CN103674251B - The identification of cosmic rays interference in Raman spectrum and removing method - Google Patents
The identification of cosmic rays interference in Raman spectrum and removing method Download PDFInfo
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- CN103674251B CN103674251B CN201310631802.8A CN201310631802A CN103674251B CN 103674251 B CN103674251 B CN 103674251B CN 201310631802 A CN201310631802 A CN 201310631802A CN 103674251 B CN103674251 B CN 103674251B
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Abstract
The invention discloses identification and the removing method of cosmic rays in a kind of Raman spectrum, comprise the steps: step 1, obtain the concussion peak in Raman spectrum and analyze, obtaining the concussion peak that cosmic rays is formed; Step 2, the concussion peak formed by cosmic rays corrects, thus eliminates the interference of cosmic rays.The inventive method comparatively accurately and simply can identify the interference that in Raman spectrum, cosmic rays produces, and effectively eliminates these interference.
Description
Technical field
The present invention relates to astronomical images processing field, the identification of particularly cosmic rays interference in a kind of Raman spectrum and removing method.
Background technology
Raman spectrum embodies the Vibration Condition of different molecular group in material, accurately can carry out the qualitative and quantitative analysis of material.By feat of such advantage, Raman spectroscopy successful Application in industrial on-line analysis fields such as Chemical Manufacture, pipeline transmission, biochemical reaction monitorings.Highly sensitive Charged Couple (CCD) detecting device is widely used in imaging and spectrometer, but when using CCD detecting device, the charged high energy subatomic particle from the outer space can be detected, thus produces cosmic rays.Raman spectrometer is also adopt charge-coupled image sensor (CCD) to detect spectral signal, so Raman spectrum is also usually subject to the interference of cosmic rays.Cosmic rays is now the narrower sharp-pointed peak of a series of peak width in Raman spectrogram upper body, and these cosmic rayss make the Raman spectrogram gross distortion of test substance, cannot obtain the attribute information of normal test substance.Therefore need in Raman spectrogram, reject the interference of penetrating in universe.
Appearance due to cosmic rays is irregularities, all eliminate by the subjective judgement of people all the time, the removing method that neither one is unified, and this traditional human eye subjective judgement method has clearly shortcoming: 1. it is Raman signal that the cosmic rays that signal intensity is little is easy to be mistaken as.2. the Raman signal that some intensity is little can be considered to cosmic rays and be deleted by mistake again.Therefore need a clear and definite decision method to find cosmic rays, to reduce this unnecessary personal error.And after finding cosmic rays, also need a more accurate method to eliminate cosmic rays.
In order to remove in online Raman spectrum cosmic rays, " a kind of simple online Raman spectrum spike elimination method " [light scattering journal, V01.23, No.3,2011.Li Sheng, Dai Liankui] propose one simply based on moving window correlation analysis, the cosmic rays of residual error spectrum analysis and local linear fitting rejects algorithm.The document combines the advantage of residual error spectrum analysis, moving window correlation analysis simultaneously, effectively can detect the cosmic rays on optional position, and utilize local linear fitting to repair cosmic rays.
But the method determines that the process carrying out eliminating cosmic rays to it is more complicated, consuming time longer when being processed in a large number by computing machine, therefore needs a kind of better simply method identify and eliminate cosmic rays.
Summary of the invention
In order to comparatively accurately simultaneously again fairly simplely identify and eliminate the interference that cosmic rays produces, the invention provides identification and the removing method of cosmic rays interference in a kind of Raman spectrum, comprise the steps:
Step 1, carries out first derivation to original Raman spectrum, obtains having the single order spectrum at concussion peak continuously;
Step 2, judges whether each concussion peak is formed by cosmic rays, behind the concussion peak obtaining the formation of all cosmic rayss, enters step 3 one by one;
Step 3, corrects the concussion peak that cosmic rays is formed in original Raman spectrum, thus eliminates the interference of cosmic rays.
First derivation is carried out to original spectrum, those making in original Raman spectrogram occur that the position of raman characteristic peak and cosmic rays highlights, contribute to positioning the position at these peaks better, the more important thing is as the follow-up process carried out cosmic rays on the other hand, the position of Wave crest and wave trough will be obtained in the contact of this first order derivative, and the intensity level etc. of correspondence, as the foundation judged.
In step 2, judge that the concussion peak method that cosmic rays is formed is:
Step 2a, beam location residing for beam location residing for the crest obtaining waiting judging concussion peak and trough, thus obtain the peak width at this concussion peak;
Step 2b, compares this peak width with first threshold, and as being greater than this first threshold, then this concussion peak is Raman signal; As being less than first threshold, then enter next step;
Step 2c, obtain the peak height at concussion peak, by peak height divided by peak width, and compare with Second Threshold, as being less than this Second Threshold, then this concussion peak is Raman signal; As being greater than Second Threshold, then it is concussion peak that cosmic rays is formed.
The raman scattering intensity at concussion spike peak place is deducted the peak height that trough place raman scattering intensity can obtain this concussion peak.Due to cosmic rays, to have peak width narrower and comparatively sharp-pointed, therefore, by comparing peak width, the less Raman signal of some intensity can be prevented to be mistaken as and be cosmic rays and delete; By comparing the ratio of peak height and peak width, can prevent the less cosmic rays of some intensity from being retained by as Raman signal.
Wherein said first threshold is 4cm
-1.Cosmic rays is narrower, can obtain by experiment, and the peak width being greater than this threshold value can think Raman signal.
Wherein said Second Threshold is 1000.Can obtain by experiment, the signal being less than this value is comparatively mild, can think Raman signal.
In step 3, carry out replacement by the raman scattering intensity value at each wave number place in the wave-number range to cosmic rays place and correct concussion peak.
By the raman scattering intensity value at concussion peak is replaced, make the raman scattering intensity value of shaking peak place close to other positions, thus eliminate the concussion peak of cosmic rays generation.
The method that within the scope of the concussion peak formed by cosmic rays, the raman scattering intensity value at each wave number place carries out replacing is:
Step 3-1, if identify obtain cosmic rays institute produce concussion peak peak width be d, and shake peak comprise n wave number, so respectively get n-1 wave number as 2 (n-1) individual observed reading at the concussion peak left and right sides that this cosmic rays produces; If the wave number of wherein side, the concussion peak that this cosmic rays produces lacks m, then get m wave number again from opposite side, obtain 2(n-1 equally) individual wave number is as observed reading;
Step 3-2, using the wave number of described 2 (n-1) individual observed reading as independent variable, using raman scattering intensity corresponding for described 2 (n-1) individual observed reading as dependent variable, sets up unitary 2 (n-1)-1 equation of n th order n.
Step 3-3, described 2 (n-1) individual observed reading is substituted into respectively unitary 2 (n-1)-1 equation of n th order n that step 3-2 sets up, to solve an equation each term coefficient obtained in described unitary 2 (n-1)-1 equation of n th order n, namely obtain the relational expression between raman scattering intensity and wave number;
Step 3-4, substitutes into this unitary 2 (n-1)-1 equation of n th order n by each wave number in the wave-number range of cosmic rays place, be used for the Raman spectrum at each wave number place replaced in cosmic rays place wave-number range.
Near the top that may appear at Raman spectrum, concussion peak produced due to cosmic rays or end position, now the left side at earthquake peak or the wave number on right side individual less than n-1, then opposite side after obtaining n-1 wave number again more get the wave number of lacked number.Such as, the concussion peak that cosmic rays produces is positioned at end position, and n is 4, then lack 3 wave numbers in its right positions, therefore, after left side obtains 3 wave numbers, then gets 3 wave numbers, has 6 altogether as known observed reading.
By estimating the Raman signal near concussion peak, thus obtaining the Raman signal shaking peak position, making whole spectrum mild comparatively continuously, therefore more accurately eliminating cosmic rays interference.
The inventive method comparatively accurately and simply can identify the interference that in Raman spectrum, cosmic rays produces, and effectively eliminates these interference.
Accompanying drawing explanation
Fig. 1 is method flow diagram of the present invention;
Fig. 2 is the original Raman spectrum of sample 1 in first embodiment of the invention;
Fig. 3 is the first order derivative spectrogram of the original Raman spectrum of sample 1 in the first embodiment;
Fig. 4 is wave number 2358-2530cm in the first embodiment
-1the Raman spectrum of scope is eliminating the comparison before and after cosmic rays;
Fig. 5 is wave number 2024-2014cm in the first embodiment
-1scope Raman spectrum before and after elimination cosmic rays compares
Fig. 6 is that in the first embodiment, sample 1 is eliminated Raman spectrum before and after cosmic rays and compared;
Fig. 7 is the original Raman spectrum of 10 samples in second embodiment of the invention;
Fig. 8 is the first order derivative spectrogram of original Raman spectrum in second embodiment of the invention;
Fig. 9 is the Raman spectrum after eliminating cosmic rays in second embodiment of the invention;
Figure 10 is the original Raman spectrum of urea sample in third embodiment of the invention;
Figure 11 is based on the nitrogen isotope abundance predicted value of urea original spectrum and the correlationship figure of actual value in third embodiment of the invention;
Figure 12 be remove cosmic rays in third embodiment of the invention after Raman spectrum;
Figure 13 be remove cosmic rays in third embodiment of the invention after model to the correlationship figure of isotopic abundance predicted value and actual value.
Embodiment
Now the present invention is described in detail with accompanying drawing in conjunction with the embodiments.
First embodiment
In the present example, for sample 1, carry out the judgement of cosmic rays:
As shown in Figure 2, the original Raman spectrum of sample 1 first derivative spectrum after first derivation as shown in Figure 3 for the original Raman spectrum of sample 1.
Wave number 1630cm as shown in Figure 3
-1and 2300cm
-1near have little concussion peak, at wave number 2000cm
-1near have strong concussion peak.
Analyze these three concussion peaks:
1. wave number 1630cm is positioned at
-1neighbouring concussion peak, crest is positioned at wave number λ=1639cm
-1place, trough is positioned at λ=1627cm
-1place, calculates peak width d=1639-1627=12 > 4, can judge wave number 1630cm thus
-1neighbouring concussion peak is not cosmic rays.
2. wave number 2300cm is positioned at
-1neighbouring concussion peak, this crest is positioned at λ=2355cm
-1, the raman scattering intensity Y at crest place
max=65963.9, trough is positioned at wave number λ=2353cm
-1, trough place raman scattering intensity Y
min=63237.6; Calculate difference in height (peak height) h=Y between crest and trough
max-Y
min=2726.3, peak width d=2355-2353=2,
meet the Rule of judgment d≤4cm of cosmic rays
-1, and
wave number 2353cm can be judged thus
-1to 2355cm
-1between Raman response be caused by cosmic rays.
3. wave number 2000cm is positioned at
-1neighbouring concussion peak, this crest is positioned at wave number λ=2020cm
-1, crest place raman scattering intensity Y
max=74439; Trough is positioned at wave number λ=2017cm
-1, trough place raman scattering intensity Y
min=53396; Calculate difference in height (i.e. peak height) h=Y between crest and trough
max-Y
min=74439-53396=21043, peak width d=2020-2017=3,
meet the Rule of judgment d≤4cm of cosmic rays
-1, and
wave number 2017cm can be judged thus
-1to 2020cm
-1between Raman response caused by cosmic rays.
For sample 1, after identifying the concussion peak caused by cosmic rays, carry out the elimination of cosmic rays:
Elimination to first cosmic rays interference:
Step 1) obtains wave number 2355cm
-1to 2353cm
-1the cosmic rays peak width d at place is 2(d=2), wherein comprise three wave numbers and be respectively 2355cm
-1, 2354cm
-1and 2353cm
-1(i.e. n=3), then get 2 wave number 2357cm on the left of this wave-number range
-1, 2356cm
-1with 2 wave number 2352cm on right side
-1, 2351cm
-1for known 4 observed readings.
Step 2) be independent variable by the wave number of these 4 observed readings, and the raman scattering intensity of these 4 observed readings is dependent variable, sets up simple cubic equation Y=aX
3+ bX
2+ cX+d.
Step 3) brings this simple cubic equation into respectively known 4 observed readings, after solving an equation, the constant term and the every coefficient that obtain this simple cubic equation are a=-38.5256556971368, b=272137.560126769, c=-640774827.209553 and d=502922376875.37.
Step 4) wave-number range (from 2355cm
-1to 2353cm
-1) in each wave number (2355cm
-1, 2354cm
-1and 2353cm
-1) substituting into this simple cubic equation, can obtain for replacing cosmic rays place wave-number range (from λ
minto λ
maxbetween) in the Raman spectrum at each wave number place, the correction of cosmic rays can be realized.
Original raman scattering intensity value and the comparison eliminating the raman scattering intensity value after cosmic rays at three wave number places, place, concussion peak that table 1 produces for cosmic rays.
Table 1
To the elimination of second cosmic rays interference
1. in wave number at 2020-2017cm
-1the cosmic rays peak width d at scope place is 3, wherein comprises four wave numbers, is respectively 2020cm
-1, 2019cm
-1, 2018cm
-1and 2017cm
-1(i.e. n=4).Get 2023cm on the left of this wave-number range
-1, 2022cm
-1, 2021cm
-13 wave numbers at place and right side 2016cm
-1, 2015cm
-1, 2014cm
-13 wave numbers at place are as known six observed readings.
2. set the wave number of these six observed readings as independent variable, and the raman scattering intensity of these six observed readings is dependent variable, sets up unitary quintic equation Y=aX
5+ bX
4+ cX
3+ dX
2+ eX+f.
3. these known six observed readings are substituted into this unitary quintic equation respectively, the constant term and the every coefficient that obtain this unitary quintic equation after solving an equation are as follows:
a=2.756291794912280173312461714773
b=-27812.458416779283631261328421842
c=112256922.85724283313127778844129
d=-2265460365 10.2738270327 5611989304
e=228596398876407.07883407872267623
f=-9226603734 3097082.8988785981 21169
4. then wave-number range at 2020-2017cm
-1interior each wave number (2020cm
-1, 2019cm
-1, 2018cm
-1and 2017cm
-1) substituting into this unitary quintic equation, can obtain for replacing cosmic rays place wave-number range (from λ
minto λ
maxbetween) in the Raman spectrum at each wave number place, the correction of cosmic rays can be realized.
The comparison of the value of the original raman scattering intensity that table 2 is four wave number places, cosmic rays place and the raman scattering intensity after eliminating cosmic rays.
Table 2
Second embodiment
The second embodiment of the present invention carries out judgement and the elimination of cosmic rays in Raman spectrum for other 10 samples.Wherein, contain 10 samples in Fig. 7 to Fig. 9, owing to only needing the interference observing cosmic rays in each 10 samples, therefore in figure, multiple sample is distinguished.
Fig. 7 is the original Raman spectrogram of 10 samples, can see there are many narrow peaks sharply, be the interference of cosmic rays in figure.Fig. 8 is the first derivative spectrum figure of 10 original Raman spectrums of sample.Then according to the inventive method, first carry out the identification of cosmic rays, then set up unitary polynomial equation and eliminate cosmic rays, Raman spectrum after the interference of 10 sample elimination cosmic rayss as shown in Figure 8, can see that the sample after eliminating cosmic rays interference eliminates sharp-pointed narrow peak, remain the Raman signal that signal is stronger simultaneously.
In order to verify the validity of this cosmic rays removing method, cosmic rays removing method is applied in the detection of Raman spectrum for urea nitrogen isotopic abundance.
3rd embodiment
Figure 10 to Figure 13 contains 43 samples, for carrying out qualitative observation, not needing to distinguish, therefore do not distinguish sample in figure between each sample.
Gather the Raman spectrum with 8 nitrogen isotope abundance gradient urea, amount to 43 samples, as shown in Figure 10, the specifying information of urea sample is as shown in table 3 for the original Raman spectrum of these 43 samples.
Table 3
Isotopic abundance (%) | Number of samples |
50.15 | 6 |
40.19 | 6 |
30.12 | 6 |
20.21 | 6 |
10.13 | 6 |
5.2 | 5 |
4.25 | 2 |
2.25 | 6 |
Based on the original Raman spectrum of these 43 samples, optimize 1927-1957cm
-1wave band and adopt multiple linear regression analysis to set up based on the urea nitrogen isotopic abundance detection model of Raman spectrum.This linear model for the isotopic abundance predicted value of 43 samples and actual value correlationship figure as shown in figure 11.
The cosmic rays null method adopting this patent to propose processes the cosmic rays in urea sample Raman spectrum, removes the Raman spectrum after cosmic rays as shown in figure 12.Optimize 1927-1957cm equally
-1wave band and adopt multiple linear regression analysis to set up based on the urea nitrogen isotopic abundance detection model of Raman spectrum, this linear model for the isotopic abundance predicted value of 43 samples and actual value correlationship as shown in figure 13.
From the prediction effect of these two models, after removing the cosmic rays in Raman spectrum, the accuracy of detection of institute's established model is obviously better than the precision based on original Raman spectrum institute established model, and the coefficient of determination brings up to 0.9389 from original 0.8639.Illustrate that the removing method that cosmic rays of the present invention disturbs effectively can remove cosmic rays, improve the precision that Raman spectrum detects urea isotopic abundance.
Claims (6)
1. the identification that in Raman spectrum, cosmic rays disturbs and a removing method, is characterized in that, comprise the steps:
Step 1, carries out first derivation to original Raman spectrum, obtains having the single order spectrum at concussion peak continuously;
Step 2, judges whether each concussion peak is formed by cosmic rays, behind the concussion peak obtaining the formation of all cosmic rayss, enters step 3 one by one;
Step 3, corrects the concussion peak that cosmic rays is formed in original Raman spectrum, thus eliminates the interference of cosmic rays.
2. the identification of cosmic rays interference in Raman spectrum as claimed in claim 1 and removing method, is characterized in that, in step 2, judge that the concussion peak method that cosmic rays is formed is:
Step 2a, beam location residing for beam location residing for the crest obtaining waiting judging concussion peak and trough, thus obtain the peak width at this concussion peak;
Step 2b, compares this peak width with first threshold, and as being greater than this first threshold, then this concussion peak is Raman signal; As being less than first threshold, then enter next step;
Step 2c, obtain the peak height at concussion peak, by peak height divided by peak width, and compare with Second Threshold, as being less than this Second Threshold, then this concussion peak is Raman signal; As being greater than Second Threshold, then it is concussion peak that cosmic rays is formed.
3. the identification of cosmic rays interference in Raman spectrum as claimed in claim 2 and removing method, it is characterized in that, wherein said first threshold is 4cm
-1.
4. the identification of cosmic rays interference in Raman spectrum as claimed in claim 2 and removing method, it is characterized in that, wherein said Second Threshold is 1000.
5. the identification of cosmic rays interference in Raman spectrum as claimed in claim 1 and removing method, is characterized in that, in step 3, carry out replacement correct concussion peak by the raman scattering intensity value at each wave number place in the wave-number range to cosmic rays place.
6. the identification of cosmic rays interference in Raman spectrum as claimed in claim 5 and removing method, it is characterized in that, the method that within the scope of the concussion peak formed by cosmic rays, the raman scattering intensity value at each wave number place carries out replacing is:
Step 3-1, if identify obtain cosmic rays institute produce concussion peak peak width be d, and shake peak comprise n wave number, so respectively get n-1 wave number as 2 (n-1) individual observed reading at the concussion peak left and right sides that this cosmic rays produces; If the wave number of wherein side, the concussion peak that this cosmic rays produces lacks m, then get m wave number again from opposite side, obtain 2 (n-1) individual wave number equally as observed reading;
Step 3-2, using the wave number of described 2 (n-1) individual observed reading as independent variable, using raman scattering intensity corresponding for described 2 (n-1) individual observed reading as dependent variable, sets up unitary 2 (n-1)-1 equation of n th order n;
Step 3-3, described 2 (n-1) individual observed reading is substituted into respectively unitary 2 (n-1)-1 equation of n th order n that step 3-2 sets up, to solve an equation each term coefficient obtained in described unitary 2 (n-1)-1 equation of n th order n, namely obtain the relational expression between raman scattering intensity and wave number;
Step 3-4, will substitute into each wave number in the wave-number range of cosmic rays place this unitary 2 (n-1)-1 equation of n th order n, is used for the Raman spectrum at each wave number place replaced in cosmic rays place wave-number range.
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CN108181295B (en) * | 2018-01-24 | 2019-09-03 | 华南师范大学 | The identification of cosmic ray Spike and modification method in Raman spectroscopy data |
CN110874548A (en) * | 2018-08-31 | 2020-03-10 | 天津理工大学 | Lung cancer cell and normal cell recognition method based on combination of Raman spectrum and SVM |
CN109001182B (en) * | 2018-09-29 | 2022-01-04 | 西安电子科技大学 | Raman spectrum nondestructive testing method for alcohol content in closed container |
CN111289489B (en) * | 2020-03-05 | 2023-06-02 | 长春长光辰英生物科学仪器有限公司 | Raman spectrum-based microorganism single cell growth detection method |
CN113109318B (en) * | 2021-03-26 | 2022-05-10 | 中国科学院西安光学精密机械研究所 | Raman spectrum quantitative analysis method and system based on spectral peak height direct extraction |
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