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CN112782121B - A multi-angle optical particle counting and refractive index online measurement device and method - Google Patents

A multi-angle optical particle counting and refractive index online measurement device and method Download PDF

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CN112782121B
CN112782121B CN202011561816.3A CN202011561816A CN112782121B CN 112782121 B CN112782121 B CN 112782121B CN 202011561816 A CN202011561816 A CN 202011561816A CN 112782121 B CN112782121 B CN 112782121B
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refractive index
particle
mirror
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CN112782121A (en
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桂华侨
申林
程寅
余同柱
王杰
伍德侠
陈大仁
刘建国
刘文清
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Hefei Institutes of Physical Science of CAS
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    • G01N21/17Systems in which incident light is modified in accordance with the properties of the material investigated
    • G01N21/41Refractivity; Phase-affecting properties, e.g. optical path length
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Abstract

The invention discloses a multi-angle optical particle counting and refractive index online measuring device and method. The device comprises a laser, a collimation light path, a scattering light path, a photoelectric detector and a signal processing circuit. The collimating light path includes an aspherical mirror and a cylindrical mirror. The scattered light path includes a mirror, a dichroic mirror, and a focusing lens. And after being collimated by a collimation system, two or more paths of lasers collect forward and backward scattered light through four detectors so as to realize synchronous on-line measurement of particle size and refractive index. The measuring method is simple, manual operation is not needed, the particle size and refractive index of the particles with a wider particle size range can be accurately measured, and a novel method is provided for real-time online measurement of physical and chemical properties of the atmospheric particles.

Description

Multi-angle optical particle counting and refractive index online measuring device and method
Technical Field
The invention relates to the technical field of atmospheric particulate optical detection, in particular to a multi-angle optical particle counting and refractive index online measuring device and method.
Background
Atmospheric particulates are one of the important contaminants affecting the quality of ambient air; is a key point for influencing the earth atmosphere radiation balance and even the global climate; is also one of the main hazard factors affecting human health. Therefore, the development of the atmospheric particulate monitoring technology is particularly important. The particle size distribution of the particulate matter is an important characteristic of the atmospheric particulate matter, and particularly, the measurement of the number concentration is particularly important, and the measurement of the particle concentration spectrum distribution is also the basis for observing the characteristics of the atmospheric particulate matter. In order to measure the concentration spectrum distribution of the particle number, firstly, the particle number concentration needs to be accurately measured, and an optical counting method is mostly adopted. The principle is that a photoelectric detector is utilized to measure scattered light signals generated by particles through light beams, the particle size is obtained by inverting the light signals, meanwhile, particles sequentially pass through the light beams in a single particle form through ingenious design of particle nozzles, the pulses of the scattered light signals are counted, and the number concentration of the particles is obtained by inversion. The method has the advantages of accurate measurement, high precision, simple structure and non-contact rapid measurement capability, and gradually becomes one of the mainstream measurement methods of the particle counter.
In the last three decades, the technology of optical particle counters has been rapidly developed and has become mature, towards applications with miniature, higher precision, higher efficiency and higher concentration. Commercial instruments were also successively introduced by TSI, met one, grimm, japan, and the like. Such as the american Met one company, designs a 100LPM high-flow optical particle counter by modifying the air inlet. After the 21 st century, and in particular after 2010, the advent of unmanned aerial vehicles has advanced the development of optical particle counters. By mounting the optical particle counter on an unmanned plane, more accurate distribution information of aerosol in the whole atmosphere can be provided, and with the development of technology, scientific researchers develop various optical particle counters with high performance and complexity design to meet the requirement of atmospheric detection, such as the lower detection limit of 0.14 microns researched by the national ocean and atmospheric management agency earth systems research laboratory in 2016, and the novel optical particle counter for realizing lens-free optical path particle size measurement by the scientific researchers of the university of Orland in 2016. The advent of these technologies has driven the further development and application of optical particle counting. However, in the aspect of online monitoring of the atmospheric particulate matters, the light scattering technology has the following problems and disadvantages: (1) The optical particle counting can realize the measurement of the particle size and the number concentration of the atmospheric particles, but the synchronous measurement of the particle size and the refractive index of the atmospheric particles is difficult to realize; (2) The existing light scattering particle size measurement result is easily influenced by parameters such as the refractive index of particles, the shape of particles and the like, so that the range and the accuracy of particle size measurement are reduced.
Disclosure of Invention
The invention aims to provide a multi-angle optical particle counting and refractive index online measuring device and method based on a light scattering principle, which can solve the defects existing in the prior art and realize real-time and non-contact measurement of particle size and refractive index.
In order to achieve the above purpose, the present invention adopts the following technical scheme: a multi-angle optical particle counting and refractive index online measuring device comprises a laser, a collimation system, a scattering system, a detector, a signal processing circuit and a computer; the laser emitted by the two or more paths of lasers is collimated by the collimating system and then is incident on the particles to obtain four groups of scattered light of 10-30 degrees in the forward direction and 150-170 degrees in the backward direction, and the scattered light is split by the dichroic mirror through the reflecting mirror and then is incident in the four groups of detectors; the four groups of detectors receive the optical signals I 1 、I 2 、I 3 、I 4 Respectively converted into electric signals and input into a signal processing circuit, the signal processing circuit amplifies the signal variation and peaks the signal P 1 、P 2 、P 3 、P 4 Respectively input into computer, the computer makes peak value P 1 、P 2 、P 3 、P 4 Comparing with the data in the pre-calculated database in real time, finding out the quadruple with the closest response value by the least square method,the size of the particles to be measured and the real part and the imaginary part of the refractive index are obtained; the collimation system is provided with two or more paths, including an aspheric mirror, a cylindrical mirror and a diaphragm; the aspheric mirror, the cylindrical mirror and the diaphragm are coaxially arranged;
the scattering system is provided with two or more paths, including a reflecting mirror, a dichroic mirror and a focusing lens; the reflector comprises a forward reflector and a backward reflector;
furthermore, the laser adopts a semiconductor laser to output stable light intensity laser so as to improve the measurement accuracy of the particle size of the atmospheric particulates.
Furthermore, the two paths of lasers respectively adopt blue light and green light lasers, so that the dichroic mirror can split light conveniently.
Furthermore, the aspheric mirror and the cylindrical mirror are made of PMMA.
Further, the forward mirror scatter angle is 10-30 °.
Further, the back mirror scatter angle is 150-170 °.
Further, the dichroic mirror is placed at an angle of 45 degrees, so that wavelength splitting is realized.
Further, the sample particulate should ensure a single pass through the optical path to enable real-time measurement and analysis of the size and refractive index of a single atmospheric particulate.
The invention also provides a method for carrying out optical particle counting and online measurement of the refractive index of the particles, which comprises the following steps:
firstly, randomly generating particles with different particle diameters, real parts of refractive indexes and imaginary parts of refractive indexes by using a Monte Carlo algorithm, calculating four groups of responses of forward scattered light and backward scattered light of different particles under the irradiation of green light and blue light, and combining to obtain a primary particle scattering database;
step two, enabling the standard particles to pass through the laser beams in sequence, collecting forward and backward scattered light of the laser through four groups of detectors, and obtaining a standard particle signal peak value P through a signal processing circuit and a computer 1 、P 2 、P 3 、P 4
Third, calculating the standard particulate matter signal peak value P 1 、P 2 、P 3 、P 4 The relation between the particle scattering database signals and the particle scattering database signals is subjected to third-order linear fitting to obtain a scale factor;
and fourthly, measuring single particle scattered light signals passing through laser spots in the sampling process, comparing four data of the detector with a pre-calculated evaluation table consisting of four columns in real time, and finding out the quadruple with the closest response value by a least square method to obtain the size of the particle to be detected and the real part and the imaginary part of the refractive index.
Compared with the prior art, the invention has the following beneficial effects:
(1) The multi-angle optical particle counting and refractive index measuring device has the characteristics of simple structure, convenience in operation, no need of artificial film sampling and the like, and realizes the synchronous measurement function of the refractive index of the particle size of the atmospheric particles by the characteristic that the scattering signal of the particles is positively correlated with the particle size under the light scattering of small angles and the scattering signal of the particles is positively correlated with the refractive index under the light scattering of large angles. The method plays a good technical support role in the change characteristics and source analysis of the atmospheric fine particles.
(2) The multi-angle optical particle counting and refractive index measuring device optimizes and improves the collimation light path, compresses the laser width at the focus, effectively improves the lower limit of particle size measurement, and reduces the false alarm rate.
(3) According to the multi-angle optical particle counting and refractive index measuring device, a scattering light path is built, so that four groups of detector signals are obtained by one particle, analysis and verification are carried out on the four groups of signals, and the measuring precision of particle size and refractive index is improved.
Drawings
FIG. 1 is a schematic diagram of an on-line measuring apparatus for multi-angle optical particle counting and refractive index in the present invention;
wherein:
1. 532nm green laser, 2, green aspheric mirror, 3, green cylindrical mirror, 4, green diaphragm, 5, green forward mirror, 6, blue backward mirror, 7, green backward mirror, 8, blue forward mirror, 9, blue diaphragm, 10, blue cylindrical mirror, 11, blue aspheric mirror, 12, 450nm blue laser, 13, blue forward detector, 14, blue forward focusing lens, 15, first dichroic mirror, 16, green backward focusing lens, 17, green backward detector, 18, green forward detector, 19, green forward focusing lens, 20, second dichroic mirror, 21, blue backward focusing lens, 22, blue backward detector, 23, signal processing circuit, 24, computer.
Detailed Description
The technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings in the embodiments of the present invention, and it is apparent that the described embodiments are only some embodiments of the present invention, but not all embodiments, and all other embodiments obtained by those skilled in the art without the inventive effort based on the embodiments of the present invention are within the scope of protection of the present invention.
The multi-angle optical particle counting and refractive index online measuring device shown in fig. 1 comprises a green laser 1, a blue laser 12, a collimation system, a scattering system, a photoelectric detector, a signal processing circuit 23 and a computer 24, wherein the green laser 1 and the blue laser 12 can realize more wavelength incidence through a time division multiplexing technology. The laser emitted by the two or more paths of lasers is collimated by the collimation system and then is incident on the particles to obtain two groups of forward (10-30 degrees) and two groups of backward (150-170 degrees) four groups of scattered light, wherein the green light forward scattered light is received by the green light forward detector 18 after passing through the green light forward reflecting mirror 5, the second dichroic mirror 20 and the green light forward focusing lens 19; the green light back-scattered light is received by a green light back detector 17 via a green light back mirror 7, a first dichroic mirror 15 and a green light back focusing lens 16; the blue light forward scattered light is received by the blue light forward detector 13 via the blue light forward reflecting mirror 8, the first dichroic mirror 15 and the blue light forward focusing lens 14; the blue light back-scattered light is received by the blue light back detector 22 via the blue light back-reflecting mirror 6, the second dichroic mirror 20 and the blue light back-focusing lens 21; the four groups of detectors receive the optical signalsNumber I 1 、I 2 、I 3 、I 4 Respectively converted into electric signals and input to the signal processing circuit 23, the signal processing circuit 23 amplifies the signal variation and peaks the signal P 1 、P 2 、P 3 、P 4 Respectively, are input into the computer 24, and the computer 24 outputs the peak value P 1 、P 2 、P 3 、P 4 And (3) comparing the real-time data with a pre-calculated database, and finding out the quadruple with the closest response value by a least square method to obtain the size of the particle to be detected and the real part and the imaginary part of the refractive index.
The collimation system comprises a green light aspheric mirror 2, a blue light aspheric mirror 11, a green light cylindrical mirror 3, a blue light cylindrical mirror 10, a green light diaphragm 4 and a blue light diaphragm 9; the aspheric mirror, the cylindrical mirror and the diaphragm are coaxially arranged, so that the quality of light beams can be guaranteed, the lower limit of particle size measurement is improved, and the false alarm rate is reduced.
The scattering system comprises a green light forward mirror 5, a blue light backward mirror 6, a green light backward mirror 7, a blue light forward mirror 8, a first dichroic mirror 15, a second dichroic mirror 20, a blue light forward detector 13, a green light backward focusing lens 16, a green light forward focusing lens 19, and a blue light backward focusing lens 21.
Further, the green light laser 1 and the blue light laser 12 adopt semiconductor lasers, and output laser with stable light intensity, so as to improve the measurement accuracy of the particle size of the atmospheric particulate matters.
Further, the green laser 1 and the blue laser 12 adopt 532nm and 450nm lasers. The light splitting is convenient, and the lower limit of particle size detection is low.
Furthermore, the green aspherical mirror 2, the green cylindrical mirror 3, the blue cylindrical mirror 10 and the blue aspherical mirror 11 are made of PMMA material so as to achieve the best laser collimation effect.
Further, the scattering angles of the green light forward reflecting mirror 5 and the blue light forward reflecting mirror 8 are 10-30 degrees. According to Mie scattering simulation results, the positive correlation coefficient between the scattering signal and the particle size of the angle is selected to be higher, and particle size measurement is facilitated.
Further, the scattering angles of the blue light retro-reflector 6 and the green light retro-reflector 7 are 150-170 degrees. According to Mie scattering simulation results, the positive correlation coefficient between the scattering signal and the refractive index of the angle is selected to be higher, and the refractive index measurement is facilitated.
Further, the first dichroic mirror 15 and the second dichroic mirror 20 are disposed at an angle of 45 °, which is more advantageous for splitting blue light and green light according to experimental results.
Further, the sample particulate should ensure a single pass through the optical path to enable real-time measurement and analysis of the size and refractive index of a single atmospheric particulate.
The invention also relates to a measuring method of the measuring device, which comprises the following steps of;
firstly, randomly generating particles with different particle diameters (0.1-10 mu m), refractive index real parts (1.1-2.0) and refractive index imaginary parts (0-1) by using a Monte Carlo algorithm, calculating four groups of responses of forward scattered light and backward scattered light of different particles under green light and blue light irradiation, and combining to obtain a primary particle scattering database;
step two, making standard particles (Duke standard particles with the particle diameters of 0.1um, 0.3um, 0.5um, 0.7um, 1.0um, 2.0um, 3.0um, 5.0um and 10 um) pass through laser beams individually and sequentially, collecting forward and backward scattered light of two lasers by four groups of detectors, and obtaining a standard particle signal peak P by a signal processing circuit and a computer 1 、P 2 、P 3 、P 4
Third, calculating the standard particulate matter signal peak value P 1 、P 2 、P 3 、P 4 The relation between the particle scattering database signals and the particle scattering database signals is subjected to third-order linear fitting to obtain a scale factor; wherein, the fitting formula is y=B0+B1 x≡1+B2 x≡2+B3 x≡3, y is standard light intensity, x is standard particle size, B0, B1, B2, B3 are fitting parameters;
and fourthly, measuring single particle scattered light signals passing through laser spots in the sampling process, comparing four data of the detector with a pre-calculated evaluation table consisting of four columns in real time, and finding out the quadruple with the closest response value by a least square method to obtain the size of the particle to be detected and the real part and the imaginary part of the refractive index.
The basic principle of the invention is as follows:
when monochromatic light is incident on the particulate matter in the positive Z-axis direction, the scattered light intensity can be expressed as:
wherein the relative refractive index is m=m p /m 1 =n(1-i·η)(m p Is the refractive index of the particles, m 1 N and eta are real and imaginary parts of complex refractive index respectively, and when the imaginary part exists, the particles have absorption effect on incident light; alpha is a particle size parameter, when the surrounding medium of the particle is vacuum or air, the refractive index of the surrounding medium is 1, the size parameter is alpha=pi D/lambda, lambda is the wavelength of incident light, I 0 For the incident light intensity, gamma is the scattering angle, r is the distance between the scattering center and the detection point, i 1 (α,mγ)、i 2 (α, mγ) are the intensity distribution functions of the scattering photoelectric vector perpendicular to and parallel to the scattering plane, respectively.
i 1 (α,mγ)=S 1 (α,mγ)·S 1 * (α,mγ)
i 2 (α,mγ)=S 2 (α,mγ)·S 2 * (α,mγ)
Wherein S is 1 (α,mγ)、S 2 (alpha, mgamma) is the amplitude function of the scattering, S 1 * (α,mγ)、S 2 * (alpha, mgamma) are S respectively 1 (α,mγ)、S 2 (alpha, mgamma) complex conjugation.
For amplitude of vibrationFunctional expression S 1 (α,mγ)、S 2 (alpha, mgamma) wherein a l 、b l Called Mie scattering coefficient, the expression is as follows:
the above formula is l (x)、ξ l (x) Is a Bessel function, and the calculation formula is as follows:
wherein the method comprises the steps ofBessel function of the first type, which is a half integer order,>as a second kind of Hanker function, ψ' l (x)、ξ′ l (x) Respectively represent psi l (x)、ξ l (x) Deriving the respective variables.
Also for the amplitude function expression S 1 (α,mγ)、S 2 (alpha, mgamma) wherein pi l 、τ l The expression is:
wherein P is l (cosγ)、P l (1) (cos γ) is the first order Legendre function and the first order associative Legendre function, respectively, for cos γ.
The above theory of Mie scattering, and the above analysis shows that the important requirement is to calculate the scattered light intensity function i in order to calculate the scattered light intensity 1 (α,mγ)、i 2 (α, mγ). While the key to solving the intensity function is to solve the Mie scattering coefficient a l 、b l And a scattering angle function pi l 、τ l Wherein a is l 、b l The function is a function of the relative refractive index m of the particles and the particle size parameter α, pi l 、τ l The function is a function of the scattering angle gamma. In summary, the particle scattered light intensity I is strongly related to the particle size D (size parameter α), the refractive index m, and the scattering angle γ. The particle size and refractive index of the particles can be judged according to the scattered light intensity I.
What is not described in detail in the present specification belongs to the prior art known to those skilled in the art.
The foregoing is merely a preferred embodiment of the present invention and it should be noted that modifications and adaptations to those skilled in the art may be made without departing from the principles of the present invention, which are intended to be comprehended within the scope of the present invention.

Claims (6)

1.一种多角度光学粒子计数和折射率在线测量装置,其特征在于:包括激光器、准直系统、散射系统、探测器、信号处理电路和计算机;两路或多路激光器出射的激光经准直系统准直后入射到颗粒物上,共得到两组前向10—30°、两组后向150—170°共四组散射光,并通过反射镜后经二向色镜分光入射在四组探测器内;四组探测器将接收到的光信号I1、I2、I3、I4分别转化为电信号并输入到信号处理电路,由信号处理电路将信号变化量放大并将信号峰值P1、P2、P3、P4分别输入计算机,计算机将峰值P1、P2、P3、P4与预先计算的数据库中的数据进行实时比较,通过最小二乘法找到响应值最接近的四元组,便得到了待测粒子的大小、折射率实部虚部;1. A multi-angle optical particle counting and refractive index online measurement device, characterized in that: it includes a laser, a collimation system, a scattering system, a detector, a signal processing circuit, and a computer; lasers emitted from two or more lasers are collimated by the collimation system and then incident on the particles, resulting in four sets of scattered light: two sets forward (10-30°) and two sets backward (150-170°), which are then dispersed by a dichroic mirror and incident on the four detectors; the four detectors convert the received optical signals I1 , I2 , I3 , and I4 into electrical signals and input them to the signal processing circuit, which amplifies the signal changes and inputs the signal peaks P1 , P2 , P3 , and P4 into the computer, which compares the peaks P1 , P2 , P3 , and P4 with data in a pre-calculated database in real time, and finds the quadruplet with the closest response value using the least squares method, thus obtaining the size and real and imaginary parts of the refractive index of the particle to be measured; 所述准直系统设置有两路或多路,包括非球面镜、柱面镜和光阑;所述非球面镜、柱面镜、和光阑同轴设置;The collimation system is provided with two or more channels, including an aspherical lens, a cylindrical lens, and an aperture stop; the aspherical lens, the cylindrical lens, and the aperture stop are arranged coaxially. 所述散射系统设置有两路或多路,包括反射镜、二向色镜和聚焦透镜;所述反射镜包括前向反射镜和后向反射镜;The scattering system is provided with two or more paths, including a reflector, a dichroic mirror, and a focusing lens; the reflector includes a forward reflector and a backward reflector; 所述两路激光器分别采用蓝光、绿光激光器,便于二向色镜分光;The two lasers are blue and green lasers, respectively, which facilitates beam splitting by the dichroic mirror. 所述前向反射镜散射角度为10—30°;The scattering angle of the forward reflecting mirror is 10-30°; 所述后向反射镜散射角度为150—170°。The scattering angle of the rearward reflecting mirror is 150-170°. 2.根据权利要求1所述的一种多角度光学粒子计数和折射率在线测量装置,其特征在于:所述激光器采用半导体激光器,输出稳定光强激光,以提高大气颗粒物的粒径测量精度。2. The multi-angle optical particle counting and refractive index online measurement device according to claim 1, characterized in that: the laser is a semiconductor laser that outputs a stable intensity laser to improve the particle size measurement accuracy of atmospheric particulate matter. 3.根据权利要求1所述的一种多角度光学粒子计数和折射率在线测量装置,其特征在于:所述非球面镜、柱面镜采用PMMA材质。3. The multi-angle optical particle counting and refractive index online measurement device according to claim 1, characterized in that: the aspherical mirror and cylindrical mirror are made of PMMA material. 4.根据权利要求1所述的一种多角度光学粒子计数和折射率在线测量装置,其特征在于:所述二向色镜以45°角放置,实现对波长分光。4. The multi-angle optical particle counting and refractive index online measurement device according to claim 1, characterized in that: the dichroic mirror is placed at a 45° angle to achieve wavelength separation. 5.根据权利要求1所述的一种多角度光学粒子计数和折射率在线测量装置,其特征在于:采样颗粒物应确保单个通过光路,以实现单个大气颗粒物粒径大小与折射率的实时测量与分析。5. The multi-angle optical particle counting and refractive index online measurement device according to claim 1, characterized in that: the sampled particles should be ensured to pass through the optical path individually in order to realize the real-time measurement and analysis of the particle size and refractive index of individual atmospheric particles. 6.一种利用权利要求1-5任意一项所述的测量装置进行光学粒子计数与折射率在线测量的方法,其特征在于:包括以下步骤:6. A method for online optical particle counting and refractive index measurement using the measuring device according to any one of claims 1-5, characterized in that it includes the following steps: 第一步,运用蒙特卡洛算法随机产生不同粒径、折射率实部及折射率虚部大小的粒子,计算不同粒子在绿光、蓝光照射下前向、后向散射光共四组响应,组合得到初步粒子散射数据库;The first step is to use the Monte Carlo algorithm to randomly generate particles with different sizes, real parts of refractive index, and imaginary parts of refractive index, and calculate four sets of responses of different particles to forward and backward scattered light under green and blue light illumination, and combine them to obtain a preliminary particle scattering database. 第二步,使标准颗粒物单个依次通过激光束,通过四组探测器收集激光器前向、后向散射光,并通过信号处理电路及计算机得到标准颗粒物信号峰值P1、P2、P3、P4The second step involves passing standard particles one by one through the laser beam, collecting the forward and backward scattered light from the laser using four sets of detectors, and obtaining the standard particle signal peaks P1 , P2 , P3 , and P4 through signal processing circuitry and a computer. 第三步,计算标准颗粒物信号峰值P1、P2、P3、P4与粒子散射数据库信号之间的关系,通过三阶线性拟合得到比例因子;The third step is to calculate the relationship between the peak values P1 , P2 , P3 , and P4 of the standard particulate matter signal and the signal from the particle scattering database, and obtain the scaling factor through third-order linear fitting. 第四步,测量在采样过程中通过激光光斑的单颗粒物散射光信号,将探测器四个数据与由四列组成的预先计算的评估表进行实时比较,通过最小二乘法找到响应值最接近的四元组,得出待测粒子粒径的大小、折射率实部虚部。The fourth step involves measuring the scattered light signal of a single particle passing through the laser spot during the sampling process. The four data points from the detector are compared in real time with a pre-calculated evaluation table consisting of four columns. The least squares method is used to find the quadruple with the closest response value, and the particle size, real part, and imaginary part of the refractive index of the particle to be measured are obtained.
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