Structural analysis method, structural analysis apparatus, and structural analysis program

Abstract

This technology enables the identification of the structural characteristics of individual microcrystals within a microcrystalline aggregate without unnecessarily increasing computational costs. [Solution] The structural analysis device (1) acquires a two-dimensional X-ray diffraction image corresponding to each of the multiple oscillation angles obtained by irradiating the microcrystal aggregate (3) with coherent X-rays (2), generates a three-dimensional autocorrelation image of each target microcrystal using multiple two-dimensional partial X-ray diffraction images that include the diffraction spot of the target microcrystal, which are extracted from each of the multiple acquired two-dimensional X-ray diffraction images, and calculates the characteristic quantities of each target microcrystal with respect to each structural feature by referring to the generated three-dimensional autocorrelation image of the target microcrystal.

Description

[Technical Field]

[0001] The present invention relates to a structural analysis method, a structural analysis apparatus, and a structural analysis program for analyzing the structure of microcrystalline aggregates. [Background technology]

[0002] Bragg Coherent X-ray Diffraction Imaging (BCDI) is a known method for analyzing the structure of microcrystals (see Non-Patent Literature 1). In the BCDI method, the process of irradiating a microcrystal with X-rays to obtain a two-dimensional X-ray diffraction pattern and the process of changing the oscillation angle of the microcrystal are repeated alternately, and the three-dimensional structure of the microcrystal is visualized by analyzing the diffraction spots contained in each of the multiple two-dimensional X-ray diffraction patterns obtained.

[0003] Furthermore, powder X-ray diffraction is known as a method for analyzing the structure of microcrystalline aggregates (see Patent Document 1). In powder X-ray diffraction, the powder (microcrystalline aggregate) is irradiated with X-rays, and the average characteristics of the microcrystalline aggregate (e.g., lattice constant and average dislocation density) are identified by analyzing the Debye-Scherrer rings (collections of diffraction spots) contained in the obtained two-dimensional X-ray diffraction pattern. [Prior art documents] [Patent Documents]

[0004] [Patent Document 1] Japanese Patent Publication No. 2019-39893 [Non-patent literature]

[0005] [Non-Patent Document 1] Norihiro Oshime et al, "Lattice strain visualization inside a 400 nm single grain of BaTiO3 in polycrystalline ceramics by Bragg coherent X-ray diffraction imaging", Jpn. J. Appl. Phys. 62 SM1022, 2023 [Overview of the Initiative] [Problems that the invention aims to solve]

[0006] The BCDI method is a technique for analyzing the structure of a single microcrystal, and therefore is insufficient for understanding the properties of a microcrystal aggregate. This is because the structure of the analyzed microcrystal may not be representative of the structures of the microcrystals that make up the aggregate. While it is not impossible to understand the properties of a microcrystal aggregate by applying the BCDI method to each of a sufficient number of microcrystals, this is not practical considering the computational cost.

[0007] Furthermore, since powder X-ray diffraction is a method for analyzing the average characteristics of a microcrystalline aggregate, it cannot identify the structural characteristics of individual microcrystals (for example, the size of individual microcrystals). Therefore, statistical analysis and correlation analysis regarding the structural characteristics of individual microcrystals cannot be performed. Consequently, powder X-ray diffraction does not enable an understanding of the properties of a microcrystalline aggregate through these analyses.

[0008] One aspect of the present invention has been made in view of the above-mentioned problems, and one of its objectives is to realize a structural analysis technique that can identify the structural characteristics of individual microcrystals in a microcrystal aggregate without unnecessarily increasing computational costs. [Means for solving the problem]

[0009] A structural analysis method according to one aspect of the present invention is a structural analysis method characterized by comprising: an acquisition process that alternately repeats a measurement step of irradiating a target region of a microcrystalline aggregate with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystalline structure, thereby obtaining a plurality of two-dimensional X-ray diffraction patterns, each corresponding to each of a plurality of oscillation angles; a generation process that uses the microcrystalline crystals from which the coherent X-rays were diffracted in the measurement step as the target microcrystalline crystals to be analyzed, synthesizes a plurality of two-dimensional partial X-ray diffraction patterns, each containing the diffraction spot of the target microcrystalline crystal, extracted from each of the plurality of two-dimensional X-ray diffraction patterns obtained in the acquisition process, and generates a three-dimensional autocorrelation pattern corresponding to each target microcrystalline crystal by performing a three-dimensional Fourier transform on the obtained three-dimensional partial X-ray diffraction pattern; and a calculation process that calculates the characteristic quantities of each target microcrystalline crystal with respect to at least one type of structural feature by referring to the three-dimensional autocorrelation pattern corresponding to the target microcrystalline crystal generated in the generation process.

[0010] A structural analysis method according to one aspect of the present invention includes: (1) obtaining a single two-dimensional X-ray diffraction pattern by irradiating a target region of a microcrystalline aggregate with coherent X-rays; or (2) an acquisition process that obtains multiple two-dimensional X-ray diffraction patterns, each corresponding to a plurality of oscillation angles, by alternately repeating a measurement step of irradiating the target region with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystalline structure; and, using the microcrystalline crystals included in the target region of analysis from which the coherent X-rays were diffracted in the measurement step as the target microcrystalline crystals, (1) generating a single two-dimensional autocorrelation pattern corresponding to each target microcrystalline crystal by performing a two-dimensional Fourier transform on a single two-dimensional partial X-ray diffraction pattern containing the diffraction spot of the target microcrystalline crystal, which is extracted from the single two-dimensional X-ray diffraction pattern obtained in the acquisition process. Alternatively, the structural analysis method is characterized by comprising: (2) a generation process in which a single or multiple two-dimensional autocorrelation images corresponding to each analyte microcrystal are generated by performing a two-dimensional Fourier transform on each of the single or multiple two-dimensional partial X-ray diffraction images selected from a plurality of two-dimensional partial X-ray diffraction images containing the diffraction spot of the analyte microcrystal, which are extracted from each of the plurality of two-dimensional X-ray diffraction images acquired in the acquisition process; and a calculation process in which, for at least one type of structural feature, the feature quantities of each analyte microcrystal with respect to each structural feature are calculated by (1) referring to the single two-dimensional autocorrelation image corresponding to the analyte microcrystal generated in the generation process, or (2) referring to the single or multiple two-dimensional autocorrelation images selected from the single or multiple two-dimensional autocorrelation images corresponding to the analyte microcrystal generated in the generation process.

[0011] A structural analysis apparatus according to one aspect of the present invention is characterized by comprising at least one processor that performs an acquisition process to obtain a plurality of two-dimensional X-ray diffraction images, each corresponding to each of a plurality of oscillation angles, obtained by alternately repeating a measurement process to obtain a two-dimensional X-ray diffraction image by irradiating an analysis target region of a microcrystalline aggregate with coherent X-rays and an oscillation process to change the oscillation angle of the microcrystalline structure; a generation process to generate a three-dimensional autocorrelation image corresponding to each analysis target microcrystalline, using the microcrystalline crystals from which the coherent X-rays were diffracted in the measurement process as the analysis target microcrystalline, synthesizing a plurality of two-dimensional partial X-ray diffraction images containing the diffraction spot of the analysis target microcrystalline, which are extracted from each of the plurality of two-dimensional X-ray diffraction images obtained in the acquisition process, and performing a three-dimensional Fourier transform on the obtained three-dimensional partial X-ray diffraction image; and a calculation process to calculate the feature quantities of each analysis target microcrystalline related to each structural feature for at least one type of structural feature by referring to the three-dimensional autocorrelation image corresponding to the analysis target microcrystalline generated in the generation process.

[0012] A structural analysis apparatus according to one aspect of the present invention includes: (1) obtaining a single two-dimensional X-ray diffraction pattern by irradiating a target region of a microcrystalline aggregate with coherent X-rays; or (2) an acquisition process that obtains multiple two-dimensional X-ray diffraction patterns, each corresponding to each of multiple oscillation angles, by alternately repeating a measurement step of irradiating the target region with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystalline structure; and, using the microcrystalline crystals included in the target region of analysis from which the coherent X-rays have been diffracted in the measurement step as the target microcrystalline crystals, (1) generating a single two-dimensional autocorrelation pattern corresponding to each target microcrystalline crystal by performing a two-dimensional Fourier transform on a single two-dimensional partial X-ray diffraction pattern containing the diffraction spot of the target microcrystalline crystal, which is extracted from the single two-dimensional X-ray diffraction pattern obtained in the acquisition process; or (2) each target The structural analysis apparatus is characterized by comprising at least one processor that performs a generation process for generating single or multiple two-dimensional autocorrelation images corresponding to a microcrystal by performing a two-dimensional Fourier transform on each of the single or multiple two-dimensional partial X-ray diffraction images selected from a plurality of two-dimensional partial X-ray diffraction images containing the diffraction spot of the microcrystal to be analyzed, which are extracted from each of the plurality of two-dimensional X-ray diffraction images acquired in the acquisition process; and a calculation process for calculating the feature quantities of each microcrystal to be analyzed with respect to at least one type of structural feature by (1) referring to the single two-dimensional autocorrelation image corresponding to the microcrystal to be analyzed generated in the generation process, or (2) referring to the single or multiple two-dimensional autocorrelation images selected from the single or multiple two-dimensional autocorrelation images corresponding to the microcrystal to be analyzed generated in the generation process.

[0013] A structural analysis program according to one aspect of the present invention is a structural analysis program characterized by causing at least one processor to execute the following: an acquisition process that alternately repeats a measurement process to obtain a two-dimensional X-ray diffraction image by irradiating a target region of a microcrystalline aggregate with coherent X-rays and an oscillation process to change the oscillation angle of the microcrystalline structure, thereby obtaining a plurality of two-dimensional X-ray diffraction images, each corresponding to each of a plurality of oscillation angles; a generation process that uses the microcrystalline crystals from which the coherent X-rays were diffracted in the measurement process as the target microcrystalline crystals for analysis, synthesizes a plurality of two-dimensional partial X-ray diffraction images containing the diffraction spot of the target microcrystalline crystal, extracted from each of the plurality of two-dimensional X-ray diffraction images obtained in the acquisition process, and generates a three-dimensional autocorrelation image corresponding to each target microcrystalline crystal by performing a three-dimensional Fourier transform on the obtained three-dimensional partial X-ray diffraction image; and a calculation process that calculates the feature quantities of each target microcrystalline crystal related to each structural feature for at least one type of structural feature by referring to the three-dimensional autocorrelation image corresponding to the target microcrystalline crystal generated in the generation process.

[0014] A structural analysis program according to one aspect of the present invention includes: (1) obtaining a single two-dimensional X-ray diffraction pattern by irradiating a target region of a microcrystalline aggregate with coherent X-rays; or (2) an acquisition process that obtains multiple two-dimensional X-ray diffraction patterns, each corresponding to each of multiple oscillation angles, by alternately repeating a measurement step of irradiating the target region with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystalline structure; and, using the microcrystalline crystals included in the target region of analysis from which the coherent X-rays were diffracted in the measurement step as the target microcrystalline crystals, (1) generating a single two-dimensional autocorrelation pattern corresponding to each target microcrystalline crystal by performing a two-dimensional Fourier transform on a single two-dimensional partial X-ray diffraction pattern containing the diffraction spot of the target microcrystalline crystal, which is extracted from the single two-dimensional X-ray diffraction pattern obtained in the acquisition process; or (2) each analysis The structural analysis program is characterized by having at least one processor execute the following: a generation process that generates a single or multiple two-dimensional autocorrelation images corresponding to a target microcrystal by performing a two-dimensional Fourier transform on each of the single or multiple two-dimensional partial X-ray diffraction images selected from a plurality of two-dimensional partial X-ray diffraction images containing the diffraction spot of the target microcrystal, which are extracted from each of the plurality of two-dimensional X-ray diffraction images acquired in the acquisition process; and a calculation process that calculates the feature quantities of each target microcrystal with respect to at least one type of structural feature by (1) referring to the single two-dimensional autocorrelation image corresponding to the target microcrystal generated in the generation process, or (2) referring to the single or multiple two-dimensional autocorrelation images selected from the single or multiple two-dimensional autocorrelation images corresponding to the target microcrystal generated in the generation process. [Effects of the Invention]

[0015] According to one aspect of the present invention, a structural analysis technique can be realized that makes it possible to identify the structural characteristics of individual microcrystals contained in a microcrystalline aggregate without unnecessarily increasing computational costs. [Brief explanation of the drawing]

[0016] [Figure 1]These are a plan view and a top view showing the configuration of a structural analysis system according to one embodiment of the present invention. [Figure 2] This is a flowchart showing the flow of a structural analysis method related to one embodiment of the present invention. [Figure 3] Figure 2 is a schematic diagram illustrating the overview of the generation process included in the structural analysis method shown. [Figure 4] Figure 2 is a schematic diagram illustrating the overview of the calculation process included in the structural analysis method. [Figure 5] This figure illustrates two-dimensional X-ray diffraction images and two-dimensional autocorrelation images referenced in a structural analysis method according to one embodiment of the present invention. [Figure 6] This figure illustrates a histogram created in a structural analysis method according to one embodiment of the present invention. [Modes for carrying out the invention]

[0017] (Configuration of the structural analysis system) The configuration of the structural analysis system 100 according to one embodiment of the present invention will be described with reference to Figure 1. In Figure 1, (a) is a schematic side view showing the configuration of the structural analysis system 100, and (b) is a schematic top view showing the configuration of the structural analysis system 100.

[0018] The structural analysis system 100 is an apparatus for analyzing the structure of a microcrystalline aggregate 3 using coherent X-rays 2. The structural analysis system 100 comprises a lens 101, an image sensor 102, and a structural analysis device 1. The coherent X-rays 2 are, for example, coherent X-rays generated in a synchrotron radiation facility. The microcrystalline aggregate 3 is, for example, a thin film-like microcrystalline aggregate supported on a substrate not shown (e.g., a SiN substrate). A plate-like microcrystalline aggregate (e.g., ceramics) formed by solidifying (e.g., sintering) a group of microcrystals may also be used as the microcrystalline aggregate 3.

[0019] Lens 101 is configured to focus coherent X-rays 2 so that the beam waist of the coherent X-rays 2 is formed in the analysis target region A of the microcrystal aggregate 3. For example, a focusing mirror can be used as lens 101. The coherent X-rays 2 focused by lens 101 are diffracted by microcrystals in the analysis target region A whose crystal plane orientation satisfies the Bragg condition. In this embodiment, lens 101 is used to limit the area of ​​the microcrystal aggregate 3 irradiated with coherent X-rays 2, but the present invention is not limited thereto. For example, a configuration in which the area of ​​the microcrystal aggregate 3 irradiated with coherent X-rays 2 is limited using a slit may be adopted.

[0020] The image sensor 102 is configured to detect coherent X-rays 2 diffracted by microcrystals in the analysis target region A whose crystal plane orientation satisfies the Bragg condition, and to generate a two-dimensional X-ray diffraction pattern. For example, the image sensor 102 is composed of multiple cells arranged in a matrix, and the two-dimensional X-ray diffraction pattern is composed of multiple pixels arranged in a matrix. Here, there is a one-to-one correspondence between the cells of the image sensor 102 and the pixels of the two-dimensional X-ray diffraction pattern. In this case, the pixel value of each pixel in the two-dimensional X-ray diffraction pattern represents the X-ray intensity detected by the cell of the image sensor 102 corresponding to that pixel. As the image sensor 102, for example, a multi-port CCD (Charge Coupled Device) detector, a flat panel detector, or a photon counting type two-dimensional X-ray detector can be used.

[0021] The structural analysis device 1 is configured to analyze the structure of the microcrystalline aggregate 3, particularly the structure of the analysis target region A, by referring to a two-dimensional X-ray diffraction image generated by the image sensor 102. By repeating the structural analysis while changing the analysis target region A, it is possible to perform structural analysis on all or part of the microcrystalline aggregate 3. As the structural analysis device 1, for example, a general-purpose computer equipped with a processor 11 and memory 12 can be used. In this case, the structural analysis program is stored in the memory 12. The processor 11 executes the instructions contained in the structural analysis program to perform the structural analysis method S1 described later.

[0022] The microcrystalline aggregate 3 is held in a position to swing around a straight line L perpendicular to the optical axis of the lens 101 as its axis of rotation, and the oscillation angle θ of the microcrystalline aggregate 3 can be arbitrarily set using an oscillation mechanism (not shown). When the oscillation angle θ = 0°, the main surface of the microcrystalline aggregate 3 is perpendicular to the optical axis of the lens 101; in other words, the thickness direction of the microcrystalline aggregate 3 is parallel to the optical axis of the lens 101. When the oscillation angle θ = 90°, the main surface of the microcrystalline aggregate 3 is parallel to the optical axis of the lens 101; in other words, the thickness direction of the microcrystalline aggregate 3 is perpendicular to the optical axis of the lens 101. Note that the oscillation of the microcrystalline aggregate 3 only needs to change the angle of incidence of coherent X-rays on the microcrystalline aggregate 3, so the choice of the axis of rotation is arbitrary.

[0023] In the structural analysis system 100, a measurement process is performed in which coherent X-rays 2 are irradiated onto the microcrystalline aggregate 3 to obtain a two-dimensional X-ray diffraction pattern, and an oscillation process is performed in which the oscillation angle θ of the microcrystalline aggregate 3 is changed, and these processes are repeated alternately. As a result, each of the m oscillation angles θ1, θ2, ..., θ m (θ1<θ2<…<θ m m 2D X-ray diffraction images corresponding to each of ) I1, I2, ..., I m The following is generated (where m is any natural number greater than or equal to 2). Here, the two-dimensional X-ray diffraction pattern I i The oscillation angle θ i The corresponding two-dimensional X-ray diffraction pattern, i.e., the oscillation angle θ of the microcrystalline aggregate 3 is θ iis a two-dimensional X-ray diffraction image generated by the image sensor 102 when the condition is satisfied (i is each natural number from 1 to m inclusive).

[0024] Hereinafter, among the microcrystals contained in the analysis target region A, the number of microcrystals that diffract coherent X-rays in the measurement step is denoted as n (n is any natural number of 2 or more). Further, among the microcrystals contained in the analysis target region A, the microcrystals that diffract coherent X-rays in the measurement step are referred to as analysis target microcrystals P j (j is each natural number from 1 to n inclusive). Two-dimensional X-ray diffraction images I1, I2, ..., I m include n diffraction spots corresponding to each of the n analysis target microcrystals P1, P2, ..., P n .

[0025] In the powder X-ray structure analysis method, the average characteristics (for example, lattice constant and average dislocation density) of a large number of analysis target microcrystals are specified by analyzing the aggregate of a large number of diffraction spots (Debye-Scherrer ring) contained in the two-dimensional X-ray diffraction image. In addition, in the BCDI (Bragg Coherent X-ray Diffraction Imaging) method, the structure of one analysis target microcrystal is visualized by analyzing one diffraction spot contained in the two-dimensional X-ray diffraction image. In contrast, in the structure analysis method S1 according to the present embodiment, as will be described later, by analyzing each of the n diffraction spots formed on the two-dimensional X-ray diffraction images I1, I2, ..., I m , the structural characteristics (for example, size, anisotropy, shape, and texture structure) of each of the n analysis target microcrystals P1, P2, ..., P n are specified, and then statistical analysis and / or correlation analysis thereof is performed.

[0026] Therefore, in the structure analysis method S1 according to the present embodiment, in order to enhance the significance of the statistical analysis and / or correlation analysis, the analysis target microcrystals P1, P2, ..., P nThe number n is preferably 20 or more, more preferably 50 or more, more preferably 100 or more, more preferably 200 or more, and more preferably 400 or more. In addition, in order to reduce computational costs, the analyte microcrystals P1, P2, ..., P n The number n is 10 4 It is more preferable that the number be 5 × 10 3 It is more preferable that there be 10 or fewer. 3 It is even more preferable that the number be 5 × 10 2 It is even more preferable that the number be less than or equal to 1. By satisfying these conditions, meaningful statistical analysis and / or correlation analysis can be performed without unnecessarily incurring computational costs.

[0027] (Structural analysis method flow) The flow of the structural analysis method S1 performed by the structural analysis device 1 will be explained with reference to Figures 2 to 4. Figure 2 is a flowchart showing the flow of the structural analysis method S1. Figure 3 is a schematic diagram showing an overview of the generation process S12 included in the structural analysis method S1. Figure 4 is a schematic diagram showing an overview of the calculation process S13 included in the structural analysis method S1.

[0028] The structural analysis method S1 includes an acquisition process S11, a generation process S12, a calculation process S13, and an analysis process S14. The acquisition process S11, generation process S12, calculation process S13, and analysis process S14 are processes executed by the processor 11 according to a structural analysis program stored in memory 12.

[0029] The acquisition process S11 involves acquiring m oscillation angles θ1, θ2, ..., θ m m 2D X-ray diffraction images corresponding to each of I1, I2, ..., I m This is the process for obtaining the image. In the acquisition process S11, the processor 11 acquires a two-dimensional X-ray diffraction image Ii corresponding to each oscillation angle θi from the image sensor 102.

[0030] The generation process S12 involves each of the n analyte microcrystals P1, P2, ..., P nn 3D autocorrelation images J'1, J'2, ..., J' corresponding to each of them n This is a process for generating the microcrystals P. In the generation process S12, the processor 11 processes each of the analyte microcrystals P. j The 3D autocorrelation image J' j The m 2D X-ray diffraction images I1, I2, ..., I obtained in acquisition process S11 m It is generated by referring to the following. Specifically, the 3D autocorrelation image J' of each analyte microcrystal Pj. j m 2D X-ray diffraction images I1, I2, ..., I m The microcrystals P, which were cut out from each of these, were the target of analysis. j m 2D partial X-ray diffraction images I containing the diffraction spot 1j ,I 2j ,…,I mj The resulting 3D partial X-ray diffraction pattern I' was synthesized. j This is generated by performing a 3D Fourier transform (see process A1 in Figure 3).

[0031] The calculation process S13 involves o types of structural features Q 1 ,Q 2 ,…,Q o For each of these (where o is any natural number greater than or equal to 1), each has n analyte microcrystals P1, P2, ..., P n n feature quantities Q corresponding to each of them k 1,Q k 2, ..., Q k n This is a process for calculating (k is any natural number between 1 and 0). In calculation process S13, the processor 11 calculates each structural feature Q k Each of the analytes P microcrystals j Feature Q k j The analyte microcrystal P generated in the generation process S12 j 3D autocorrelation image J' j Calculate by referring to the following. For example, each structural feature Q k Each of the analytes P microcrystals j Feature Q k j This is the 3D autocorrelation image J' jCross-sectional image S represents the cross-sectional area where the maximum pixel value is maximized among the two-dimensional cross-sections (a cross-sectional area where the maximum pixel value is not lower than the maximum pixel value of any other two-dimensional cross-section). j The calculation is performed by executing at least one of the following processes B1 to B4 (see Figure 4).

[0032] Processing B1: Cross-sectional image S j In this context, the area representing the figure (the area other than the area representing the ground) is the cross-sectional image S j This is identified by binarization. Then, the size of the analyte microcrystal (first structural feature Q) is determined. 1 ) Microcrystals P that are the target of analysis j Feature Q 1 j The area of ​​the identified region is then calculated. Here, the area of ​​the region representing the figure can be identified, for example, by counting the pixels that make up the region representing the figure. Instead of the area of ​​the identified region, the length of one side of the smallest square that encloses the identified region is considered as the particle size of the analyte microcrystal Pj, and this is used as the analyte microcrystal P j Feature Q 1 j That is also acceptable.

[0033] Processing B2: Cross-sectional image S j In this context, the area representing the figure (the area other than the area representing the ground) is the cross-sectional image S j This is identified by binarization. Then, the anisotropy of the analyte microcrystal (the second structural feature Q) is identified. 2 ) Microcrystals P that are the target of analysis j Feature Q 2 j Then, the aspect ratio = (length of principal axis) / (length of secondary axis) is calculated from the lengths of the principal and secondary axes of the identified region.

[0034] Processing B3: Cross-sectional image S j In this context, the area representing the figure (the area other than the area representing the ground) is the cross-sectional image S j This is identified by binarization. Then, the shape of the analyte microcrystal (the third structural feature Q) is determined. 3 ) Microcrystals P that are the target of analysis j Feature Q3 j as the circularity = 4π × (area) / (perimeter) from the area and perimeter of the identified region 2 is calculated. Here, the perimeter of the region representing a figure can be specified, for example, by counting the pixels constituting the boundary between the region representing the figure and the region representing the background.

[0035] Process B4: For the tissue structure of the analysis target microcrystal (the fourth structural feature Q 4 ), the feature quantity Q of the analysis target microcrystal P j 4 j is calculated as the kurtosis of the pixel value distribution in the cross-sectional image S j . Instead of calculating the kurtosis of the pixel value distribution in the cross-sectional image S j , the kurtosis of the pixel value distribution in the three-dimensional autocorrelation image J' may be calculated. Here, the cross-sectional image S j j or the three-dimensional autocorrelation image J' j the kurtosis of the pixel value distribution in represents the crystallographic distortion of the analysis target microcrystal P j . Note that examples of the feature quantity related to the tissue structure of the analysis target microcrystal that correlates with the kurtosis of the pixel value distribution include, in addition to the crystallographic distortion of the analysis target microcrystal, the defect density of the analysis target microcrystal, the domain structure of the analysis target microcrystal, and the like.

[0036] The analysis process S14 is a process for performing one or both of statistical analysis of one type of structural feature Q k and correlation analysis of two types of structural features Q k , Q k’ . When performing statistical analysis in the analysis process S14, the processor 11 performs statistical analysis on one type of structural feature Q arbitrarily selected from o types of structural features Q 1 , Q 2 , ..., Q o k using the feature quantities Q related to that structural feature Q calculated in the calculation process S13 k k 1, Q k 2, ..., Q k n as references. For example, at least one of the following processes C1 to C2 is executed.​​​​

[0037] Process C1: Structural feature Q k Feature quantity Q related to k 1, Q k 2, ..., Q k n A histogram (frequency distribution) of is created.

[0038] Process C2: Structural feature Q k Feature quantity Q related to k 1, Q k 2, ..., Q k n A statistic of is calculated. For the feature quantity Q k 1, Q k 2, ..., Q k n Examples of the statistic include, for the feature quantity Q k 1, Q k 2, ..., Q k n the mean, median, mode, maximum value, minimum value, variance, standard deviation, skewness, kurtosis, and the like.

[0039] When correlation analysis is performed in the analysis process S14, the processor 11 performs correlation analysis on o types of structural features Q 1 , Q 2 , ..., Q o Correlation analysis of two arbitrarily selected types of structural features Q k , Q k’ is performed with reference to the feature quantities related to one structural feature Q calculated in the calculation process S13 k Feature quantity Q related to k 1, Q k 2, ..., Q k n and the feature quantities related to the other structural feature Q calculated in the calculation process S13 k’ Feature quantity Q related to k’ 1, Q k’ 2, ..., Q k’ n . For example, at least one of the following processes D1 to D2 is executed.

[0040] Process D1: Structural feature Q k Feature quantity Q related to k 1, Q k2, ..., Q k n and structural feature Q k’ Features related to Q k’ 1,Q k’ 2, ..., Q k’ n Create a scatter plot with the data.

[0041] Process D2: Structural Features Q k Features related to Q k 1,Q k 2, ..., Q k n and structural feature Q k’ Features related to Q k’ 1,Q k’ 2, ..., Q k’ n Calculate the correlation coefficient or partial correlation coefficient between the two.

[0042] (Variations of generation and calculation processes) In the generation process S12, each of the n analyte microcrystals P1, P2, ..., P n n 3D autocorrelation images J'1, J'2, ..., J' corresponding to each of them n Although a configuration for generating the above has been described, the present invention is not limited thereto. For example, in the generation process S12, each of the n analyte microcrystals P1, P2, ..., P n n 2D autocorrelation image sets J1, J2, ..., J corresponding to each of the above. n A configuration that generates this may also be adopted.

[0043] In this case, during the generation process S12, the processor 11 processes each of the microcrystals P to be analyzed. j The corresponding 2D autocorrelation image group J j The two-dimensional X-ray diffraction images I1, I2, ..., I obtained in acquisition process S11. m It is generated by referring to the following. Specifically, each analyte microcrystal P j The corresponding 2D autocorrelation image group J j m 2D X-ray diffraction images I1, I2, ..., I m The microcrystals P, which were cut out from each of these, were the target of analysis. j m 2D partial X-ray diffraction images I containing the diffraction spot 1j ,I2j ,…,I mj Each of the m' selected 2D partial X-ray diffraction images (where m' is a natural number between 1 and m) is subjected to a 2D Fourier transform, and the resulting m' 2D autocorrelation images J 1j ,J 2j ,…,J m’j It is generated by collecting (see process A2 in Figure 3: when m'=m). Here, m two-dimensional partial X-ray diffraction images I 1j ,I 2j ,…,I mj One method for selecting m' two-dimensional partial X-ray diffraction images from m two-dimensional partial X-ray diffraction images I 1j ,I 2j ,…,I mj One possible method involves calculating the maximum intensity (the pixel value of the pixel with the highest pixel value) for each of these, and then selecting the single 2D partial X-ray diffraction image with the highest calculated maximum intensity, along with m'-1 other 2D partial X-ray diffraction images with a corresponding oscillation angle θ close to that image.

[0044] In this case, in calculation process S13, the processor 11 processes each structural feature Q k Each of the analytes P microcrystals j Feature Q k j The analyte microcrystal P generated in the generation process S12 j The corresponding 2D autocorrelation image group J j m' 2D autocorrelation images J that make up the array 1j ,J 2j ,…,J m’j It is calculated by referring to m" (where m is a natural number between 1 and m') 2D autocorrelation images selected from the data. Specifically, each structural feature Q k Each of the analytes P microcrystals j Feature Q k j m' 2D autocorrelation images J 1j ,J 2j ,…,J m’j The calculation is performed by applying one of the above processes B1 to B4 to each of the m'' 2D autocorrelation images selected from the above. Here, the m' 2D autocorrelation images J 1j ,J2j ,…,J m’j One way to select m'' 2D autocorrelation images from a set is, for example, to select m' 2D autocorrelation images J 1j ,J 2j ,…,J m’j One method involves calculating the maximum correlation value (the pixel value of the pixel with the highest pixel value) for each of the two-dimensional autocorrelation images, selecting the one 2D autocorrelation image with the largest calculated maximum correlation value, and then selecting m''-1 2D autocorrelation images whose corresponding fluctuation angles are close to that image. If m'' is 2 or greater, the representative values ​​(e.g., mean, median, maximum, or minimum) of the m'' features obtained by applying one of the above processes B1 to B4 to each of the m'' 2D autocorrelation images are used to define the feature Q. k j That's all you need to do.

[0045] In the above explanation, each 2D autocorrelation image group J j The two-dimensional autocorrelation image J that constitutes the structure 1j ,J 2j ,…,J mj The present invention assumes that the number of images m is two or more, but is not limited to this. That is, each two-dimensional autocorrelation image group J j The two-dimensional autocorrelation image J that constitutes the structure 1j ,J 2j ,…,J mj The number of images m may be 1. Each 2D autocorrelation image group J j This is a single 2D autocorrelation image J 1j When composed of, each structural feature Q k Each of the analytes P microcrystals j Feature Q k j This is its two-dimensional autocorrelation image J 1j This can be calculated by applying processes B1 to B4 to the given value. In this case, it is not necessary to change the oscillation angle θ of the microcrystalline aggregate 3.

[0046] (Examples) As microcrystalline aggregate 3, a sample was prepared containing multiple secondary particles (microcrystalline aggregates) formed by the aggregation of primary particles (microcrystals) with an average particle diameter of 100 nm. From the multiple secondary particles contained in this sample, six secondary particles were selected. For each of the six selected secondary particles, a measurement process of irradiating with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation process of changing the oscillation angle θ of the sample were alternately repeated, resulting in 501 two-dimensional X-ray diffraction patterns per secondary particle and a total of 3006 two-dimensional X-ray diffraction patterns. In the oscillation process, the minimum oscillation angle θ1 was set to 0°, and the maximum oscillation angle θ m Let θ be 10°, and the change in the oscillation angle per step is Δθ = θ i’ -θ i’-1 The angle was set to 0.02°. The time required to obtain 3006 two-dimensional X-ray diffraction images was less than 110 minutes.

[0047] Using these 3006 two-dimensional X-ray diffraction images, structural analysis method S1 was performed, targeting 55 primary particles picked from 80 primary particles contained in 6 selected secondary particles. Figure 5 shows (a) an image obtained by integrating 501 two-dimensional X-ray diffraction images obtained by irradiating each of the 6 selected secondary particles with coherent X-rays, and (b) a two-dimensional autocorrelation image obtained by performing a two-dimensional Fourier transform on the two-dimensional partial X-ray diffraction image with the highest maximum intensity among the 501 two-dimensional partial X-ray diffraction images corresponding to each of the 55 picked primary particles. Observing these two-dimensional autocorrelation images reveals the presence of various primary particles with different sizes, aspect ratios, circularity, and structural characteristics.

[0048] In the analysis process S14, for the 55 primary particles to be analyzed, a size-related feature Q is obtained. 1A histogram of particle size was created. The created histogram is shown in Figure 6. According to the histogram in Figure 6, a peak that cannot be explained by a normal distribution centered on an average particle size of 100 nm appears in the region of particle size 150 nm to 160 nm. The discovery of such a peak opens the door to new research that will lead to improvements in material properties and optimization of material manufacturing processes.

[0049] (summary) A structural analysis method according to Embodiment 1 is a structural analysis method characterized by comprising: an acquisition process that alternately repeats a measurement step of irradiating a target region of a microcrystalline aggregate with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystalline structure, thereby obtaining a plurality of two-dimensional X-ray diffraction patterns, each corresponding to each of a plurality of oscillation angles; a generation process that uses the microcrystalline crystals from which the coherent X-rays were diffracted in the measurement step as the target microcrystalline crystals to be analyzed, synthesizes a plurality of two-dimensional partial X-ray diffraction patterns, each containing the diffraction spot of the target microcrystalline crystal, extracted from each of the plurality of two-dimensional X-ray diffraction patterns obtained in the acquisition process, and generates a three-dimensional autocorrelation pattern corresponding to each target microcrystalline crystal by performing a three-dimensional Fourier transform on the obtained three-dimensional partial X-ray diffraction pattern; and a calculation process that calculates the characteristic quantities of each target microcrystalline crystal with respect to each structural feature for at least one type of structural feature by referring to the three-dimensional autocorrelation pattern corresponding to the target microcrystalline crystal generated in the generation process.

[0050] The structural analysis method according to Embodiment 2 is: (1) obtaining a single two-dimensional X-ray diffraction pattern by irradiating a target region of a microcrystal aggregate with coherent X-rays; or (2) an acquisition process that obtains multiple two-dimensional X-ray diffraction patterns, each corresponding to a plurality of oscillation angles, by alternately repeating a measurement step of irradiating the target region of the analysis with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystal structure; and, using the microcrystals from which the coherent X-rays were diffracted in the measurement step as the target microcrystals, (1) generating a single two-dimensional autocorrelation pattern corresponding to each target microcrystal by performing a two-dimensional Fourier transform on a single two-dimensional partial X-ray diffraction pattern containing the diffraction spot of the target microcrystal, which is extracted from the single two-dimensional X-ray diffraction pattern obtained in the acquisition process, or The structural analysis method is characterized by comprising: (2) a generation process in which a single or multiple two-dimensional autocorrelation images corresponding to each microcrystal to be analyzed are generated by performing a two-dimensional Fourier transform on each of the single or multiple two-dimensional partial X-ray diffraction images selected from a plurality of two-dimensional partial X-ray diffraction images containing the diffraction spot of the microcrystal to be analyzed, which are extracted from each of the plurality of two-dimensional X-ray diffraction images acquired in the acquisition process; and a calculation process in which, for at least one type of structural feature, the feature quantities of each microcrystal to be analyzed with respect to each structural feature are calculated by (1) referring to the single two-dimensional autocorrelation image corresponding to the microcrystal to be analyzed generated in the generation process, or (2) referring to the single or multiple two-dimensional autocorrelation images selected from the single or multiple two-dimensional autocorrelation images corresponding to the microcrystal to be analyzed generated in the generation process.

[0051] The structural analysis method according to embodiment 3 is a structural analysis method according to embodiment 1 or 2, characterized in that it further includes an analysis process in which a statistical analysis of one type of structural feature is performed by referring to the feature quantity related to the structural feature calculated in the calculation process, or a correlation analysis of two types of structural features is performed by referring to the feature quantity related to one structural feature calculated in the calculation process and the feature quantity related to the other structural feature calculated in the calculation process.

[0052] The structural analysis method according to embodiment 4 is characterized in that the number of microcrystals to be analyzed is 20 or more. 4 This is a structural analysis method according to embodiment 3, characterized in that the number is less than or equal to 1.

[0053] The structural analysis method according to Embodiment 5 is a structural analysis method according to any one embodiment of Embodiments 1 to 4, characterized in that, in the calculation process, the characteristic quantities of each analyte microcrystal with respect to each structural feature are calculated by referring to a three-dimensional autocorrelation image or a two-dimensional autocorrelation image corresponding to the analyte microcrystal generated in the generation process, for at least one of the following: the size of the analyte microcrystal, which is a first structural feature; the anisotropy of the analyte microcrystal, which is a second structural feature; the shape of the analyte microcrystal, which is a third structural feature; and the microstructure of the analyte microcrystal, which is a fourth structural feature.

[0054] The structural analysis apparatus according to embodiment 6 is characterized by comprising at least one processor that performs an acquisition process to obtain a plurality of two-dimensional X-ray diffraction images, each corresponding to each of a plurality of oscillation angles, obtained by alternately repeating a measurement process to obtain a two-dimensional X-ray diffraction image by irradiating an analysis target region of a microcrystal aggregate with coherent X-rays and an oscillation process to change the oscillation angle of the microcrystal structure; a generation process to generate a three-dimensional autocorrelation image corresponding to each analysis target microcrystal, using the microcrystals from which the coherent X-rays were diffracted in the measurement process as analysis target microcrystals, synthesizing a plurality of two-dimensional partial X-ray diffraction images containing the diffraction spot of the analysis target microcrystal, which are cut out from each of the plurality of two-dimensional X-ray diffraction images obtained in the acquisition process, and performing a three-dimensional Fourier transform on the obtained three-dimensional partial X-ray diffraction image; and a calculation process to calculate the feature quantities of each analysis target microcrystal related to each structural feature for at least one type of structural feature by referring to the three-dimensional autocorrelation image corresponding to the analysis target microcrystal generated in the generation process.

[0055] The structural analysis apparatus according to embodiment 7 includes (1) a single two-dimensional X-ray diffraction pattern obtained by irradiating a target region of a microcrystalline aggregate with coherent X-rays, or (2) an acquisition process which involves alternately repeating a measurement step of irradiating the target region with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystalline structure, each acquiring a plurality of two-dimensional X-ray diffraction patterns corresponding to each of a plurality of oscillation angles, and using the microcrystalline aggregates included in the target region of analysis, from which the coherent X-rays diffracted in the measurement step as the target microcrystalline, (1) generating a single two-dimensional autocorrelation pattern corresponding to each target microcrystalline by performing a two-dimensional Fourier transform on a single two-dimensional partial X-ray diffraction pattern containing the diffraction spot of the target microcrystalline, which is extracted from the single two-dimensional X-ray diffraction pattern obtained in the acquisition process, or (2) each target microcrystalline The structural analysis apparatus is characterized by comprising at least one processor that performs a generation process to generate a single or more two-dimensional autocorrelation images corresponding to a crystal by performing a two-dimensional Fourier transform on each of the single or more two-dimensional partial X-ray diffraction images selected from a plurality of two-dimensional partial X-ray diffraction images containing the diffraction spot of the microcrystal to be analyzed, which are extracted from each of the plurality of two-dimensional X-ray diffraction images acquired in the acquisition process; and a calculation process that calculates the feature quantities of each microcrystal to be analyzed with respect to at least one type of structural feature by (1) referring to the single two-dimensional autocorrelation image corresponding to the microcrystal to be analyzed generated in the generation process, or (2) referring to the single or more two-dimensional autocorrelation images selected from the single or more two-dimensional autocorrelation images corresponding to the microcrystal to be analyzed generated in the generation process.

[0056] The structural analysis program according to embodiment 8 is a structural analysis program characterized by having at least one processor execute the following: an acquisition process that alternately repeats a measurement process to obtain a two-dimensional X-ray diffraction image by irradiating a target region of a microcrystalline aggregate with coherent X-rays and an oscillation process to change the oscillation angle of the microcrystalline structure, thereby obtaining a plurality of two-dimensional X-ray diffraction images, each corresponding to each of a plurality of oscillation angles; a generation process that uses the microcrystalline crystals from which the coherent X-rays were diffracted in the measurement process as the target microcrystalline crystals for analysis, synthesizes a plurality of two-dimensional partial X-ray diffraction images containing the diffraction spot of the target microcrystalline crystal, extracted from each of the plurality of two-dimensional X-ray diffraction images obtained in the acquisition process, and generates a three-dimensional autocorrelation image corresponding to each target microcrystalline crystal by performing a three-dimensional Fourier transform on the obtained three-dimensional partial X-ray diffraction image; and a calculation process that calculates the feature quantities of each target microcrystalline crystal for each structural feature related to at least one type of structural feature by referring to the three-dimensional autocorrelation image corresponding to the target microcrystalline crystal generated in the generation process.

[0057] The structural analysis program according to embodiment 9 includes: (1) obtaining a single two-dimensional X-ray diffraction pattern by irradiating a target region of a microcrystalline aggregate with coherent X-rays; or (2) obtaining a plurality of two-dimensional X-ray diffraction patterns, each corresponding to a plurality of oscillation angles, by alternately repeating a measurement step of irradiating the target region with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystalline structure; and, using the microcrystalline crystals included in the target region of analysis from which the coherent X-rays were diffracted in the measurement step as the target microcrystalline crystals, (1) generating a single two-dimensional autocorrelation pattern corresponding to each target microcrystalline crystal by performing a two-dimensional Fourier transform on a single two-dimensional partial X-ray diffraction pattern containing the diffraction spot of the target microcrystalline crystal, which is extracted from the single two-dimensional X-ray diffraction pattern obtained in the acquisition process; or (2) each target The structural analysis program is characterized by having at least one processor execute the following: a generation process that generates a single or multiple two-dimensional autocorrelation images corresponding to a microcrystal by performing a two-dimensional Fourier transform on each of the single or multiple two-dimensional partial X-ray diffraction images selected from a plurality of two-dimensional partial X-ray diffraction images containing the diffraction spot of the microcrystal to be analyzed, which are extracted from each of the plurality of two-dimensional X-ray diffraction images acquired in the acquisition process; and a calculation process that calculates the feature quantities of each microcrystal to be analyzed with respect to at least one type of structural feature by (1) referring to the single two-dimensional autocorrelation image corresponding to the microcrystal to be analyzed generated in the generation process, or (2) referring to the single or multiple two-dimensional autocorrelation images selected from the single or multiple two-dimensional autocorrelation images corresponding to the microcrystal to be analyzed generated in the generation process.

[0058] (Additional notes) The present invention is not limited to the embodiments described above, and various modifications are possible within the scope of the claims. Embodiments obtained by appropriately combining the technical means disclosed in each of the embodiments described above are also included within the technical scope of the present invention. [Explanation of Symbols]

[0059] 1 Structural analysis device 11 processors 12 memory 100 Structural Analysis Systems 101 Lens 102 Image Sensor S1 Structural analysis method S11 Acquisition process S12 Generation Process S13 Calculation process S14 Analysis Processing

Claims

1. An acquisition process is performed by alternately repeating a measurement step of irradiating a target region of a microcrystalline aggregate with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern, and an oscillation step of changing the oscillation angle of the microcrystalline structure, thereby obtaining multiple two-dimensional X-ray diffraction patterns, each corresponding to one of multiple oscillation angles. A generation process is performed in which, among the microcrystals included in the region to be analyzed, the microcrystals that diffracted the coherent X-rays in the measurement step are used as the target microcrystals for analysis, and a three-dimensional autocorrelation image corresponding to each target microcrystal is generated by synthesizing multiple two-dimensional partial X-ray diffraction images, each containing the diffraction spot of the target microcrystal, which are extracted from each of the multiple two-dimensional X-ray diffraction images acquired in the acquisition process, and then performing a three-dimensional Fourier transform on the resulting three-dimensional partial X-ray diffraction image. The process includes a calculation process in which, for at least one type of structural feature, the characteristic quantity of each analyte microcrystal related to each structural feature is calculated by referring to a three-dimensional autocorrelation image corresponding to the analyte microcrystal generated in the generation process, A structural analysis method characterized by the following features.

2. (1) A single two-dimensional X-ray diffraction pattern obtained by irradiating a target region of a microcrystalline aggregate with coherent X-rays, or (2) An acquisition process to obtain multiple two-dimensional X-ray diffraction patterns, each corresponding to a plurality of oscillation angles, obtained by alternately repeating a measurement step of irradiating the target region of the analyzer with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystalline structure. Of the microcrystals included in the area to be analyzed, the microcrystals whose coherent X-rays were diffracted in the measurement step are to be analyzed. (1) A generation process that generates a single two-dimensional autocorrelation image corresponding to each microcrystal to be analyzed by performing a two-dimensional Fourier transform on a single two-dimensional partial X-ray diffraction image containing the diffraction spot of the microcrystal to be analyzed, which is extracted from a single two-dimensional X-ray diffraction image obtained in the acquisition process, or (2) A generation process that generates a single or multiple two-dimensional autocorrelation images corresponding to each microcrystal to be analyzed by performing a two-dimensional Fourier transform on each of the single or multiple two-dimensional partial X-ray diffraction images selected from each of the multiple two-dimensional X-ray diffraction images obtained in the acquisition process, which contain the diffraction spot of the microcrystal to be analyzed, For at least one type of structural feature, the calculation process includes: (1) calculating the feature quantity of each analyte microcrystal with respect to each structural feature by referring to a single two-dimensional autocorrelation image corresponding to the analyte microcrystal generated in the generation process, or (2) calculating the feature quantity by referring to a single or multiple two-dimensional autocorrelation images selected from the single or multiple two-dimensional autocorrelation images corresponding to the analyte microcrystal generated in the generation process; A structural analysis method characterized by the following features.

3. The analysis process further includes either performing a statistical analysis of one type of structural feature by referring to the feature quantity related to the structural feature calculated in the calculation process, or performing a correlation analysis of two types of structural features by referring to the feature quantity related to one structural feature calculated in the calculation process and the feature quantity related to the other structural feature calculated in the calculation process. The structural analysis method according to claim 1 or 2.

4. The number of microcrystals to be analyzed is 20 or more. ４ It is less than or equal to one. The structural analysis method according to feature 3.

5. In the calculation process described above, the characteristic quantities of each analyte microcrystal relating to each structural characteristic are calculated by referring to the three-dimensional autocorrelation image or two-dimensional autocorrelation image corresponding to the analyte microcrystal generated in the generation process described above, for at least one of the following: the size of the analyte microcrystal, which is the first structural characteristic; the anisotropy of the analyte microcrystal, which is the second structural characteristic; the shape of the analyte microcrystal, which is the third structural characteristic; and the microstructure of the analyte microcrystal, which is the fourth structural characteristic. The structural analysis method according to claim 1 or 2.

6. An acquisition process is performed by alternately repeating a measurement step of irradiating a target region of a microcrystalline aggregate with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern, and an oscillation step of changing the oscillation angle of the microcrystalline structure, thereby obtaining multiple two-dimensional X-ray diffraction patterns, each corresponding to one of multiple oscillation angles. A generation process is performed in which, among the microcrystals included in the region to be analyzed, the microcrystals that diffracted the coherent X-rays in the measurement step are used as the target microcrystals for analysis, and a three-dimensional autocorrelation image corresponding to each target microcrystal is generated by synthesizing multiple two-dimensional partial X-ray diffraction images, each containing the diffraction spot of the target microcrystal, which are extracted from each of the multiple two-dimensional X-ray diffraction images acquired in the acquisition process, and then performing a three-dimensional Fourier transform on the resulting three-dimensional partial X-ray diffraction image. The system includes at least one processor that performs a calculation process to calculate the characteristic quantities of each microcrystal to be analyzed for each structural feature, with respect to at least one type of structural feature, by referring to a three-dimensional autocorrelation image corresponding to the microcrystal to be analyzed generated in the generation process. A structural analysis device characterized by the following features.

7. (1) A single two-dimensional X-ray diffraction pattern obtained by irradiating a target region of a microcrystalline aggregate with coherent X-rays, or (2) An acquisition process to obtain multiple two-dimensional X-ray diffraction patterns, each corresponding to a plurality of oscillation angles, obtained by alternately repeating a measurement step of irradiating the target region of the analyzer with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystalline structure. Of the microcrystals included in the area to be analyzed, the microcrystals whose coherent X-rays were diffracted in the measurement step are to be analyzed. (1) A generation process that generates a single two-dimensional autocorrelation image corresponding to each microcrystal to be analyzed by performing a two-dimensional Fourier transform on a single two-dimensional partial X-ray diffraction image containing the diffraction spot of the microcrystal to be analyzed, which is extracted from a single two-dimensional X-ray diffraction image obtained in the acquisition process, or (2) A generation process that generates a single or multiple two-dimensional autocorrelation images corresponding to each microcrystal to be analyzed by performing a two-dimensional Fourier transform on each of the single or multiple two-dimensional partial X-ray diffraction images selected from each of the multiple two-dimensional X-ray diffraction images obtained in the acquisition process, which contain the diffraction spot of the microcrystal to be analyzed, The system includes at least one processor that performs a calculation process for each structural feature of a target microcrystal, which involves (1) calculating the feature quantity of each target microcrystal with respect to each structural feature by referring to a single two-dimensional autocorrelation image corresponding to the target microcrystal generated in the generation process, or (2) calculating the feature quantity of each target microcrystal with respect to each structural feature by referring to a single or more two-dimensional autocorrelation images selected from the single or more two-dimensional autocorrelation images corresponding to the target microcrystal generated in the generation process. A structural analysis device characterized by the following features.

8. An acquisition process is performed by alternately repeating a measurement step of irradiating a target region of a microcrystalline aggregate with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern, and an oscillation step of changing the oscillation angle of the microcrystalline structure, thereby obtaining multiple two-dimensional X-ray diffraction patterns, each corresponding to one of multiple oscillation angles. A generation process is performed in which, among the microcrystals included in the region to be analyzed, the microcrystals that diffracted the coherent X-rays in the measurement step are used as the target microcrystals for analysis, and a three-dimensional autocorrelation image corresponding to each target microcrystal is generated by synthesizing multiple two-dimensional partial X-ray diffraction images, each containing the diffraction spot of the target microcrystal, which are extracted from each of the multiple two-dimensional X-ray diffraction images acquired in the acquisition process, and then performing a three-dimensional Fourier transform on the resulting three-dimensional partial X-ray diffraction image. The method involves having at least one processor perform a calculation process that calculates the characteristic quantities of each microcrystal under analysis for each structural feature by referring to the three-dimensional autocorrelation image corresponding to the microcrystal under analysis generated in the generation process, for at least one type of structural feature. A structural analysis program characterized by the following features.

9. (1) A single two-dimensional X-ray diffraction pattern obtained by irradiating a target region of a microcrystalline aggregate with coherent X-rays, or (2) An acquisition process to obtain multiple two-dimensional X-ray diffraction patterns, each corresponding to a plurality of oscillation angles, obtained by alternately repeating a measurement step of irradiating the target region of the analyzer with coherent X-rays to obtain a two-dimensional X-ray diffraction pattern and an oscillation step of changing the oscillation angle of the microcrystalline structure. Of the microcrystals included in the area to be analyzed, the microcrystals whose coherent X-rays were diffracted in the measurement step are to be analyzed. (1) A generation process that generates a single two-dimensional autocorrelation image corresponding to each microcrystal to be analyzed by performing a two-dimensional Fourier transform on a single two-dimensional partial X-ray diffraction image containing the diffraction spot of the microcrystal to be analyzed, which is extracted from a single two-dimensional X-ray diffraction image obtained in the acquisition process, or (2) A generation process that generates a single or multiple two-dimensional autocorrelation images corresponding to each microcrystal to be analyzed by performing a two-dimensional Fourier transform on each of the single or multiple two-dimensional partial X-ray diffraction images selected from each of the multiple two-dimensional X-ray diffraction images obtained in the acquisition process, which contain the diffraction spot of the microcrystal to be analyzed, For at least one type of structural feature, the feature quantities of each analyte microcrystal related to each structural feature are calculated by (1) referring to a single two-dimensional autocorrelation image corresponding to the analyte microcrystal generated in the generation process, or (2) referring to a single or more two-dimensional autocorrelation images selected from the single or more two-dimensional autocorrelation images corresponding to the analyte microcrystal generated in the generation process, and the calculation process is performed by at least one processor. A structural analysis program characterized by the following features.

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