CN115963092A - Self-adaptive Rayleigh scattering processing method based on turbidity compensation and scattering width estimation - Google Patents
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Abstract
The invention discloses a self-adaptive Rayleigh scattering processing method based on turbidity compensation and scattering width estimation, which comprises the following steps of: s1, acquiring original fluorescence spectrum data; s2, deducting Raman scattering; s3, carrying out interpolation conversion on the emission wavelength; s4, searching a left boundary and a right boundary of a first-order Rayleigh scattering removal area of an emission spectrum corresponding to each excitation wavelength; s5, estimating a left boundary and a right boundary of the second-order Rayleigh scattering by combining the left boundary and the right boundary of the first-order Rayleigh scattering removal area obtained in the S4 and the turbidity value of the sample; s6, setting the fluorescence intensity in the first-order Rayleigh scattering removal region boundary obtained in the S4 and the second-order Rayleigh scattering removal region boundary obtained in the S5 to be zero; s7, performing S-G smoothing on the spectrum obtained in the S6; and S8, carrying out interpolation fitting on the deduction area by using a Delaunay triangular interpolation method. The method can effectively reduce the influence of broadening and enhancing the strength of the Rayleigh scattering region, and can better represent the chemical fluorescence signal in the sample.
Description
Technical Field
The invention relates to the technical field of three-dimensional fluorescence water quality detection, in particular to a self-adaptive Rayleigh scattering processing method based on turbidity compensation and scattering width estimation.
Background
The organic matter pollution prevention and control of the urban river water body is one of key contents of water pollution monitoring and treatment work, organic pollutants are monitored, early warning is timely carried out on the river water body, different polluted organic matters are identified, and the method has important significance for early warning, tracing, subsequent treatment and the like of water body pollution. The traditional conventional water quality parameter monitoring method is difficult to generate obvious reaction on low-concentration organic pollutants; compared with the prior art, the three-dimensional fluorescence spectrometry has higher detection sensitivity.
However, in the process of applying the three-dimensional fluorescence spectroscopy, because the rayleigh scattering effect of the incident light is caused by the tiny particles existing in the river water, the obtained original three-dimensional fluorescence data contains the interference of the rayleigh scattering, which is not beneficial to the later detection work. The existing method for deducting Rayleigh scattering by using the specified wavelength width has a plurality of problems, particularly when the turbidity of a sample to be detected is large, the area of an area affected by Rayleigh scattering is large, and the specified wavelength width is difficult to adapt to Rayleigh scattering peaks with different widths corresponding to different excitation wavelengths, so that organic matter fluorescence signals of a scattering edge are greatly affected by residual scattering light, the representation of actual fluorescence signals is affected, and the precision of later detection work is adversely affected.
Therefore, aiming at the problems of different rayleigh scattering widths and the like under different water qualities and turbidities, the research on a rayleigh scattering removal method with adaptive wavelength width is urgently needed.
Disclosure of Invention
The invention aims to overcome the defects of the existing Rayleigh scattering removal method and provide a self-adaptive Rayleigh scattering processing method based on turbidity compensation and scattering width estimation.
In order to achieve the purpose, the invention is realized by the following technical scheme:
an adaptive Rayleigh scattering processing method based on turbidity compensation and scattering width estimation comprises the following steps:
s1, acquiring original fluorescence spectrum data;
s2, deducting the Raman scattering by using a background deduction method;
s3, carrying out interpolation conversion on the emission wavelength;
s4, searching a left boundary and a right boundary of a first-order Rayleigh scattering removal area of the emission spectrum corresponding to each excitation wavelength;
s5, estimating a left boundary and a right boundary of the second-order Rayleigh scattering by combining the left boundary and the right boundary of the first-order Rayleigh scattering removal area obtained in the S4 and the turbidity value of the sample;
s6, setting the fluorescence intensity in the boundary of the first-order Rayleigh scattering removal area obtained in the S4 and the boundary of the second-order Rayleigh scattering removal area obtained in the S5 to be zero;
s7, performing S-G smoothing on the spectrum obtained in the S6;
s8, carrying out interpolation fitting on the deduction area by using a Delaunay triangle interpolation method to obtain a final pretreatment result about the three-dimensional fluorescence spectrum.
S4, the method comprises the following steps:
s4.1, setting an upper threshold and a lower threshold of a right boundary;
s4.2, starting from the central axis of the spectrum, searching a minimum value point of the emission spectrum corresponding to each excitation wavelength, and taking the minimum value point as the right boundary of the scattering area;
s4.3, regarding the condition that the right boundary is not found in the upper threshold, taking the upper threshold as the right boundary;
s4.4, for the condition that the right boundary is smaller than the lower threshold, taking the lower threshold as the lower boundary;
s4.5, the left boundary does not influence the preprocessing result, and is uniformly taken as a larger value, and finally left and right boundary vectors of first-order Rayleigh scattering are obtained.
The S5 comprises the following steps:
s5.1, mapping the right boundary of the first-order Rayleigh scattering to the second-order situation according to the principle that the widths of the first-order scattering area and the second-order scattering area under the same excitation wavelength are not changed;
s5.2, carrying out weighted summation on the mapping result of the first-order Rayleigh scattering right boundary and the turbidity of the sample to obtain a right boundary under the second-order condition;
s5.3 the second-order Rayleigh scattering left boundary and right boundary take the same value.
The method of the second order rayleigh scattering right boundary in step S5.1 is calculated by the following formula:
whereinAnd &>The left and right widths of the second order rayleigh scattering respectively,Tbis the turbidity of the sample and is,ω 1 andω 2 is a reference weight to the first order estimate width and turbidity.
In the step S8, delaunay triangulation is used to describe the triangular meshes of the spectral plane data points, and for missing values, a triangle including an interpolation point is found, and then natural neighboring point interpolation is performed on the triangle, and the reconstructed three-dimensional fluorescence spectrum is the final result of the original spectrum after preprocessing.
Compared with the prior art, the method has the following beneficial effects:
(1) After a compromised fixed wavelength range is set in the conventional method, in the pretreatment of a three-dimensional fluorescence spectrum of a high-turbidity sample, due to the increase of scattering width, a Rayleigh scattering signal is difficult to effectively remove; the method can adaptively adjust the de-scattering range based on the turbidity information and the distribution of Rayleigh scattering peaks, so that first-order and second-order Rayleigh scattering signals can be effectively removed.
(2) After a compromised fixed wavelength range is set in the conventional method, in the pretreatment of the three-dimensional fluorescence spectrum of the low-turbidity sample with the chemical fluorescence signal near the axis, the useful fluorescence signal corresponding to the normal chemical substances in the river water is easy to lose; the method can adaptively adjust the de-scattering range based on the turbidity information and the distribution of Rayleigh scattering peaks, so that more useful chemiluminescence signals are reserved while the Rayleigh scattering signals are effectively removed.
Drawings
FIG. 1 is a flow chart of a three-dimensional fluorescence spectrum preprocessing method based on adaptive Rayleigh scattering removal according to the present invention.
Fig. 2 is a schematic view of rayleigh scattering width and boundaries.
The left image of fig. 3 is a diagram of the effect of the three-dimensional fluorescence spectrum of the high turbidity sample after being subjected to the de-scattering by the adaptive wavelength width method, and the right image is a diagram of the effect after being subjected to the de-scattering and interpolation.
The left image of fig. 4 is a diagram of the effect of the three-dimensional fluorescence spectrum of the low turbidity sample after being subjected to the de-scattering by the adaptive wavelength width method, and the right image is a diagram of the effect after the de-scattering and interpolation.
FIG. 5 is a graph comparing the effect of fixed width subtraction and adaptive subtraction on the high turbidity samples.
FIG. 6 is a graph comparing the effect of fixed width subtraction and adaptive subtraction on the low turbidity samples.
Figure 7 is a graph of the difference of the PARAFAC residual squared sum comparison.
Fig. 8 is a comparative display of emission spectra of different rayleigh scattering removal methods.
FIG. 9 is a comparison of the results of different pretreatment PARAFAC analyses.
Detailed Description
The invention is further illustrated by the following figures and examples.
As shown in fig. 1, an adaptive rayleigh scattering processing method based on turbidity compensation and scattering width estimation includes the following steps:
s1, acquiring original fluorescence spectrum data;
s2, removing Raman scattering by using a background subtraction method;
s3, carrying out interpolation conversion on the emission wavelength;
s4, searching the left boundary and the right boundary of a first-order Rayleigh scattering removal area of the emission spectrum corresponding to each excitation wavelength, and the method comprises the following steps:
s4.1, setting an upper threshold and a lower threshold of a right boundary;
s4.2, starting from the central axis of the spectrum, searching a minimum value point of the emission spectrum corresponding to each excitation wavelength, and taking the minimum value point as the right boundary of the scattering area;
s4.3, regarding the condition that the right boundary is not found in the upper threshold, taking the upper threshold as the right boundary;
s4.4, for the condition that the right boundary is smaller than the lower threshold, taking the lower threshold as the lower boundary;
s4.5, the left boundary does not influence the preprocessing result, and is uniformly taken as a larger value, and finally left and right boundary vectors of first-order Rayleigh scattering are obtained.
S5, estimating the left boundary and the right boundary of the second-order Rayleigh scattering by combining the left boundary and the right boundary of the first-order Rayleigh scattering removal area obtained in the S4 and the turbidity value of the sample, and comprising the following steps of:
s5.1, mapping the right boundary of the first-order Rayleigh scattering to the second-order situation according to the principle that the widths of the first-order scattering area and the second-order scattering area under the same excitation wavelength are not changed;
s5.2, carrying out weighted summation on the mapping result of the first-order Rayleigh scattering right boundary and the turbidity of the sample to obtain a right boundary under the second-order condition;
s5.3 the second-order Rayleigh scattering left boundary and right boundary take the same value.
S6, setting the fluorescence intensity in the boundary of the scattering area obtained in S4 and S5 to be zero;
s7, performing S-G smoothing on the spectrum obtained in the S6;
s8, carrying out interpolation fitting on the deduction area by using a Delaunay triangle interpolation method to obtain a final preprocessing result about the three-dimensional fluorescence spectrum.
In the step S4, specifically, the upper threshold wr of the right boundary is first set max =40nm and lower threshold value wr min And =10nm, and then starting from the central axis of the spectrum, searching a minimum value point of the emission spectrum corresponding to each excitation wavelength as the right boundary of the scattering region. If the search area exceeds wr max Then, no minimum value point is found, which indicates that no chemifluorescence signal exists near the first-order Rayleigh scattering region corresponding to the excitation wavelength, and the right boundary is set as wr max (ii) a If the searched wr is less than wr min The value of wr is discarded and wr = wr is taken min . Thereby obtaining the emission width vector of the first-order Rayleigh scattering region corresponding to each excitation wavelength in the three-dimensional fluorescence spectrum
Where I is the number of excitation wavelengths. Wherein wr can be calculated according to the above steps, and the left boundary wl can be not considered, and is directly unified to be larger value 50nm, or can be doubled wr.
In the step S5, the left and right boundary values of the second-order rayleigh scattering region are obtained by combining the estimated width of the first-order rayleigh scattering and the turbidity of the sample, and the specific calculation formula is as follows:
whereinAnd &>The left and right widths of the second order rayleigh scattering respectively,Tbis the turbidity of the sample and is,ω 1 andω 2 is a reference weight for the first order estimate width and turbidity.
In the step S8, delaunay triangulation is used to describe the triangular meshes of the spectral plane data points, and for missing values, a triangle including an interpolation point is found, and then natural neighboring point interpolation is performed on the triangle, and the reconstructed three-dimensional fluorescence spectrum is the final result of the original spectrum after preprocessing.
Examples
And (4) carrying out experimental verification by taking riverway water solutions with different turbidities collected at actual monitoring points as experimental samples. The specific experimental procedure is as follows:
(1) And (6) sampling. Sampling Water was taken from polypropylene plastic bottles or glass bottles, whichever the material, the sampling bottles were previously washed by 10% HCl and rinsed with purified water.
(2) And (5) filtering. And removing insoluble particles from the collected river water sample by filtration, filtering by a vacuum pump, and matching with a water system filter membrane and a sand core filter device, wherein the aperture of the water system filter membrane is 0.45 mu m, and the diameter of the water system filter membrane is 55 mm.
(3) And (4) storing. The samples were kept at 4 ℃ in the dark, brought back to the laboratory within two days and analyzed as soon as possible.
(4) And (6) detecting. The fluorescence measuring instrument adopts Aqualog of Horiba company as detection equipment, the setting range of excitation wavelength is 220nm to 800nm, the wavelength interval is 5nm, the setting range of emission wavelength is 243.544nm to 823.84nm, the wavelength interval is about 2.33nm, CCD gain Medium, the integration time is 0.1S, and the sensitivity S/N is 20000. The samples were measured in a quartz detection cuvette with an optical path of 1 cm. The dimension of a single fluorescence spectrum matrix EEM obtained in the measurement is 250 × 117, emission parts are automatically interpolated to 250nm to 800nm through Aqualog instrument detection software, the interval is 2.5nm, namely the size of a single three-dimensional fluorescence spectrum is changed to 221 × 117, and meanwhile, a turbidity meter is used for detecting the turbidity corresponding to each sample.
(5) And (4) performing primary pretreatment. And performing primary pretreatment on the three-dimensional fluorescence spectrum data of all river water samples, namely performing background subtraction to remove Raman scattering and performing interpolation conversion on emission wavelengths to obtain an original data set.
(6) And (4) performing de-scattering. And respectively adopting a fixed wavelength width Rayleigh scattering removal method and an adaptive Rayleigh scattering removal method for the obtained three-dimensional fluorescence spectra of the samples with different turbidities. When a fixed wavelength width Rayleigh scattering removal method is used, the left width and the right width of a first-order Rayleigh scattering area and a second-order Rayleigh scattering area are both larger by 15nm; when the adaptive rayleigh scattering removal method is used, the left and right widths of the first-order and second-order rayleigh scattering regions are adaptively adjusted based on the turbidity information and the distribution of rayleigh scattering peaks. And after the left and right boundaries of the scattering region are obtained, directly setting the fluorescence intensity value in the scattering region to be zero.
(7) And (4) smoothing and interpolation reconstruction. And performing S-G smoothing and Delaunay triangle interpolation reconstruction on the three-dimensional fluorescence spectrum after the Rayleigh scattering is deducted.
Fig. 2 is a schematic diagram of the left and right boundaries of a first-order rayleigh scattering region.
FIG. 3 is a graph showing the effect of three-dimensional fluorescence spectroscopy on the backscattering of a high turbidity sample by an adaptive wavelength width method, wherein the turbidity of the sample is 55NTU; FIG. 4 is a graph of the effect of three-dimensional fluorescence spectroscopy on the backscatter of a low turbidity sample with a turbidity of 7.2NTU using an adaptive wavelength width method. It can be seen from the figure that the method can remove the first-order and second-order Rayleigh scattering at different emission wavelengths more selectively and pertinently, thereby retaining more useful chemical fluorescence signals and removing more useless scattering signals.
Fig. 5 is a comparison diagram of the scattering effect of a high turbidity sample by using a fixed width subtraction method and an adaptive subtraction method, and it can be seen from the comparison effect in fig. 5 that the fixed width subtraction method is difficult to effectively cover the scattering region in a 55NTU high turbidity scene, so that the left side of first-order scattering is caused, and many scattered fluorescence signals are not subtracted, but the adaptive rayleigh scattering removal method based on turbidity compensation of the present invention is used to estimate the scattering widths of different intensities and then subtract them, so as to effectively remove the influence of scattering interference on the normal fluorescent substance signal; fig. 6 is a comparison graph of the fixed width subtraction and the adaptive subtraction for the scattering effect in the low turbidity sample, in a 7.2NTU low turbidity scene, wr and wl are still set to fixed values of 15nm, more normal fluorescence signals of the river water are lost, the width of the method is estimated to have some expansion under a few excitation wavelengths, the whole width is maintained to be wr + wl =10nm +10nm, and more normal fluorescence signals of the river water can be retained on the premise of effectively removing rayleigh scattering, so that in a subsequent fluorescence spectrum interpolation reconstruction link, a signal in a fluorescence interpolation subtraction region with less scattering interference can be obtained according to the remaining signals in the fluorescence interpolation subtraction region, so as to obtain a better preprocessing result.
Fig. 7 shows the residual sum-squares comparison of the parallel factorization of the data sets obtained by the two preprocessing methods, and it can be seen that both correction sets can converge the model, but the final model residual of the fixed-width preprocessing method is much larger than that of the adaptive preprocessing method based on the turbidity compensation. The sum of the squared residuals of the portions that differ in phase is the portion of the residual scattered fluorescence signal that cannot be included in the trilinear model.
FIG. 8 is a graph showing the effect of different Rayleigh scattering removal methods on the emission spectrum at an excitation wavelength of 400nm, followed by delaunay interpolation.
FIG. 9 is a graph comparing the results of different Rayleigh scattering removal methods after Rayleigh scattering subtraction and PARAFAC analysis.
Therefore, the fluorescence spectrum preprocessing method provided by the invention can effectively reduce the influence of broadening and enhancing intensity of a Rayleigh scattering region aiming at the adaptive Rayleigh scattering removing method based on turbidity compensation used for detection in different turbidity water quality environments in a river channel scene, so that the preprocessed fluorescence spectrum can better represent chemical fluorescence signals in a sample in the subsequent processing and analyzing processes, and a technical support is provided for the subsequent analysis of the three-dimensional fluorescence spectrum of the river channel water.
The technical features of the above-mentioned embodiments can be further combined, and for the sake of brevity, all possible combinations of the technical features in the above-mentioned embodiments are not described, however, as long as there is no contradiction between the combinations of the technical features, the scope of the present description should be considered as being described in the present specification.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is specific and detailed, but not to be construed as limiting the scope of the invention. It should be noted that various changes and modifications can be made by those skilled in the art without departing from the spirit of the invention, and these changes and modifications are all within the scope of the invention. Therefore, the protection scope of the present invention should be subject to the appended claims.
Claims (5)
1. An adaptive Rayleigh scattering processing method based on turbidity compensation and scattering width estimation is characterized by comprising the following steps:
s1, acquiring original fluorescence spectrum data;
s2, deducting the Raman scattering by using a background deduction method;
s3, carrying out interpolation conversion on the emission wavelength;
s4, searching a left boundary and a right boundary of a first-order Rayleigh scattering removal area of the emission spectrum corresponding to each excitation wavelength;
s5, estimating a left boundary and a right boundary of second-order Rayleigh scattering by combining the left boundary and the right boundary of the first-order Rayleigh scattering removal area obtained in the S4 and the turbidity value of the sample;
s6, setting the fluorescence intensity in the first-order Rayleigh scattering removal region boundary obtained in the S4 and the second-order Rayleigh scattering removal region boundary obtained in the S5 to be zero;
s7, performing S-G smoothing on the spectrum obtained in the S6;
s8, carrying out interpolation fitting on the deduction area by using a Delaunay triangle interpolation method to obtain a final preprocessing result about the three-dimensional fluorescence spectrum.
2. The method according to claim 1, wherein said S4. Comprises the following steps:
s4.1, setting an upper threshold and a lower threshold of a right boundary;
s4.2, starting from the central axis of the spectrum, searching a minimum value point of the emission spectrum corresponding to each excitation wavelength, and taking the minimum value point as the right boundary of the scattering area;
s4.3, regarding the condition that the right boundary is not found in the upper threshold, taking the upper threshold as the right boundary;
s4.4, for the condition that the right boundary is smaller than the lower threshold, taking the lower threshold as the lower boundary;
s4.5, the left boundary does not influence the preprocessing result, and is uniformly taken as a larger value, and finally left and right boundary vectors of first-order Rayleigh scattering are obtained.
3. The method of claim 1, wherein S5 comprises the steps of:
s5.1, mapping the right boundary of the first-order Rayleigh scattering to the second-order situation according to the principle that the widths of the first-order scattering area and the second-order scattering area under the same excitation wavelength are not changed;
s5.2, carrying out weighted summation on the mapping result of the first-order Rayleigh scattering right boundary and the turbidity of the sample to obtain a right boundary under the second-order condition;
s5.3 the second-order Rayleigh scattering left boundary and right boundary take the same value.
4. The method of claim 1, wherein the second order rayleigh scattering right boundary method in step S5.1 is calculated by:
5. The method according to claim 1, wherein in step S8, the Delaunay triangulation is used to describe a triangular mesh of the data points on the plane of the spectrum, and for the missing values, a triangle containing the interpolated points is found, and then natural neighboring point interpolation is performed on the triangle, and the reconstructed three-dimensional fluorescence spectrum is the final result of the preprocessing of the original spectrum.
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"基于三维荧光光谱的城市河道特征有机污染物检测与识别研究", 万方数据知识服务平台, pages 21 - 47 * |
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CN118484637A (en) * | 2024-07-10 | 2024-08-13 | 安徽中科天立泰技术有限公司 | Directional screening system and method for fluorescent spectrum scattering signals of wide-distribution light source |
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