CN105699356B - Judge the method that the fluorescence of Raman spectrum eliminates degree by comentropy - Google Patents
Judge the method that the fluorescence of Raman spectrum eliminates degree by comentropy Download PDFInfo
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Abstract
A method of judging that the fluorescence of Raman spectrum eliminates degree by comentropy, it is related to a kind of Raman spectrum fluorescence elimination method, it reduces criterion using the comentropy of discrete series as fluorescent component, fluorescence is gradually reduced from mixed signal, when comentropy reaches minimum, the fluorescence in mixed signal is completely eliminated.The present invention judges the elimination degree of fluorescence using comentropy, more scientific and reasonable, not by instrument wave number scope limitation, instrument performance is made to be not fully exerted, and increases the degree of freedom of Instrument Design and manufacture；And solve the limitation for needing that fluorescence residual condition is judged in particular range of wavelengths in prior art, to spectral region without particular/special requirement, it is suitable for the Instrument Design of different wave length setting.Also it can quickly and accurately obtain the Raman actual signal not interfered by fluorescence for meeting actual mechanism, application easy to spread in the case where not increasing equipment complexity and changing existing measurement custom.
Description
Technical field
It is especially a kind of that Raman spectrum is judged by comentropy the present invention relates to a kind of Raman spectrum fluorescence elimination method
The method that fluorescence eliminates degree.
Background technology
Laser Raman spectroscopy can provide molecular spectrum information, while having and being not easy by moisture interference, non-contact and not
The advantages that destroying sample, is a kind of qualitative and quantitative analysis means of fast development.But generated while Raman scattering excitation
Fluorescence generates interference to Raman spectrum identifiability and signal quality.
It has developed rapidly in recent years using the photosensitive miniature beam splitting type Raman spectrometer of array, advantage is simple in structure, is not necessarily to
Complex maintenance, but it uses hardware elimination fluorescence to interfere the complexity that can increase equipment, for example, utilizing the migration of Raman light
With stablizing relatively for fluorescence, is excited by dual wavelength and eliminate fluorescence, instrument cost and complexity can all be promoted.Baseline fitting is reduced
It is that current such Raman spectrometer disappears the main thought of fluorescence, most methods are reduced using spectrum baseline fitting to initial position,
It provides fluorescence and eliminates presentation, can not actually be explained from mechanism or substantially, it is as a result both untrue or unreasonable.
The another bleach effect for thering is technology to be gradually reduced using fluorescence intensity under strong illumination, fluorescence intensity entire lowering, this
Part measurement reflects the fluorescent characteristic in signal, and is gradually deducted from signal, the final fluorescence interference for eliminating Raman signal.
Using Raman signal between specific wave number migration area this flat characteristic is presented to judge whether fluorescence is cut down completely in the technology,
But with the proviso that must include the spectrum that this section is free of effective information in Instrument Design, limitation be constituted to Instrument Design.
Invention content
The technical problem to be solved by the present invention is to：A kind of fluorescence elimination degree judging Raman spectrum by comentropy is provided
Method, to solve, increase instrument cost and complexity, result of the existing technology are untrue, are construed as limiting to Instrument Design
Shortcoming.
Solving the technical solution of above-mentioned technical problem is：It is a kind of to judge that the fluorescence of Raman spectrum eliminates degree by comentropy
Method, this method is to reduce criterion as fluorescent component using the comentropies of discrete series, is gradually reduced from mixed signal
Fluorescence, when comentropy reaches minimum, the fluorescence in mixed signal is completely eliminated.
The present invention further technical solution be：This approach includes the following steps：
A, using the mixed signal of raman laser probe measurement sample, fixed-focus sets the time of integration, 2 groups of record with
Spectroscopic data under upper different momentsS；
B, serial weights are multiplied by later moment in time spectroscopic data successively, calculate the difference with previous moment spectroscopic data, obtains
Decline metric Δ to the fluorescence without Raman signalS；
C, metric Δ is declined to fluorescenceSNoise reduction is carried out, the fluorescence after noise reduction declines metric ΔSAs mixed signalS
In the fluorescence component that containsF S ；
D, it is gradually reduced from mixed signaln*△*F S ,nFor the step number reduced,n=1,2 ...,△To reduce step-length,F S For
Fluorescence component, and calculate often step and reducen*△*F S Comentropy afterwards；
E, judge that often step is reducedn*△*F S Whether comentropy afterwards is minimum value, if it is not, then step D is repeated, if
It is then to show that fluorescence reduces completion, obtains the pure Raman signal without fluorescence.
The present invention further technical solution be：In stepb, the serial weights are 0.95~1.05.
The present invention further technical solution be：It is described that metric Δ is declined to fluorescence in step CSIt is dropped
It makes an uproar selectionSAvitzky-Golay filters, it is the 1/10 of overall signal length to select the filtering of 2 ranks, window width.
The present invention further technical solution be：The step D includes following specific method：
D1, according to formula, calculate the comentropy of mixed signalH(X), formula
InP(a i ) it is mixed signalSTakeiThe probability of a luminous intensity,i=1,2 ...,Q, qValue is number of data points contained by spectrum；
Step-length △ is reduced in D2, setting, is gradually reduced from mixed signaln*△*F S ,nFor the step number reduced,n=1,2 ...,F S For fluorescence component, and calculates often step and reducen*△*F S Comentropy afterwards.
The present invention further technical solution be：The step-length △ that reduces is 0.01~0.1.
Due to using the above structure, the present invention by comentropy judge the fluorescence of Raman spectrum eliminate the method for degree with
The prior art is compared, and is had the advantages that：
1. the fluorescence of Raman spectrum really rationally, can be eliminated effectively：
The present invention is to reduce criterion as fluorescent component using the comentropy of discrete series, is gradually reduced from mixed signal
Fluorescence, when comentropy reaches minimum, the fluorescence in mixed signal is completely eliminated.Excite Raman light also can be same since light irradiates
Shi Jifa fluorescence, to generate interference to Raman light.However, Raman light and fluorescence and asynchronous, Raman information contained amount is apparent
Higher than fluorescence；Research confirms that the uncertainty of the mixed signal containing fluorescence is always greater than pure Raman signal, i.e., signal is completely by drawing
Graceful spectrum is constituted, and entropy is minimum.Therefore, the present invention really can rationally, effectively eliminate the fluorescence of Raman spectrum.
2. method is easy：
It is unrelated with amplitude since the size of the entropy of mixed signal is only related with the composition situation of the signal, it need not mark
Other data preprocessing methods such as standardization are suitable for the processing of each single-measurement data；Therefore, the present invention is repeatedly surveyed with needs
The methods of the order judgement that measuring could use is compared, and method of the invention is more easy.
3. the degree of freedom of Instrument Design and manufacture can be increased：
The present invention judges the elimination degree of fluorescence using comentropy, more scientific and reasonable, not by instrument wave number scope limitation,
So that instrument performance is not fully exerted, increases the degree of freedom of Instrument Design and manufacture.Therefore, the present invention solves the prior art and needs
The limitation that fluorescence residual condition is judged in particular range of wavelengths is suitable for different wave length and sets to spectral region without particular/special requirement
The Instrument Design set.
4. equipment used in is simple, low cost：
The acquisition requirement of the present invention and acquisition step and existing acquisition method indifference, equipment is simple, low cost, not
In the case of increasing equipment manufacturing cost, measurement attachment and changing existing acquisition step, quickly and accurately obtains and meet actual mechanism
The Raman actual signal not interfered by fluorescence, application easy to spread.
In the following, judging that the fluorescence of Raman spectrum eliminates degree by comentropy to the present invention in conjunction with the accompanying drawings and embodiments
The technical characteristic of method is further described.
Description of the drawings
Fig. 1：The spectrogram measured in one step A of embodiment,
Fig. 2：In one step B of embodiment, the spectrum comparison diagram subtracted using weighting subtractive and non-weighted difference,
Fig. 3：The spectrogram of the fluorescence component contained in mixed signal described in one step C of embodiment,
Fig. 4：In one step D of embodiment, comentropy with the amount of reducing figure of changing,
Fig. 5：In one step E of embodiment, the obtained Raman signal without fluorescenceRWith the mixed signal of original measurementSIt
Between spectrum comparison diagram；
Fig. 6：In 200-1800cm-1When band signal, comentropy is with the amount of reducing figure of changing；
Fig. 7：The fluorescence for simulating Raman-fluorescence mixed signal is eliminated in experiment, is simulated respectively using Lorentzian pair
Should in the spectral curve of Raman and fluorescence,
Fig. 8：The fluorescence for simulating Raman-fluorescence mixed signal is eliminated in experiment, 1 times of Raman signal and 5 times of fluorescence signals
Design sketch is summed it up,
Fig. 9：The fluorescence for simulating Raman-fluorescence mixed signal is eliminated in experiment, and 1 times of Raman signal has summed it up -1 ~ 5 times
Fluorescence comentropy figure of changing.
Specific implementation mode
A method of judging that the fluorescence of Raman spectrum eliminates degree by comentropy, this method is using discrete series
Comentropy reduces criterion as fluorescent component, and fluorescence is gradually reduced from mixed signal, when comentropy reaches minimum, mixing letter
Fluorescence in number is completely eliminated.
This approach includes the following steps：
A, using the mixed signal of raman laser probe measurement sample, fixed-focus sets the time of integration, 2 groups of record with
Spectroscopic data under upper different momentsS；
B, serial weights are multiplied by later moment in time spectroscopic data successively, which is 0.95~1.05, is calculated with before
The difference of one moment spectroscopic data obtains the fluorescence without Raman signal and declines metric ΔS；
C, it selectsSAvitzky-Golay filters decline metric Δ to fluorescenceSNoise reduction is carried out, the filtering of 2 ranks, window are selected
Mouth width degree is the 1/10 of overall signal length, and the fluorescence after noise reduction declines metric ΔSAs mixed signalSIn the fluorescence that contains
ComponentF S ；
D, it is gradually reduced from mixed signaln*△*F S, nFor the step number reduced,n=1,2 ...,△To reduce step-length,F S For
Fluorescence component, and calculate often step and reducen*△*F S Comentropy afterwards；
D1, according to formula, calculate the comentropy of mixed signalH(X), formula
InP(a i ) it is mixed signalSTakeiThe probability of a luminous intensity,i=1,2 ...,Q, qValue is number of data points contained by spectrum；
Step-length △ is reduced in D2, setting, is gradually reduced from mixed signaln*△*F S ,nFor the step number reduced,n=1,2 ...,F S For fluorescence component, and calculates often step and reducen*△*F S Comentropy afterwards；
E, judge that often step is reducedn*△*F S Whether comentropy afterwards is minimum value, if it is not, then step D is repeated, if
It is then to show that fluorescence reduces completion, obtains the pure Raman signal without fluorescence.
The following is specific embodiments of the present invention：
Embodiment one：
A method of judging that the fluorescence of sucrose Raman spectrum eliminates degree by comentropy, this method includes following step
Suddenly：
A, using raman laser probe 785nm laser excitations, sucrose Raman spectrum, fixed-focus, when setting integrates are measured
Between 10s, time interval 30s measures 2 times, record gained mixed signalS 1、 S 2, as shown in fig. 1,S 1For the measurement light at moment 1
Spectrum,S 2For the measure spectrum at moment 2；
B, the weights for adjusting 2 spectrum of moment are 1.028, with previous moment spectrum subtraction, obtain effectively eliminating drawing therein
The fluorescence of graceful ingredient declines decreasing concentration magnitude ΔS, respectively by the spectrum of subtractive after weightingS 3With the spectrum for not weighting direct subtractiveS 4Make
Comparison is as shown in Fig. 2, as can be seen from Figure 2, using weighting subtractive, can effectively eliminate Raman ingredient therein；
C, it selectsSAvitzky-Golay filters decline metric Δ to fluorescenceSNoise reduction is carried out, the filtering of 2 ranks, window are selected
Mouth width degree is 91；Fluorescence after noise reduction declines metric ΔSAs mixed signalSIn the fluorescence component that containsF S , such as Fig. 3 institutes
Show；
D, it is gradually reduced from mixed signaln*△*F S ,nFor the step number reduced,n=1,2 ...,△To reduce step-length,F S For
Fluorescence component, and calculate often step and reducen*△*F S Comentropy afterwards, specific method are：
D1, according to formula, the comentropy of mixed signal is calculated, in formulaP
(a i ) it is mixed signalSTakeiThe probability of a luminous intensity,i=1,2 ...,Q, qValue is number of data points contained by spectrum；
Step-length △ is reduced in D2, setting, is gradually reduced from mixed signaln*△*F S ,nFor the step number reduced,n=1,2 ...,F S For fluorescence component, and calculates often step and reducen*△*F S Comentropy afterwards；
E, judge that often step is reducedn*△*F S Whether comentropy afterwards is minimum value, if it is not, then step D is repeated, if
It is then to show that fluorescence reduces completion, obtains the pure Raman signal without fluorescence.Fig. 4 is comentropy with the amount of reducing situation of change,F S 5.83 times when, there is minimum value in comentropy, is from original mixed signalSIt is middle to deduct corresponding 5.83 timesF S Afterwards, it obtains
Raman signal R without fluorescence；The Raman signal without fluorescence that Fig. 5 isRWith the mixed signal of original measurementSBetween
Spectrum comparison diagram.
Present inventor also selects 200-1800cm-1Band signal calculates comentropy, as shown in fig. 6, in fluorescence
ComponentF S 5.88 times there is minimum value, with using in embodiment one in 200-3000cm-1The comentropy of the calculating of band signal
5.83* when minimum valueF S Error be less than 1%, show that the present invention can not depend on specific range of signal, and obtain consistent
Effective result.
The elimination degree of fluorescence is judged using comentropy, it is more scientific and reasonable, not by instrument wave number scope limitation, make instrument
Performance is not fully exerted, and increases the degree of freedom of Instrument Design and manufacture.The present invention, which solves, to be needed in the prior art specific
Wave-length coverage judges the limitation of fluorescence residual condition, to spectral region without particular/special requirement, is suitable for the instrument of different wave length setting
Design.In the case of not increasing equipment complexity and changing existing measurement custom, it can quickly and accurately obtain and meet reality
The Raman actual signal of mechanism not interfered by fluorescence.
In addition, fluorescence content is 0 when in order to demonstrate,prove comentropy with minimum value, present inventor has also made simulation and has drawn
Fluorescence in graceful-fluorescence mixed signal eliminates experiment：
1. simulating the curve of spectrum corresponding to Raman and fluorescence respectively using Lorentzian, as shown in Figure 7.
2. the Raman of simulation and fluorescence signal are summed it up, the mixed signal that can be simulated.Fig. 8 is 1 times of Raman signal and 5
The adduction effect of times fluorescence signal.
3. calculating simulation Raman signal sums it up the information entropy after the fluorescence of different content respectively.The Raman that Fig. 9 is 1 times is believed
Number adduction comentropy situation of change of -1 ~ 5 times of fluorescence, it can be seen that fluorescence content is 0 when comentropy has minimum value,
Output is the Raman signal without fluorescence.
Claims (5)
1. a kind of method judging that the fluorescence of Raman spectrum eliminates degree by comentropy, it is characterised in that：This method is to use
The comentropy of discrete series reduces criterion as fluorescent component, and fluorescence is gradually reduced from mixed signal, when comentropy reaches most
Hour, the fluorescence in mixed signal is completely eliminated；This approach includes the following steps：
A, using the mixed signal of raman laser probe measurement sample, fixed-focus sets the time of integration, and 2 groups of record or more is no
Spectroscopic data under in the same timeS；
B, serial weights are multiplied by later moment in time spectroscopic data successively, calculate the difference with previous moment spectroscopic data, obtains not
Fluorescence containing Raman signal declines metric ΔS；
C, metric Δ is declined to fluorescenceSNoise reduction is carried out, the fluorescence after noise reduction declines metric ΔSAs mixed signalSIn contain
Some fluorescence componentsF S ；
D, it is gradually reduced from mixed signaln*△*F S ,nFor the step number reduced,n=1,2 ...,△To reduce step-length,F S For fluorescence
Component, and calculate often step and reducen*△*F S Comentropy afterwards；
E, judge that often step is reducedn*△*F S Whether comentropy afterwards is minimum value, if it is not, then step D is repeated, if it is, table
Bright fluorescence reduces completion, obtains the pure Raman signal without fluorescence.
2. the method according to claim 1 for judging that the fluorescence of Raman spectrum eliminates degree by comentropy, feature exist
In：In stepb, the serial weights are 0.95~1.05.
3. the method according to claim 1 for judging that the fluorescence of Raman spectrum eliminates degree by comentropy, feature exist
In：It is described that metric Δ is declined to fluorescence in step CSCarry out noise reduction selectionSAvitzky-Golay filters select 2
Rank filters, and window width is the 1/10 of overall signal length.
4. the method according to claim 1 for judging that the fluorescence of Raman spectrum eliminates degree by comentropy, feature exist
In：The step D includes following specific method：
D1, according to formula, calculate the comentropy of mixed signalH(X), in formulaP(a i ) it is mixed
Close signalSTakeiThe probability of a luminous intensity,i=1,2 ...,Q, qValue is number of data points contained by spectrum；
Step-length △ is reduced in D2, setting, is gradually reduced from mixed signaln*△*F S ,nFor the step number reduced,n=1,2 ...,F S For
Fluorescence component, and calculate often step and reducen*△*F S Comentropy afterwards.
5. the method according to claim 4 for judging that the fluorescence of Raman spectrum eliminates degree by comentropy, feature exist
In：The step-length △ that reduces is 0.01~0.1.
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| CN108169201B (en) * | 2016-12-08 | 2020-07-28 | 同方威视技术股份有限公司 | Raman spectrum detection method for deducting package interference |
| CN108195817B (en) * | 2016-12-08 | 2020-09-15 | 同方威视技术股份有限公司 | Raman spectrum detection method for removing solvent interference |
| CN109752364B (en) * | 2019-03-11 | 2021-06-08 | 广西科技大学 | Asynchronous fading fluorescence elimination method of multi-component system Raman spectrum |
| CN109765212B (en) * | 2019-03-11 | 2021-06-08 | 广西科技大学 | Method for eliminating asynchronous fading fluorescence in Raman spectrum |
| CN110108689B (en) * | 2019-05-17 | 2021-07-30 | 广西科技大学 | Method for rapidly eliminating 3D fluorescence background noise |
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