WO2022131336A1 - 測定条件探索方法、コンピュータプログラム、測定条件探索装置、及び測定システム - Google Patents

測定条件探索方法、コンピュータプログラム、測定条件探索装置、及び測定システム Download PDF

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Publication number
WO2022131336A1
WO2022131336A1 PCT/JP2021/046543 JP2021046543W WO2022131336A1 WO 2022131336 A1 WO2022131336 A1 WO 2022131336A1 JP 2021046543 W JP2021046543 W JP 2021046543W WO 2022131336 A1 WO2022131336 A1 WO 2022131336A1
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Prior art keywords
measurement
preliminary
sample
conditions
past
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English (en)
French (fr)
Japanese (ja)
Inventor
優穂 佐藤
嘉健 安藤
哲也 森
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Horiba Ltd
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Horiba Ltd
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    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/62—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
    • G01N21/63—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light optically excited
    • G01N21/64—Fluorescence; Phosphorescence
    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/62—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
    • G01N21/63—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light optically excited
    • G01N21/65—Raman scattering
    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N23/00—Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00
    • G01N23/22—Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00 by measuring secondary emission from the material
    • G01N23/223—Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00 by measuring secondary emission from the material by irradiating the sample with X-rays or gamma-rays and by measuring X-ray fluorescence

Definitions

  • the present invention relates to a measurement condition search method, a computer program, a measurement condition search device, and a measurement system for searching measurement conditions when performing a specific measurement on a sample.
  • the physical quantity of the sample is measured, and the sample is analyzed based on the measurement result. For example, light or radiation emitted from a sample such as fluorescent X-ray, Raman scattered light, fluorescence or cathode luminescence is measured, a spectrum is acquired, and the sample is analyzed such as composition analysis based on the measurement result including the spectrum. Be radiated. In addition, analysis targeting biological samples is also being performed.
  • Patent Document 1 discloses a technique for analyzing a biological sample based on a measurement result of Raman scattered light.
  • the measurement conditions In order to properly analyze the sample, it is necessary to properly adjust the measurement conditions when performing the measurement. For example, when measuring Raman scattered light, it is necessary to appropriately adjust the measurement conditions such as the intensity of the laser light irradiating the sample, the irradiation time, or the number of times the intensity of the Raman scattered light is integrated. If the measurement conditions are not appropriate, inappropriate measurement results such as measurement results with a small S / N (signal / noise) ratio will be obtained, and the accuracy of analysis will decrease. Therefore, it is necessary to search for appropriate measurement conditions by performing preliminary measurement before performing analysis. Usually, by repeating the preliminary measurement while changing the measurement conditions, an appropriate measurement condition that enables analysis with sufficient accuracy is searched for. However, the efficiency of searching for appropriate measurement conditions varies depending on the proficiency level of the user who uses the measuring device. It takes time for users to become highly proficient, and the number of highly proficient users is small. Therefore, efficient sample analysis is difficult.
  • the present invention has been made in view of such circumstances, and an object thereof is a measurement condition search method, a computer program, and a measurement condition search device that enable easy search for appropriate measurement conditions. , And to provide a measurement system.
  • the measurement condition search method is a method for searching for measurement conditions when performing a specific measurement on a sample, in which sample information representing the contents of a sample for which the specific measurement has been performed in the past and past measurement conditions From the database recorded in association with, the past measurement conditions associated with the sample information representing the contents similar to the contents of the sample to be measured are extracted, and the measurement for preliminary measurement is performed based on the extracted past measurement conditions. Determine the conditions, perform the preliminary measurement according to the determined measurement conditions for the preliminary measurement, evaluate the result of the preliminary measurement, and update the measurement conditions for the preliminary measurement according to the result of the evaluation and the result of the preliminary measurement. Is performed, and the preliminary measurement is executed, the evaluation and the update are repeated.
  • the measurement conditions for the preliminary measurement are determined based on the past measurement conditions recorded in the database, the preliminary measurement is executed, and the result of the preliminary measurement is obtained.
  • the measurement conditions are searched by repeating the evaluation and the update of the measurement conditions for the preliminary measurement. Finally, the measurement conditions for which the evaluation of the preliminary measurement result is good are obtained, and the appropriate measurement conditions for the main measurement are obtained.
  • the measurement condition search method performs the evaluation by determining whether or not the evaluation target included in the preliminary measurement result satisfies the predetermined criteria, and the evaluation target satisfies the predetermined criteria. If not, the update is performed, and when the evaluation target satisfies the predetermined criteria, the measurement condition for the preliminary measurement is determined as the measurement condition for the main measurement.
  • the measurement conditions for the preliminary measurement are updated and the evaluation target meets the predetermined criteria.
  • Predetermined criteria are predetermined so that the sample can be analyzed with sufficient accuracy, and appropriate measurement conditions are searched for.
  • the present measurement is performed according to the determined measurement conditions for the present measurement, and the sample information indicating the content of the sample to be measured, the measurement conditions for the present measurement, and the result of the present measurement are used. Is associated with and recorded in the database.
  • the main measurement is performed according to the obtained measurement conditions for the main measurement, and the measurement conditions for the main measurement and the result of the main measurement are recorded in the database.
  • the measurement conditions and measurement results are accumulated in the database referred to when determining the measurement conditions for preliminary measurement, and it is easier to obtain more appropriate measurement conditions when determining the measurement conditions for preliminary measurement by referring to the database. Become.
  • the specific measurement is to irradiate a sample with light or radiation and acquire a spectrum of light or radiation generated from the sample, and the measurement condition is to irradiate the sample.
  • the evaluation target is the signal intensity contained in the acquired spectrum, the S / N ratio of the spectrum, or the peak contained in the spectrum. It is characterized by including the resolution of.
  • the specific measurement is a measurement for acquiring a spectrum of light or radiation generated from a sample, such as a measurement of Raman scattered light.
  • the measurement conditions include the intensity of light or radiation irradiating the sample, or the time of irradiating the sample with light or radiation. These conditions are related to the accuracy of sample analysis.
  • the evaluation target includes the signal intensity contained in the spectrum, the signal-to-noise ratio, or the resolution of the peak contained in the spectrum.
  • the database records past measurement results in association with past measurement conditions, and measures are taken from the extracted past measurement conditions according to the past measurement results. It is characterized in that a condition is selected and the selected measurement condition is determined as a measurement condition for preliminary measurement.
  • the measurement conditions for preliminary measurement are selected from the extracted past measurement conditions according to the measurement results associated with the past measurement conditions extracted from the database.
  • the measurement conditions when good measurement results are obtained in the past can be used as the measurement conditions for preliminary measurement.
  • the database records past measurement results in association with past measurement conditions, and performs Bayesian optimization based on the past measurement results and the past measurement conditions.
  • the database By determining the measurement conditions for preliminary measurement, and performing Bayesian optimization based on the data obtained by adding the results of preliminary measurement and the measurement conditions for preliminary measurement to the past measurement results and the past measurement conditions. It is characterized by performing the above-mentioned update.
  • the measurement conditions for preliminary measurement are determined by Bayesian optimization based on the past measurement results and measurement conditions, and based on the data obtained by further adding the preliminary measurement results and the measurement conditions for preliminary measurement.
  • the measurement conditions for preliminary measurement are updated. As a result, the measurement conditions for preliminary measurement are updated to be more appropriate.
  • a rule defining how to modify the measurement condition for the preliminary measurement when the result of the preliminary measurement is in a specific state is predetermined, and the preliminary measurement is performed according to the above rule. It is characterized in that the above-mentioned update is performed by modifying the measurement conditions for the above.
  • the measurement conditions for preliminary measurement are updated according to the rules for modifying the measurement conditions for preliminary measurement according to the result of preliminary measurement.
  • the rules are predetermined so that the measurement conditions are modified to improve the measurement results, and the measurement conditions for the preliminary measurement are updated appropriately.
  • the measurement condition search method is characterized in that sample information indicating the content of a sample to be measured, measurement conditions for preliminary measurement, and the result of preliminary measurement are associated and recorded in the database.
  • the measurement conditions for preliminary measurement and the results of preliminary measurement are recorded in a database.
  • the measurement conditions for preliminary measurement and the measurement results of preliminary measurement are also accumulated in the database, and many cases that can be referred to are accumulated.
  • the measurement conditions can be appropriately obtained based on many cases.
  • the computer program according to the present invention represents contents similar to the contents of any sample from a database recorded by associating sample information representing the contents of a sample for which a specific measurement has been made in the past with past measurement conditions.
  • the past measurement conditions associated with the sample information are extracted, the measurement conditions for preliminary measurement are determined based on the extracted past measurement conditions, and the result of the preliminary measurement performed according to the determined measurement conditions for preliminary measurement.
  • the measurement conditions for the preliminary measurement are updated according to the result of the evaluation and the result of the preliminary measurement, and the computer is made to execute the process of repeating the evaluation and the update.
  • the measurement condition search device is a device for searching for measurement conditions when performing a specific measurement on a sample, and includes sample information representing the contents of a sample for which the specific measurement has been performed in the past and past measurement conditions. From the database recorded in association with, the past measurement conditions associated with the sample information representing the contents similar to the contents of the sample to be measured are extracted, and the measurement for preliminary measurement is performed based on the extracted past measurement conditions. The conditions are determined, the result of the preliminary measurement performed according to the determined measurement condition for the preliminary measurement is evaluated, and the measurement condition for the preliminary measurement is updated according to the result of the evaluation and the result of the preliminary measurement. It is characterized in that a process of repeating the evaluation and the update is executed.
  • the measurement system is a system for performing a specific measurement on a sample, and includes a database in which sample information representing the contents of the sample for which the specific measurement has been performed in the past and a database in which the past measurement conditions are associated and recorded are recorded.
  • a measurement condition search device for searching for measurement conditions when performing the specific measurement and a measurement device for executing the specific measurement are provided, and the measurement condition search device includes the contents of a sample to be measured from the database.
  • the past measurement conditions associated with the sample information representing similar contents are extracted, the measurement conditions for preliminary measurement are determined based on the extracted past measurement conditions, and the measurement is performed according to the determined measurement conditions for preliminary measurement. It is possible to evaluate the result of the preliminary measurement executed by the apparatus, update the measurement conditions for the preliminary measurement according to the evaluation result and the preliminary measurement result, and execute the process of repeating the evaluation and the update. It is a feature.
  • the measurement condition search device determines the measurement conditions for preliminary measurement based on the past measurement conditions recorded in the database, executes the preliminary measurement by the measuring device, and evaluates the result of the preliminary measurement. , And the measurement conditions for preliminary measurement are repeatedly updated to search for the measurement conditions. Finally, the measurement conditions for which the evaluation of the preliminary measurement result is good are obtained, and the appropriate measurement conditions for the main measurement are obtained.
  • the measuring device can perform an appropriate main measurement according to the obtained measurement conditions.
  • the present invention even if the user of the measuring device is a beginner with a low level of proficiency, appropriate measurement conditions can be obtained by the measurement condition search method. Therefore, the present invention has excellent effects such as efficient sample analysis.
  • FIG. 1 is a conceptual diagram showing an outline of a measurement condition search method according to the present embodiment.
  • the measurement conditions for preliminary measurement are determined based on the past cases in which the measurement was performed on a similar sample.
  • the preliminary measurement is a preliminary measurement performed to search for measurement conditions.
  • the measurement performed according to the determined measurement condition after the measurement condition is determined is referred to as the main measurement.
  • a preliminary measurement is performed according to the determined measurement conditions.
  • the measurement result by the preliminary measurement is evaluated. If the measurement result is good, determine the measurement conditions for this measurement.
  • the measurement condition is updated by the rule-based AI (artificial intelligence), and the preliminary measurement is executed according to the updated measurement condition. Preliminary measurements, evaluation of measurement results, and updating of measurement conditions are repeated until the measurement results are evaluated as good.
  • rule-based AI artificial intelligence
  • FIG. 2 is a block diagram showing the configuration of the measurement system 100 and showing a configuration example of the measurement device 3.
  • the measurement system 100 executes a measurement condition search method.
  • the measurement system 100 includes a measurement condition search device 1, a storage device 2, and a measurement device 3.
  • the measuring device 3 is a device that performs a specific measurement on a sample in order to measure a specific physical quantity on the sample.
  • the measuring device 3 is a device that measures light or radiation emitted from a sample, such as fluorescent X-rays, Raman scattered light, fluorescence, or cathode luminescence, and acquires a spectrum.
  • FIG. 2 shows an example in which the measuring device 3 is a Raman scattered light measuring device.
  • the measurement condition search device 1 is a device that searches for measurement conditions when measuring with the measurement device 3.
  • the storage device 2 stores a measurement condition database that records the past measurement conditions, which are the measurement conditions when the measurement was performed in the past.
  • the measurement condition search device 1, the storage device 2, and the measurement device 3 are connected to each other.
  • the measurement condition search device 1, the storage device 2, and the measurement device 3 may be connected to each other via a communication network such as a LAN (Local Area Network) or the Internet.
  • LAN Local Area Network
  • the measuring device 3 includes a sample holding unit 35 for holding the sample 4, an irradiation unit 31 for irradiating a laser beam, a mask 341, a beam splitter 342, and a lens 343.
  • sample 4 is a biological sample such as a cell.
  • the sample holding unit 35 is, for example, a sample table on which the sample 4 is placed.
  • the sample holding portion 35 may have a form other than the sample table.
  • the irradiation unit 31 includes a laser light source.
  • the mask 341 has a slit.
  • the laser beam emitted by the irradiation unit 31 is narrowed down to a thin luminous flux by passing through the slit of the mask 341, reflected by the beam splitter 342, passes through the lens 343, and is irradiated to the sample 4.
  • the measuring device 3 further includes a spectroscope 33, a detection unit 32 for detecting light, and a control unit 36.
  • Raman scattered light is generated in the portion of the sample 4 irradiated with the laser beam.
  • the generated Raman scattered light is focused by the lens 343, passes through the beam splitter 342, and is incident on the spectroscope 33.
  • the laser light and the Raman scattered light are indicated by solid arrows.
  • the spectroscope 33 disperses the incident Raman scattered light.
  • the detection unit 32 detects light of each wavelength separated by the spectroscope 33.
  • the measuring device 3 includes an optical system including a large number of optical components such as a mirror, a lens, and a filter for guiding, condensing, and separating laser light and Raman scattered light.
  • optical systems other than the mask 341, the beam splitter 342, and the lens 343 are omitted.
  • the measuring device 3 may be configured such that the laser light from the irradiation unit 31 passes through the beam splitter 342 and the Raman scattered light is reflected by the beam splitter 342.
  • the optical system may not include a mask 341, a beam splitter 342 or a lens 343.
  • the irradiation unit 31, the detection unit 32, and the spectroscope 33 are connected to the control unit 36.
  • the control unit 36 is connected to the measurement condition search device 1.
  • the control unit 36 includes a calculation unit that executes an operation for controlling each unit of the measurement device 3, a memory, and a communication unit that transmits / receives data to / from the measurement condition search device 1.
  • the control unit 36 controls each unit of the measuring device 3.
  • the irradiation unit 31 is controlled on and off by the control unit 36.
  • the spectroscope 33 is controlled by the control unit 36 to control the wavelength of light that is separated and detected by the detection unit 32.
  • the detection unit 32 outputs a signal corresponding to the detection intensity of light of each wavelength to the control unit 36.
  • the control unit 36 inputs the signal output by the detection unit 32, and generates a Raman spectrum based on the wavelength of the light dispersed by the spectroscope 33 and the detection intensity of the light indicated by the input signal.
  • the control unit 36 can adjust the measurement conditions when measuring the Raman scattered light.
  • the measurement conditions include, for example, the intensity of the laser beam applied to the sample 4, the irradiation time, the number of times the intensity of the Raman scattered light is integrated, the width of the slit through which the laser beam passes, the wavelength of the laser beam, or the focal distance.
  • the control unit 36 adjusts the intensity of the laser beam by changing the output of the laser light source included in the irradiation unit 31.
  • the irradiation unit 31 includes a filter that attenuates the laser beam, and the control unit 36 adjusts the intensity of the laser beam by changing the filter.
  • the control unit 36 measures the intensity of the Raman scattered light of each wavelength detected by the detection unit 32 while changing the wavelength of the light to be split by the spectroscope 33, repeats the detection for each wavelength, and measures the Raman scattered light. Adjust the number of times to integrate the strength of.
  • the mask 341 has a plurality of slits having different widths, and the control unit 36 adjusts the width of the slits by changing the slit through which the laser beam passes.
  • the irradiation unit 31 includes a plurality of laser light sources having different wavelengths, and the control unit 36 adjusts the wavelength of the laser light by changing the laser light source to be used.
  • the measuring device 3 includes a plurality of lenses 343 having different focal lengths, and the control unit 36 adjusts the focal lengths by changing the lens 343 to be used.
  • the measuring device 3 may be in the form of changing the position of each component constituting the optical system or changing the position of the sample holding portion 35 when adjusting the focal length.
  • FIG. 3 is a block diagram showing an example of internal functional configurations of the measurement condition search device 1 and the storage device 2.
  • the storage device 2 is configured by using a computer such as a server device.
  • the storage device 2 includes a calculation unit 21, a memory 22, a storage unit 23, and a communication unit 24.
  • the arithmetic unit 21 is configured by using, for example, a CPU (Central Processing Unit), a GPU (Graphics Processing Unit), or a multi-core CPU. Further, the arithmetic unit 21 may be configured by using a quantum computer.
  • the memory 22 stores temporary data generated by the calculation.
  • the memory 22 is, for example, a RAM (RandomAccessMemory).
  • the storage unit 23 is non-volatile, for example, a hard disk.
  • the communication unit 24 is connected to the measurement condition search device 1 and transmits / receives data to / from the measurement condition search device 1.
  • the storage unit 23 stores the computer program 231.
  • the arithmetic unit 21 executes the processing required for the storage device 2 according to the computer program 231.
  • the storage device 2 may be configured by using a plurality of computers.
  • the storage unit 23 stores the measurement condition database 232.
  • FIG. 4 is a chart showing an example of the contents of the measurement condition database 232.
  • the measurement condition database 232 is a database that records past measurement conditions for a specific measurement made in the past.
  • the measurement condition database 232 records sample information representing the contents of a sample for which a specific measurement has been made in the past.
  • the sample information includes the sample name and the pretreatment method performed on the sample prior to the measurement.
  • the sample name included in the sample information is HeLa cells
  • the pretreatment method is that the sample is dispersed in physiological saline or a buffer solution to form a suspension, and the sample is stored at room temperature.
  • the measurement condition database 232 records the measurement conditions in association with the sample information.
  • the measurement conditions are various settings when the measurement is performed by the measuring device 3.
  • the measurement conditions include multiple types of conditions.
  • the recorded measurement conditions are the measurement conditions when the preliminary measurement or the main measurement is performed on the sample represented by the sample information.
  • Preliminary measurement is a preliminary measurement made to search for measurement conditions. This measurement is a measurement performed according to the determined measurement conditions after the measurement conditions are determined.
  • the specific measurement is the measurement of Raman scattered light, and as the measurement conditions, the intensity of the laser light applied to the sample, the irradiation time, the number of times the intensity of the Raman scattered light is integrated, and the like are recorded. There is.
  • the measurement condition database 232 records the measurement results in association with the sample information and the measurement conditions.
  • the measurement result is the result of preliminary measurement or main measurement.
  • scores of a plurality of measurement results are recorded as measurement results.
  • the score is a value obtained by evaluating the measurement result.
  • the score of the measurement result the score regarding the signal intensity, the S / N ratio, the resolution, etc. included in the spectrum of the Raman scattered light is recorded. Each score increases as the measurement result is better, and 1.0 indicates the best condition.
  • the measurement condition search device 1 is configured by using a computer such as a server device.
  • the measurement condition search device 1 includes a calculation unit 11, a memory 12, a drive unit 13, a storage unit 14, an operation unit 15, a display unit 16, and a communication unit 17.
  • the arithmetic unit 11 is configured by using, for example, a CPU, a GPU, or a multi-core CPU. Further, the arithmetic unit 11 may be configured by using a quantum computer.
  • the memory 12 stores temporary data generated by the calculation.
  • the memory 12 is, for example, a RAM.
  • the drive unit 13 reads information from a recording medium 10 such as an optical disc.
  • the storage unit 14 is non-volatile, for example, a hard disk.
  • the operation unit 15 receives information such as text by receiving an operation from the user.
  • the operation unit 15 is, for example, a keyboard or a pointing device.
  • the display unit 16 displays an image.
  • the display unit 16 is, for example, a liquid crystal display or an EL display (Electroluminescent Display).
  • the communication unit 17 is connected to the storage device 2 and the measuring device 3. The communication unit 17 transmits / receives data to / from the storage device 2 and the measuring device 3.
  • the calculation unit 11 causes the drive unit 13 to read the computer program 141 recorded on the recording medium 10, and stores the read computer program 141 in the storage unit 14.
  • the arithmetic unit 11 executes the processing required for the measurement condition search device 1 according to the computer program 141.
  • the computer program 141 may be downloaded from the outside of the measurement condition search device 1. In this case, the measurement condition search device 1 does not have to include the drive unit 13.
  • the measurement condition search device 1 may be configured by using a plurality of computers.
  • the measurement condition search device 1 may be configured by using a plurality of computers connected to each other via a communication network.
  • the measurement condition search device 1 and the storage device 2 may be integrally configured.
  • the storage unit 14 may store the measurement condition database 232, and the measurement condition search device 1 may also have the function of the storage device 2.
  • the measurement condition search device 1 determines the measurement conditions for preliminary measurement, evaluates the measurement results, and executes the process for updating the measurement conditions by the rule-based AI.
  • the rule-based AI is, for example, an expert system.
  • the storage unit 14 stores the knowledge base 142 used for processing the rule-based AI.
  • the knowledge base 142 is composed of a combination of a plurality of if-then rules that specify how to update the measurement conditions for the preliminary measurement according to the result of the preliminary measurement.
  • FIG. 5 is a conceptual diagram showing an example of the contents of the knowledge base 142.
  • the knowledge base 142 contains a plurality of if-then rules.
  • Each if-then rule consists of an if part that represents a determination condition and a then part that represents a consequence.
  • the result of the preliminary measurement is recorded in the if unit.
  • the if part is associated with the then part.
  • the contents of the update of the measurement conditions are recorded in the ten unit.
  • the if-then rule is defined so that the measurement condition recorded in the ten unit associated with the if unit is updated. For example, in the example shown in FIG.
  • the order of judgment is defined in multiple if-then rules. It is determined whether or not the preliminary measurement result recorded in one if unit is obtained, and when the preliminary measurement result recorded in the if unit is obtained, the measurement condition recorded in the ten unit is determined. The update will be done. If the result of the preliminary measurement recorded in the if unit cannot be obtained, it is determined whether or not the result of the preliminary measurement recorded in the next if unit is obtained. For example, if-then rules are used in order from the top shown in FIG. A plurality of if-then rules included in the knowledge base 142 are predetermined so that the measurement conditions are modified in order to improve the measurement result according to the result of the preliminary measurement.
  • the content of the knowledge base 142 may be modifiable. For example, when the user operates the operation unit 15, an instruction to correct the content of the knowledge base 142 is input, and the calculation unit 11 may modify the content of the knowledge base 142 according to the input instruction.
  • FIG. 6 is a flowchart showing a procedure of processing executed by the measurement system 100.
  • the step is abbreviated as S.
  • the arithmetic unit 11 of the measurement condition search device 1 executes the following processing according to the computer program 141.
  • the measurement condition search device 1 first extracts past measurement conditions from the measurement condition database 232 based on the contents of the sample 4 to be measured (S1).
  • the measurement condition search device 1 when the user operates the operation unit 15, information representing the contents of the sample 4 is input to the measurement condition search device 1.
  • the information representing the content of the sample 4 includes the sample name and the pretreatment method.
  • the calculation unit 11 transmits the input information from the communication unit 17 to the storage device 2.
  • the storage device 2 receives the information transmitted from the measurement condition search device 1 in the communication unit 24, and the calculation unit 21 receives the information represented by the sample 4 from the measurement condition database 232 stored in the storage unit 23. Search for sample information that represents content similar to the content.
  • the calculation unit 21 searches for sample information in which the information representing the content of the sample 4 and the sample name and the pretreatment method match.
  • the calculation unit 21 may search for sample information in which a part of the sample name and the pretreatment method match, or may search for sample information in which the sample name matches, and the sample information in which a part of the sample name matches may be searched. You may search for. For example, the calculation unit 21 numerically represents an element included in the sample information, generates a multidimensional coordinate point corresponding to the sample information, and determines a distance from the multidimensional coordinate point corresponding to the information representing the content of the sample 4. You may search for sample information corresponding to the multidimensional coordinate points included in the range.
  • the calculation unit 21 extracts the searched sample information and the past measurement conditions and measurement results associated with the sample information from the measurement condition database 232, and transmits the measurement condition search device 1 from the communication unit 24.
  • the measurement condition search device 1 receives the transmitted sample information, measurement conditions, and measurement results in the communication unit 17.
  • the measurement condition search device 1 may directly search the measurement conditions recorded in the measurement condition database 232. Alternatively, the measurement condition search device 1 may perform a process of extracting measurement conditions based on the image of the sample 4. For example, the image of the sample may be recorded in the measurement condition database 232 as a part of the sample information. The image of the sample 4 is input to the measurement condition search device 1, and the measurement condition search device 1 may extract the measurement conditions associated with the image similar to the image of the sample 4 from the measurement condition database 232.
  • the calculation unit 11 determines the measurement conditions for preliminary measurement based on the extracted past measurement conditions (S2).
  • the measurement conditions include a plurality of types of conditions such as the intensity of the laser beam and the irradiation time.
  • the arithmetic unit 11 determines the extracted past measurement conditions as the measurement conditions for preliminary measurement.
  • the calculation unit 11 selects the past measurement conditions with the best measurement results, and determines the selected measurement conditions as the measurement conditions for preliminary measurement. For example, the calculation unit 11 determines the measurement condition for maximizing the sum of the scores of the plurality of measurement results included in the measurement result as the measurement condition for preliminary measurement.
  • the calculation unit 11 may determine the measurement condition in which the specific score included in the scores of the plurality of measurement results is the maximum as the measurement condition for the preliminary measurement.
  • the measurement conditions when good measurement results are obtained in the past can be used as the measurement conditions for preliminary measurement.
  • the calculation unit 11 may specify a plurality of measurement conditions as measurement conditions for preliminary measurement.
  • the measuring device 3 executes the preliminary measurement according to the determined measurement conditions for the preliminary measurement (S3).
  • the calculation unit 11 transmits information representing the determined measurement conditions for preliminary measurement from the communication unit 17 to the measurement device 3.
  • the control unit 36 of the measuring device 3 receives the information transmitted from the measurement condition search device 1 and executes preliminary measurement by controlling each unit of the measuring device 3 according to the measurement conditions represented by the received information.
  • the measuring device 3 measures the Raman scattered light for the sample 4.
  • the measuring device 3 measures the Raman scattered light after adjusting the measuring conditions.
  • the control unit 36 adjusts the intensity of the laser light emitted by the irradiation unit 31 so as to match the intensity of the laser light included in the measurement conditions.
  • the control unit 36 adjusts the irradiation time of the laser beam irradiated by the irradiation unit 31 so as to match the irradiation time included in the measurement conditions.
  • the control unit 36 adjusts the number of times the intensity of the Raman scattered light detected by the detection unit 32 is integrated so as to match the number of times of integration included in the measurement conditions.
  • control unit 36 adjusts the width of the slit through which the laser beam of the mask 341 passes so as to match the slit width included in the measurement conditions. For example, the control unit 36 adjusts the wavelength of the laser light emitted by the irradiation unit 31 so as to match the wavelength of the laser light included in the measurement conditions. For example, the control unit 36 adjusts the focal length when irradiating the sample 4 with the laser beam so as to match the focal length included in the measurement conditions. In this way, the measuring device 3 performs the preliminary measurement according to the determined measurement conditions for the preliminary measurement.
  • the control unit 36 acquires the result of the preliminary measurement.
  • the control unit 36 acquires a Raman spectrum as a result of measuring the Raman scattered light.
  • the control unit 36 transmits data representing the result of preliminary measurement such as data representing the Raman spectrum to the measurement condition search device 1, the measurement condition search device 1 receives the data in the communication unit 17, and the storage unit 14 receives the data.
  • the measurement condition search device 1 acquires the result of the preliminary measurement.
  • the measurement condition search device 1 next evaluates the result of the preliminary measurement (S4).
  • the calculation unit 11 determines whether or not the evaluation target included in the preliminary measurement result satisfies a predetermined criterion. When the predetermined criteria are satisfied, the predetermined criteria are predetermined so that the preliminary measurement result becomes an appropriate measurement result so that the analysis of the sample 4 can be performed with sufficient accuracy.
  • the evaluation target is the signal strength of the peak included in the Raman spectrum, and the predetermined criterion is that the signal strength exceeds a predetermined threshold value.
  • the evaluation target is the S / N ratio of the Raman spectrum, and the predetermined criterion is that the S / N ratio exceeds a predetermined threshold value.
  • the evaluation target is the resolution of the peak included in the Raman spectrum.
  • the resolution means the half width of the peak.
  • a predetermined criterion is that the resolution is less than or equal to a predetermined threshold.
  • the calculation unit 11 identifies the signal strength, S / N ratio, or resolution of the peak from the Raman spectrum, and evaluates the result of the preliminary measurement by comparing it with a predetermined threshold value.
  • the threshold value is stored in the storage unit 14 in advance or is included in the computer program 141.
  • the calculation unit 11 may calculate the score to be evaluated. For example, the calculation unit 11 calculates the score by dividing the signal strength of the peak by a predetermined threshold value. For example, the calculation unit 11 calculates the score by dividing the S / N ratio by a predetermined threshold value. For example, the calculation unit 11 calculates the score by dividing a predetermined threshold value by the resolution. The calculation unit 11 may determine the score value to 1.0 when the calculated score exceeds 1.0. For example, the calculation unit 11 may determine that the evaluation target satisfies a predetermined criterion when the score of the evaluation target is equal to or higher than a predetermined value.
  • the measurement condition search device 1 next determines whether or not to end the preliminary measurement (S5).
  • the calculation unit 11 determines that the preliminary measurement is terminated when the evaluation target satisfies the predetermined criteria in S4.
  • the calculation unit 11 may evaluate a plurality of evaluation targets in S4, and may make a determination in S5 according to the evaluation of the plurality of evaluation targets. For example, when the predetermined number or more of the evaluation targets each satisfy the predetermined criteria, the calculation unit 11 may determine that the preliminary measurement is completed. For example, when the total of the scores of the plurality of evaluation targets is a predetermined number or more, the calculation unit 11 may determine that the preliminary measurement is completed.
  • the measurement condition search device 1 evaluates the results of the plurality of preliminary measurements.
  • the measurement condition search device 1 updates the measurement conditions for the preliminary measurement (S6).
  • the calculation unit 11 updates the measurement conditions according to the result of the preliminary measurement by the processing of the rule-based AI. More specifically, the arithmetic unit 11 updates the measurement conditions according to the if-then rule included in the knowledge base 142 according to the result of the preliminary measurement. For example, the arithmetic unit 11 refers to the knowledge base 142 as shown in FIG. 5 and determines whether or not the signal strength is low in the result of the preliminary measurement.
  • the calculation unit 11 updates the measurement conditions for preliminary measurement so as to increase the intensity of the laser beam, lengthen the irradiation time, widen the slit width, and change the wavelength of the laser beam. do. If the signal strength is not low, the calculation unit 11 determines whether or not the S / N ratio is low. When the S / N ratio is low, the calculation unit 11 updates the measurement conditions for preliminary measurement so as to increase the number of integrations and widen the slit width. In this way, the measurement condition search device 1 updates the measurement conditions for the preliminary measurement according to the result of the preliminary measurement. The measurement conditions for preliminary measurement are updated appropriately so that the measurement result is better.
  • the measurement condition search device 1 After S6 is completed, the measurement condition search device 1 returns the process to S3.
  • the measurement condition search device 1 repeats the execution of the preliminary measurement, the evaluation of the measurement result, and the update of the measurement condition.
  • the calculation unit 11 repeats the processes of S3 to S6 until the evaluation target included in the preliminary measurement result satisfies a predetermined criterion.
  • the calculation unit 11 may determine that the preliminary measurement is completed when the number of times the processes of S3 to S6 are repeated reaches a predetermined number of times.
  • the calculation unit 11 may determine that the preliminary measurement is completed when the length of time during which the processes of S3 to S6 are repeated reaches a predetermined value.
  • the measurement condition search device 1 determines the measurement conditions for the main measurement (S7).
  • the calculation unit 11 determines the measurement conditions for the preliminary measurement at the time when the measurement result that the evaluation target satisfies the predetermined criteria is obtained as the measurement conditions for the main measurement.
  • the calculation unit 11 brought the measurement conditions for the final preliminary measurement or the evaluation target closest to the predetermined standard.
  • the measurement conditions for preliminary measurement at the time when the measurement result is obtained may be determined as the measurement conditions for the main measurement.
  • the measuring device 3 executes the main measurement according to the determined measurement conditions for the main measurement (S8).
  • the calculation unit 11 transmits the determined information representing the measurement conditions for the measurement from the communication unit 17 to the measurement device 3.
  • the control unit 36 of the measuring device 3 receives the information transmitted from the measurement condition search device 1 and executes this measurement by controlling each unit of the measuring device 3 according to the measurement conditions represented by the received information.
  • the measuring device 3 measures the Raman scattered light for the sample 4.
  • the control unit 36 acquires the result of this measurement such as the Raman spectrum.
  • the control unit 36 transmits data representing the result of this measurement such as a Raman spectrum to the measurement condition search device 1, and the measurement condition search device 1 receives the data in the communication unit 17 and stores it in the storage unit 14. In this way, the measurement condition search device 1 acquires the result of this measurement.
  • the measurement condition search device 1 records the measurement conditions and the measurement results in the measurement condition database 232 (S9).
  • the measurement condition search device 1 records the measurement conditions for the preliminary measurement and the result of the preliminary measurement, and the measurement conditions for the main measurement and the result of the main measurement in the measurement condition database 232.
  • the calculation unit 11 transfers the contents of the sample 4, the measurement conditions for preliminary measurement and the result of the preliminary measurement, and the measurement conditions for the main measurement and the information representing the result of the main measurement from the communication unit 17 to the storage device 2.
  • Information representing the contents of the sample 4 may be input to the measurement condition search device 1 by the user operating the operation unit 15.
  • the result of the preliminary measurement or the main measurement may be a score of the measurement result.
  • the storage device 2 receives the information transmitted from the measurement condition search device 1 in the communication unit 24.
  • the calculation unit 21 records the sample information representing the contents of the sample 4, the measurement conditions for preliminary measurement, and the result of the preliminary measurement in the measurement condition database 232 stored in the storage unit 23 in association with each other. Further, the calculation unit 21 records the sample information representing the contents of the sample 4, the measurement conditions for the main measurement, and the result of the main measurement in the measurement condition database 232 in association with each other.
  • the measurement system 100 may record the measurement conditions for the main measurement and the result of the main measurement in the measurement condition database 232 without recording the measurement conditions for the preliminary measurement and the result of the preliminary measurement.
  • the measurement condition search device 1 may analyze the sample 4 based on the result of this measurement after the processing of S1 to S9 is completed.
  • the arithmetic unit 11 may display the Raman spectrum on the display unit 16.
  • the measurement condition search device 1 determines the measurement conditions for the preliminary measurement based on the past measurement conditions, executes the preliminary measurement, evaluates the result of the preliminary measurement, and reserves.
  • the measurement conditions are searched by repeating the update of the measurement conditions for measurement. Finally, the measurement conditions are obtained so that the evaluation of the result of the preliminary measurement is good. Further, the measurement condition search device 1 updates the measurement conditions for preliminary measurement when the evaluation target included in the preliminary measurement result does not meet the predetermined criteria, and the evaluation target meets the predetermined criteria.
  • the measurement conditions for preliminary measurement are determined as the measurement conditions for main measurement. Predetermined criteria are predetermined so that the sample can be analyzed with sufficient accuracy, and appropriate measurement conditions are searched for.
  • the measurement condition search method can search for appropriate measurement conditions almost automatically, and while avoiding the user from operating the measurement device 3 as much as possible, acquire appropriate measurement conditions and execute this measurement. Can be done. Therefore, the time for the user to handle the sample 4 is shortened, and when the sample 4 is a biological sample such as a cell, the risk of infection to the user due to the biological sample is reduced.
  • the measurement conditions and the measurement results are accumulated in the measurement condition database 232.
  • the measurement conditions and the measurement results are accumulated in the measurement condition database 232.
  • many referenceable cases are accumulated in the measurement condition database 232.
  • appropriate measurement conditions can be obtained based on many cases.
  • the measurement condition search device 1 uses Bayesian optimization. It may be in the form of updating the measurement conditions for preliminary measurement.
  • the function f is Gaussian. This is a method of searching for an explanatory variable xi that maximizes or minimizes the objective variable y, assuming that a process (Gaussian Process) is followed.
  • the objective variable y is used as the score of the measurement result.
  • One of the scores of the plurality of measurement results may be set as the objective variable y, and the sum of the scores of the plurality of measurement results may be set as the objective variable y.
  • each of the plurality of conditions included in the measurement conditions is set as an explanatory variable xi.
  • the score of the past measurement result extracted in S1 and the past measurement condition are used as a data set corresponding to the objective variable and the explanatory variable.
  • the calculation unit 11 generates a plurality of data sets from the plurality of past measurement conditions and measurement results obtained in S1. At this time, the calculation unit 11 may normalize the score of the past measurement result or the past measurement condition.
  • the arithmetic unit 11 calculates an estimated value of the mean and variance of the objective variable when the explanatory variables take their respective values from a plurality of data sets by using the formula of the probability density function of a predetermined Gaussian distribution. do. Further, the calculation unit 11 calculates the explanatory variable that maximizes the predetermined acquisition function based on the estimated values of the mean and the variance of the objective variable, so that the objective variable (measurement result score) is maximized. Calculate the estimated value of the explanatory variable (measurement condition). The calculation unit 11 uses the calculated estimated value as a measurement condition for preliminary measurement. From the past measurement results and measurement conditions, measurement conditions for preliminary measurement that are presumed to be appropriate can be obtained.
  • the calculation unit 11 uses the score of the measurement result calculated from the result of the preliminary measurement and the measurement condition for the preliminary measurement used in S3 as a new data set.
  • the calculation unit 11 calculates an estimated value of the mean and variance of the objective variable when the explanatory variables take their respective values from a plurality of data sets to which a new data set is added. Further, the calculation unit 11 calculates the estimated value of the measurement condition that maximizes the score of the measurement result by calculating the explanatory variable that maximizes the acquisition function based on the calculated estimated value.
  • the calculation unit 11 updates the measurement conditions for preliminary measurement by using the calculated estimated value as the measurement conditions for preliminary measurement. Based on the result of the preliminary measurement and the measurement condition for the preliminary measurement, the measurement condition for the preliminary measurement is updated to be more appropriate.
  • the measurement condition search device 1 repeats the execution of the preliminary measurement, the evaluation of the measurement result, and the update of the measurement condition by the processing of S3 to S6.
  • the calculation unit 11 repeats the processes of S3 to S6 until the evaluation target included in the preliminary measurement result satisfies the predetermined criteria, and performs the processes of S7 to S9 when the evaluation target satisfies the predetermined criteria.
  • the measurement condition search device 1 can efficiently search for appropriate measurement conditions regardless of the user's proficiency level. Therefore, efficient analysis of the sample 4 becomes possible.
  • the measurement condition database 232 by recording the measurement conditions for preliminary measurement and the results of preliminary measurement in the measurement condition database 232, there are many cases that can be used in the Bayesian optimization process, and the time required to search for appropriate measurement conditions is shortened. Will be done.
  • the specific measurement is mainly the measurement of Raman scattered light and the measuring device 3 is the Raman scattered light measuring device, but the specific measurement is the measurement of physical quantities other than Raman scattered light.
  • the specific measurement is the measurement of light or radiation emitted from the sample, such as fluorescent X-rays, Raman scattered light, fluorescence or cathode luminescence, and the measuring device 3 measures such light or radiation and measures the spectrum. It is a device to acquire.
  • the measurement system 100 similarly searches for measurement conditions including the intensity or irradiation time of light or radiation incident on the sample according to the measurement result including signal intensity, S / N ratio or resolution. can do.
  • the specific measurement may be a measurement other than the measurement of light or radiation
  • the measuring device 3 may be a device other than the device for acquiring the spectrum. Even in this form, the measurement system 100 can search for measurement conditions according to the measurement result.
  • the measurement system 100 almost automatically executes the measurement condition search method, but the measurement condition search method may be partially executed by a person.
  • human work may be performed to perform preliminary measurements.
  • the measurement conditions searched by the measurement condition search device 1 may include a pretreatment method performed on the sample 4 before the measurement.
  • the process of performing the preliminary measurement and the main measurement includes the process of performing the pretreatment on the sample 4.
  • the measurement system 100 shows a form including the measurement condition search device 1, the storage device 2, and the measurement device 3, but the measurement system 100 further analyzes the sample 4 based on the result of this measurement. It may be equipped with an analyzer. The analyzer acquires the result of this measurement from the measurement condition search device 1 or the measuring device 3, and executes an analysis on the sample 4 such as a composition analysis.
  • the storage device 2 is connected to a single measurement condition search device 1, but the storage device 2 is connected to a plurality of measurement condition search devices 1 via a communication network such as the Internet. It may be in the same form.
  • the measurement condition database 232 stored in the storage device 2 extracts information such as measurement conditions from a plurality of measurement condition search devices 1, and adds information such as measurement results from the plurality of measurement condition search devices 1. .. It is possible to efficiently search for measurement conditions based on the measurement results obtained by the plurality of measuring devices 3.
  • Measurement system 1 Measurement condition search device 10 Recording medium 141 Computer program 2 Storage device 232 Measurement condition database 3 Measurement device 4 Sample

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WO2025204654A1 (ja) * 2024-03-28 2025-10-02 コニカミノルタ株式会社 光計測装置、光計測システム及びガンマ調整方法

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WO2025204654A1 (ja) * 2024-03-28 2025-10-02 コニカミノルタ株式会社 光計測装置、光計測システム及びガンマ調整方法

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