulse that above-mentioned two-way is derived from two optical frequency com light sources focuses on sample to be tested through micro-, generates
Anti-Stokes light the CARS signal of sample is obtained through collection, filtering, the detection of highly sensitive photodetector 11.The present embodiment
In, the repetition rate difference between double light comb light sources can be adjusted in light source repetition tunable range.It is poor with repetition rate
It is taken as 1200Hz, then can acquire 1200 width of CARS spectrum each second；Pulse relative scanning step-length is 120fs when measurement, is had
Imitating spectrographic detection interval is about 12cm-1.If the repetition of optical frequency com is changed to 1GHz in embodiment, there are following characteristics:
1, keep repetition rate difference consistent with current embodiment, then when it is constant can to acquire CARS spectrum number each second, but measuring
Pulsion phase is reduced to 1.20fs to scanning step, and effective spectrographic detection interval is about 0.12cm-1, resolution ratio greatly improves.
2, keep effective spectrum spy interval constant, then repetition rate difference can be taken as 120kHz, available CARS spectrum per second
Number reaches 120000 width, and spectrographic detection speed greatly promotes.Thus it is not difficult to find that Gao Zhongying frequency comb light source is for inventive
The promotion of energy has very big meaning.
In the present embodiment, light source repetition is 100MHz, and respective pulses interval is about 10ns, and chirped pulse width is only
Several picoseconds, in the mutual scanning process of double light combs of entire 10ns span, it is overlapping that the region only less than 10 picoseconds is that pulse has,
Effective impulse overlaps limited time.For this purpose, effective trigger signal is obtained using the method that second harmonic generates in the present embodiment,
So that system only starts to acquire in the two-way pulse matching stage.The generation process of trigger signal are as follows: double light comb light source module outputs
Light pulse through half-wave plate 2-1,2-2,2-4 and PBS3-1, incident sampling trigger module 12 after beam is closed in 3-2 regulation, through in module
Nonlinear crystal 12-2 is incident in first lens 12-1 convergence, and used herein is BBO Crystal.Due to from two optical frequencies
Comb out the pulse polarization state penetrated be it is orthogonal, meet the second type-Ⅱphase matching condition, can produce second harmonic signal:
I2ω(τ)∝∫Iω,Comb1(t)Iω,Comb2(t+τ)dt
Wherein, Iω,Comb1And Iω,Comb2It is that optical frequency com 11-1 and optical frequency com 21-2 are focused on BBO respectively
Energy, I2ωIt is the signal strength of the second harmonic generated, τ is the relative time delay between two-way pulse.When two-way pulse is in time domain
On when being completely coincident, second harmonic signal has a maximum signal strength, the Strength Changes period by two frequency combs repetition
Difference on the frequency determines.The maximum value of second harmonic signal represents the zero time delay position between two-way pulse, adopts as CARS spectrum
The trigger signal of collection realizes the spectroscopic acquisition in the setting time window of zero-lag two sides one, substantially reduces invalid data
Collection capacity is conducive to generating date and the display of practical CARS spectroscopic data.
In the present embodiment, the original spectral data that triggered high speed acquisition obtains carries out spectrum by data handling procedure and answers
It is former.The basic procedure of data processing is as shown in Figure 3: 1 uses the envelope extraction method of low-pass filtering, removes on original CARS signal
The carrier signal of the laser repetition rate of superposition；2 use resonance signal phase extraction and baseline school based on expectation maximization
The just cheap influence of reduction off-resonance background and baseline；3 on the basis of the above, and being focused under CARS difference registration according to spectrum has
Effect this intensity modulated of modulate intensity relationship is usually stable, intensity correction of the completion to detecting light spectrum.After above-mentioned processing,
Available CARS Raman spectrum corresponding with spontaneous Raman spectrum.
Fig. 4 gives the experimental result that the present embodiment realizes spectral-spatial four-dimensional imaging.Embodiment is using retinoic acid and β-
The mixing sample of carrotene is as detected object.In fig.4, respectively with 1560cm-1And 1520cm-1As retinoic acid with
Beta carotene at image contrast, obtaining the three-dimensional imaging figure of two kinds of molecules, (wherein linen for retinoic acid, grey black is
Beta carotene)；Entire areas imaging is 22 μm of 100 μ m, 100 μ m, 1 μm of 1 μ m of pixel size, 1 μ m, single pixel
Time of measuring 0.5 μ s, refresh rate 1200Hz.Any one section can be taken out from three-dimensional figure, obtain the two dimension of two kinds of molecules
Distribution, as shown in Figure 4 b, this can be used for analyzing the space structure of substance more fully hereinafter.In addition, three-dimensional broad band CARS spectrum
Imaging means that any one pixel from 3-D image can obtain a complete Raman spectrum, such as Fig. 4 c institute
Show, therefore entire micro-image contains spectral information abundant, can be used to implement to a variety of qualitative of complication system itself
And quantitative analysis, this is that narrowband CARS or SRS micro-imaging is not had.
Above-described embodiment is merely to illustrate the present invention, wherein the central wavelength of double light comb light sources, spectral bandwidth, generation this
The central wavelength of lentor light, spectral bandwidth, the detection of chirped pulse width and spectral signal and flow chart of data processing all may be used
To carry out equivalent arrangements, transformation and improvement based on the technical solution of the present invention according to detection demand, should not exclude at this
Except the protection scope of invention.
Claims (10)
1. a kind of double frequency comb spectrum focus coherent antistockes Raman spectroscopy detection system characterized by comprising
Double light comb light source modules (1) have the first frequency comb light source (1-1) and the second optical frequency of fine difference including repetition rate difference
It combs light source (1-2), pump light and detection light of the output light of the first frequency comb light source (1-1) as detection process；
Stokes light generation module (5), it is non-thread using optical fiber using the output light of the second frequency comb light source (1-2) as input light
Property effect realize optical frequency offset, obtain stokes light；
Micro- focusing and Sample Scan module (9), receive the focusing for closing the pump light and stokes light of beam and anti-Stokes
Light collection, sample 3-D scanning, obtain coherent antistockes Raman spectroscopy signal；
Coherent signal detection module (11) detects the coherent antistockes Raman spectroscopy signal；
It samples trigger module (12), for positioning pump light in stokes light overlapping region, realizes pulse orientation triggering spectrum
Acquisition；
Acquisition module (13), acquisition obtain the original spectral data of coherent antistockes Raman spectroscopy signal；
Analysis and processing module (14) carries out spectrum recovering to original spectral data processing.
2. double frequency comb spectrum focus coherent antistockes Raman spectroscopy detection system, feature according to claim 1
It is, the central wavelength of double light comb light source modules (1) is in near-infrared, the first frequency comb light source (1-1) and the second light
Frequency combs the repetition rate f of light source (1-2)rWith fine difference, i.e. fr1=fr2+δfr, wherein fr1For the first frequency comb light source (1-
1) frequency, fr2For the frequency of the second frequency comb light source (1-2), δ frIndicate that the repetition rate of two light sources is poor, value is much smaller than
Repetition rate fr。
3. double frequency comb spectrum according to claim 1 or claim 2 focus coherent antistockes Raman spectroscopy detection system, special
Sign is that the output light of the first frequency comb light source (1-1) is successively through the first half-wave plate (2-1) and the first polarization splitting prism
(3-1), transmissive portion, that is, P polarisation introduce linear chrip through the first dispersion adjustment element (4-1) and are filtered with the first optical filter (6-1)
Take the chirped pulse of required frequency range, the output light of the stokes light generation module (5) through reflecting mirror (7-1) reflection and
Second dispersion adjustment element (4-2) introduces linear chrip, and the light pulse that two-way introduces linear chrip closes beam by dichroic mirror (8), so
After be coupled into it is micro- focusing with Sample Scan module (9)；
The output light of the second frequency comb light source (1-2) is successively through the second half-wave plate (2-2) and the second polarization splitting prism (3-
2), transmissive portion, that is, P polarisation is input to the first coupling mirror (5-1) after third half-wave plate (2-3)；Pass through the second half-wave plate (2-
2), the second polarization splitting prism (3-2), third half-wave plate (2-3) and third optical filter (5-4) realize Stokes photogenerated
The adjusting of module (5) output power and output wave-number range.
4. double frequency comb spectrum focus coherent antistockes Raman spectroscopy detection system, feature according to claim 3
Be, sampling trigger module (12) include the first lens (12-1) set gradually, nonlinear crystal (12-2), second thoroughly
Mirror (12-3), the 4th optical filter (12-4) and photodetector (12-5), utilize the second harmonic generation side of two type-Ⅱphase matchings
Method obtains trigger pulse, process are as follows: the output light of the first frequency comb light source (1-1) is anti-by the first polarization splitting prism (3-1)
The part penetrated i.e. S polarisation enters the first lens (12-1), and the output light of the second frequency comb light source (1-2) is by the second polarization spectro rib
Part, that is, S polarisation of mirror (3-2) reflection, is adjusted to P polarisation through the 4th half-wave plate (2-4), then through the first polarization splitting prism (3-
1) it is transmitted into the first lens (12-1), it is secondary humorous to be incident on nonlinear crystal (12-2) formation through the first lens (12-1) convergence
Wave, then assemble through the second lens (12-3) with after the 4th optical filter (12-4) leaching, intensity is obtained by photodetector (12-5)
Signal is used for trigger collection.
5. double frequency comb spectrum focus coherent antistockes Raman spectroscopy detection system, feature according to claim 3
Be, the stokes light generation module (5) include the first coupling mirror (5-1) set gradually, nonlinear optical fiber (5-2),
Second coupling mirror (5-3) and third optical filter (5-4) export the output of wave-number range and the first frequency comb light source (1-1)
The difference of wave-number range matches sample to be tested Raman signal wave number, i.e. wave number difference and sample to be tested Raman peaks beam location is basic
Unanimously.
6. double frequency comb spectrum focus coherent antistockes Raman spectroscopy detection system, feature according to claim 5
It is, the nonlinear optical fiber (5-2) is photonic crystal fiber or high refractive index nonlinear optical fiber, the coherent
Raman spectral signal is reflected through reflecting mirror (7-2), the second optical filter (6-2) filters, after lens (10) convergence, by this relevant anti-support
The detection of gram this signal detection module (11), the coherent signal detection module (11) are highly sensitive photodetection
Device.
7. double frequency comb spectrum focus coherent antistockes Raman spectroscopy detection system, feature according to claim 3
Be, the first dispersion adjustment element (4-1) and through the second dispersion adjustment element (4-2) make two-way light pulse have it is identical
Chirp coefficient α, light pulse by femtosecond extend at picosecond.
8. double frequency comb spectrum focus coherent antistockes Raman spectroscopy detection system, feature according to claim 7
It is, there are repetition rate difference δ f for the light pulse of the two-way introducing linear chripr, make pulse pair with relative delay
It is mutually scanned for interval, with the quick self-scanning characteristic of no moving parts optics, and the time of a scan period is T=1/
δfr, a given relative delay moment, all energy, which all focus on a Raman energy level, carries out excitation detection, obtains
The spectrum point information of corresponding Raman frequency shift, different relative delays correspond to different Raman frequency shift spectrum points, and effective spectrographic detection
It is spaced △ Ω and determines there is relational expression by delay interval △ τ
9. double frequency comb spectrum focus coherent antistockes Raman spectroscopy detection system, feature according to claim 1
It is, the process to original spectral data processing includes: the envelope extraction of (a) based on low-pass filtering；(b) based on most
The resonance signal phase extraction of big expectation method and baseline correction and (c) intensity correction, obtain corresponding with spontaneous Raman spectrum
CARS Raman spectrum.
10. double frequency comb spectrum focus coherent antistockes Raman spectroscopy detection system, feature according to claim 1
It is, by the 3-D scanning to the micro- focusing and Sample Scan module (9) objective table that load sample to be tested, obtains sample three
Raman spectral information on dimension space, realizing has spectral-spatial four-dimensional imaging.
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