A method and apparatus for time-resolved electrochemical Raman testing

Abstract

This application relates to a method and apparatus for time-resolved electrochemical Raman spectroscopy. The method includes: acquiring a delay time parameter, potential waveform data, and an initial trigger signal; performing event trigger detection on the initial trigger signal to obtain an event trigger timestamp; at the event trigger timestamp, converting the potential waveform data based on the initial trigger signal to obtain a potential pulse signal; the potential pulse signal is used to indicate the initiation of an electrochemical reaction; at the event trigger timestamp, determining the laser trigger delay amount corresponding to the potential pulse signal based on the delay time parameter; at the event trigger timestamp, transforming the potential pulse signal based on the laser trigger delay amount to generate a laser trigger pulse signal; wherein the laser trigger pulse signal is used to indicate the emission of a pulsed laser; acquiring the reaction current signal corresponding to the electrochemical reaction and the Raman spectrum corresponding to the electrochemical reaction under pulsed laser irradiation. This method can improve the tracking accuracy of rapid electrochemical processes.

Description

Technical Field

[0001] This invention belongs to the field of electrochemical detection, and in particular relates to a time-resolved electrochemical Raman testing method and apparatus. Background Technology

[0002] In electrochemical research, the electrode / electrolyte interface is the core region for charge transfer and chemical reactions. A deep understanding of the microstructure at the interface, the formation and evolution of reaction intermediates, and the dynamic physicochemical processes is crucial for revealing reaction mechanisms and designing high-performance catalysts and energy storage materials. While traditional electrochemical methods offer extremely high temporal resolution and sensitivity, they cannot provide direct molecular structural information. Therefore, researchers have developed various in-situ spectroscopic electrochemical techniques. Among them, Raman spectroscopy, which can provide fingerprint structural information of molecules on the electrode surface, has become a powerful tool for studying electrochemical interfaces. However, the temporal resolution of current in-situ electrochemical Raman techniques is typically on the order of seconds to minutes, making it difficult to capture key intermediate species and interfacial processes with lifetimes of only microseconds or even shorter in electrochemical reactions.

[0003] To improve time resolution, some existing technologies have been explored, but all have certain limitations: (1) Based on software integration, the synchronization method uses a computer central control system to drive the electrochemical workstation, light source and spectral acquisition module to operate in a time sequence through program instructions. However, due to the multi-task scheduling mechanism of the operating system, the time sequence uncertainty of software instruction parsing, and the delay in the response of each module, the time error accumulates from milliseconds to seconds, making it difficult to achieve high-precision time synchronization of the key time nodes of electrochemical pumping and spectral detection. (2) Based on the pump-probe principle, the reaction is triggered by potential control, and the time-resolved spectrum is obtained by controlling the delay time of the probe laser. For example, the time resolution of the continuous laser is limited by the rotation speed and mechanical jitter of the chopper, and it is difficult to break through the bottleneck of hundreds of microseconds. (3) Most studies still use conventional electrodes at the millimeter level. Their large double-layer charging and discharging capacitance causes the response time constant of the electrochemical system to usually be at the millisecond level, which fundamentally limits the system's ability to track fast electrochemical processes. Summary of the Invention

[0004] Therefore, it is necessary to provide a time-resolved electrochemical Raman testing method and apparatus that can improve the accuracy of tracking rapid electrochemical processes, addressing the aforementioned technical problems.

[0005] In a first aspect, this application provides a time-resolved electrochemical Raman spectroscopy method, comprising:

[0006] Acquire delay time parameters, potential waveform data, and initial trigger signal; the initial trigger signal is used to characterize the mapping relationship between the spectral acquisition trigger value and the timestamp;

[0007] Perform event trigger detection on the initial trigger signal to obtain the event trigger timestamp;

[0008] At the event trigger timestamp, the potential waveform data is converted based on the initial trigger signal to obtain a potential pulse signal; the potential pulse signal is used to indicate the initiation of the electrochemical reaction;

[0009] Under the event trigger timestamp, the laser trigger delay corresponding to the potential pulse signal is determined based on the delay time parameter;

[0010] Under the event trigger timestamp, the potential pulse signal is transformed based on the laser trigger delay to generate a laser trigger pulse signal; wherein, the laser trigger pulse signal is used to indicate the emission of pulsed laser.

[0011] Obtain the reaction current signal corresponding to the electrochemical reaction and the Raman spectrum corresponding to the electrochemical reaction under pulsed laser irradiation.

[0012] Furthermore, event trigger detection is performed on the initial trigger signal to obtain the event trigger timestamp, including:

[0013] The spectral acquisition trigger values ​​in the initial trigger signal that are greater than the preset threshold voltage parameter are marked as candidate trigger values, and the timestamps corresponding to the candidate trigger values ​​are marked as candidate timestamps;

[0014] Extract consecutive candidate timestamps from the initial trigger signal to form a candidate timestamp set;

[0015] Identify the number of candidate timestamps in each candidate timestamp set, obtain the number of consecutive timestamps in each candidate timestamp set, and mark the candidate timestamp set with a number of consecutive timestamps greater than the preset debouncing value as a valid trigger set;

[0016] The earliest timestamp in each valid trigger set is determined as the event trigger timestamp.

[0017] Furthermore, the potential waveform data includes the potential amplitude and the corresponding duration. Based on the event trigger timestamp and using the initial trigger signal as a reference, the potential waveform data is transformed to obtain a potential pulse signal, including:

[0018] Using the event trigger timestamp as the starting point, the potential waveform data is transformed to obtain a potential pulse signal, where the expression for the potential pulse signal is:

[0019]

[0020]

[0021] In the formula, It is any timestamp in the potential pulse signal. It is the timestamp in the potential pulse signal The corresponding voltage amplitude, It is the potential amplitude in the potential waveform data. It is the event trigger timestamp. It is the duration corresponding to the potential amplitude in the potential waveform data.

[0022] Furthermore, under the event trigger timestamp, the laser triggering delay corresponding to the potential pulse signal is determined based on the delay time parameter, including:

[0023] Based on the delay time parameter and the preset potential pulse signal time accuracy parameter, the edge delay unit number is calculated, where the expression for the edge delay unit number is:

[0024]

[0025] In the formula, It is the number of edge delay units. It is a delay time parameter. It is a parameter for the timing accuracy of the potential pulse signal. It is a rounding down process;

[0026] The laser trigger delay is obtained by multiplying the edge delay unit number and the potential pulse signal timing accuracy parameter.

[0027] Furthermore, under the event trigger timestamp, the potential pulse signal is transformed based on the laser trigger delay to generate a laser trigger pulse signal, including:

[0028] Based on the laser triggering delay, the potential pulse signal is delayed to obtain a delayed potential pulse signal;

[0029] Edge-locking is performed on the delayed potential pulse signal to obtain the reference trigger edge signal;

[0030] Based on the preset laser trigger level amplitude, the reference trigger edge signal is level-converted to obtain the standard level trigger edge signal;

[0031] The standard level trigger edge signal is controlled by pulse width control according to the preset pulse width parameters to obtain the laser trigger pulse signal.

[0032] Secondly, this application also provides a time-resolved electrochemical Raman testing device, comprising:

[0033] The data acquisition module is used to acquire delay time parameters, potential waveform data, and initial trigger signal; the initial trigger signal is used to characterize the mapping relationship between the spectral acquisition trigger value and the timestamp.

[0034] The timestamp detection module is used to detect event triggering on the initial trigger signal and obtain the event trigger timestamp.

[0035] The reaction signal generation module is used to convert the potential waveform data based on the initial trigger signal at the event trigger timestamp to obtain a potential pulse signal; the potential pulse signal is used to indicate the initiation of the electrochemical reaction;

[0036] The delay time calculation module is used to determine the laser triggering delay amount corresponding to the potential pulse signal based on the delay time parameter under the event triggering timestamp;

[0037] The laser signal generation module is used to transform the potential pulse signal based on the laser trigger delay at the event trigger timestamp to generate a laser trigger pulse signal; wherein, the laser trigger pulse signal is used to indicate the emission of pulsed laser.

[0038] The signal acquisition unit is used to acquire the reaction current signal corresponding to the electrochemical reaction and the Raman spectrum corresponding to the electrochemical reaction under pulsed laser irradiation.

[0039] Thirdly, this application also provides a computer device, including a memory and a processor, wherein the memory stores a computer program, and the processor executes the computer program to implement any of the time-resolved electrochemical Raman testing methods described in the first aspect of this application.

[0040] Fourthly, this application also provides a computer-readable storage medium having a computer program stored thereon, which, when executed by a processor, implements any of the time-resolved electrochemical Raman testing methods described in the first aspect of this application.

[0041] The aforementioned method and apparatus for time-resolved electrochemical Raman spectroscopy involves acquiring delay time parameters, potential waveform data, and an initial trigger signal. The initial trigger signal characterizes the mapping relationship between the spectral acquisition trigger value and the timestamp. Event trigger detection is performed on the initial trigger signal to obtain the event trigger timestamp. At the event trigger timestamp, the potential waveform data is converted based on the initial trigger signal to obtain a potential pulse signal. This potential pulse signal indicates the initiation of the electrochemical reaction. At the event trigger timestamp, the laser trigger delay corresponding to the potential pulse signal is determined based on the delay time parameters. At the event trigger timestamp, the potential pulse signal is transformed based on the laser trigger delay to generate a laser trigger pulse signal, which indicates the emission of a pulsed laser. The method also acquires the reaction current signal corresponding to the electrochemical reaction and the Raman spectrum corresponding to the electrochemical reaction under pulsed laser irradiation. This achieves precise timing synchronization between the potential pulse signal and the laser trigger pulse signal at the hardware level, eliminating time errors caused by software scheduling delays and mechanical modulation jitter, achieving a time resolution at the microsecond level. This effectively captures the spectral information of short-lived intermediate species in electrochemical reactions, improving the tracking accuracy of rapid electrochemical processes. Attached Figure Description

[0042] To more clearly illustrate the technical solutions in the embodiments or related technologies of this application, the accompanying drawings used in the description of the embodiments or related technologies will be briefly introduced below. Obviously, the accompanying drawings described below are only some embodiments of this application. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0043] Figure 1 A schematic diagram illustrating the implementation environment of a time-resolved electrochemical Raman testing method according to an embodiment of this application;

[0044] Figure 2 A schematic flowchart of a time-resolved electrochemical Raman spectroscopy method provided in one embodiment of this application;

[0045] Figure 3 A waveform diagram of potential waveform data for electrode activation treatment in a time-resolved electrochemical Raman testing method provided in one embodiment of this application;

[0046] Figure 4 A schematic diagram showing the comparison of Raman spectra before and after activation for a time-resolved electrochemical Raman testing method provided in one embodiment of this application;

[0047] Figure 5 A schematic diagram of Raman spectral comparison for a time-resolved electrochemical Raman testing method provided in one embodiment of this application;

[0048] Figure 6 A schematic diagram of Raman spectral peak intensity variation for a time-resolved electrochemical Raman testing method provided in one embodiment of this application;

[0049] Figure 7 A schematic diagram of pulsed laser time interval error for a time-resolved electrochemical Raman testing method provided in one embodiment of this application;

[0050] Figure 8 This is a schematic diagram of a time-resolved electrochemical Raman testing device provided in one embodiment of this application. Detailed Implementation

[0051] To make the objectives, technical solutions, and advantages of this application clearer, the following detailed description is provided in conjunction with the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative and not intended to limit the scope of this application.

[0052] This application provides a time-resolved electrochemical Raman spectroscopy method that can be applied to, for example... Figure 1 The application environment shown includes a potential delay control terminal 101, a pulsed laser emitter 102, an electrochemical reaction device 103, a spectral acquisition device 104, and an information configuration processing terminal 105. The information configuration processing terminal 105 can be, but is not limited to, various personal computers, laptops, tablets, industrial control computers, and other electronic devices with data input and program execution capabilities. The operator can set delay time parameters and potential waveform parameters through the information configuration processing terminal 105, and process and analyze the acquired Raman spectra. The spectral acquisition device 104 may include a Raman optical path, a spectrometer, and a spectral detector; the spectral acquisition device 104 is used to send an initial trigger signal to the potential delay control terminal 101 when spectral acquisition begins, and to acquire the Raman spectrum generated by the electrochemical reaction after pulsed laser irradiation and transmit it to the potential delay control terminal 101. The pulsed laser emitter 102 is used to receive the laser trigger pulse signal output by the potential delay control terminal 101, and emits a pulsed laser to the electrochemical reaction device 103 under the trigger of this signal. The electrochemical reaction device 103 may include an electrolytic cell and a working electrode and a counter electrode disposed in the electrolytic cell, for receiving potential pulse signals output by the potential delay control terminal 101 to initiate and control the electrochemical reaction on the surface of the working electrode.

[0053] Furthermore, the potential delay control terminal 101 integrates potential control function, delay control function, and current signal sampling function. It is used to receive the delay time parameter and potential waveform parameter output by the information configuration processing terminal 105, and after receiving the initial trigger signal from the spectral acquisition device 104, it generates a potential pulse signal and a laser trigger pulse signal. At the same time, it samples the current signal of the electrochemical reaction device 103 to obtain the reaction current signal. After receiving the Raman spectrum generated by the spectral acquisition device 104, the potential delay control terminal 101 also sends the Raman spectrum and the reaction current signal to the information configuration processing terminal 105.

[0054] The potential delay control terminal 101 and the information configuration processing terminal 105 can be connected via a wired communication network or a wireless communication network. The potential delay control terminal 101 is connected to the spectral acquisition device 104, the pulsed laser emitter 102, and the electrochemical reaction device 103 via wired connections. The wired connection interface can be a signal transmission interface such as an SMA interface or a BNC interface to ensure low latency and high reliability of trigger signal transmission. The information configuration processing terminal 105 and the spectral acquisition device 104 can be connected via a wired communication network or a wireless communication network, so that the spectral acquisition device 104 can be initialized and its parameters set through the information configuration processing terminal 105.

[0055] In one exemplary embodiment, such as Figure 2 As shown, a time-resolved electrochemical Raman spectroscopy method is provided, which can be applied to... Figure 1 The following description is based on the potential delay control terminal 101, including the following steps S101 to S106:

[0056] S101, acquire delay time parameters, potential waveform data and initial trigger signal; the initial trigger signal is used to characterize the mapping relationship between the spectral acquisition trigger value and the timestamp.

[0057] Specifically, the potential delay control terminal acquires delay time parameters, potential waveform data, and an initial trigger signal. The delay time parameter is a value pre-set by the operator through the information configuration processing terminal, defining the waiting time from the start of the electrochemical reaction to the pulsed laser emission time; the unit can be microseconds. The initial trigger signal is emitted by the spectral acquisition device at the start of exposure and spectrum acquisition, characterizing the mapping relationship between the spectral acquisition trigger value and the timestamp. The timestamps in the initial trigger signal are arranged at equal intervals, with the interval between adjacent timestamps corresponding to a fixed physical duration. The mathematical form of the initial trigger signal is a time-varying level signal, which can be expressed as: ,in, It can be any timestamp. The initial trigger signal at the timestamp The corresponding spectral acquisition trigger value at that location, This is the timestamp when the spectral acquisition device begins acquiring data. The spectral acquisition trigger value is a logic level value. When it is a low level value, that is This indicates that the spectral acquisition device was at the timestamp. Stop collecting spectra. When it is a high level value, that is This indicates that the spectral acquisition device was at the timestamp. Spectral acquisition begins. Upon receiving the initial trigger signal, the potential delay control terminal samples the signal using its own system clock, aligning the timestamp of 0 in the initial trigger signal with a specific sampling time point on the system clock. Thus, each timestamp value in the initial trigger signal uniquely corresponds to a sampling time point on the system clock of the potential delay control terminal. Potential waveform data defines the amplitude and duration of the potential pulse required for a single electrochemical reaction. The potential waveform data includes the potential amplitude and its corresponding duration. The potential amplitude represents the voltage applied to the electrochemical reaction device, measured in volts; the duration represents the length of time the voltage amplitude is maintained, measured in microseconds. This data can be set and transmitted to the potential delay control terminal via the information configuration processing terminal.

[0058] S102, perform event trigger detection on the initial trigger signal to obtain the event trigger timestamp.

[0059] Specifically, during the continuous reception of the initial trigger signal, the potential delay control terminal performs event trigger detection on the initial trigger signal, identifies the spectral acquisition trigger flag and its corresponding timestamp in the initial trigger signal, and obtains the event trigger timestamp. Event trigger detection refers to the process of continuously monitoring and judging the spectral acquisition trigger value of the initial trigger signal, filtering out glitches and contact jitter on the signal line, and determining the actual moment when spectral acquisition occurs. The event trigger timestamp refers to the first timestamp in the initial trigger signal corresponding to the start of continuous spectral acquisition by the spectral acquisition device; mathematically, it can be a single timestamp. The generation of subsequent potential pulse signals and the calculation of delay times are both based on the event trigger timestamp, thus ensuring the accuracy of the timing relationship between potential pulses and laser pulses.

[0060] S103, under the event trigger timestamp, uses the initial trigger signal as a reference to convert the potential waveform data to obtain a potential pulse signal; the potential pulse signal is used to indicate the initiation of the electrochemical reaction.

[0061] Specifically, after determining the event trigger timestamp, the potential delay control terminal uses the event trigger timestamp as the starting point to convert the potential waveform data into a potential pulse signal. When the system clock of the potential delay control terminal advances to the sampling time point of the system clock corresponding to the event trigger timestamp, the potential delay control terminal generates a potential pulse signal based on the potential waveform data and outputs it to the electrochemical reaction device. The potential pulse signal is a physical voltage signal, mathematically represented as a single square wave signal with a constant potential amplitude starting from the event trigger timestamp and lasting for a duration. The potential pulse signal is used to indicate the start-up of the electrochemical reaction device and control the electrochemical reaction. By applying this potential pulse signal between the working electrode and the counter electrode, the type and intensity of the electrochemical reaction triggered on the working electrode surface are controlled. Under the system clock of the potential delay control terminal, the event trigger timestamp uniquely corresponds to a sampling time point of the system clock, and the output starting edge of the potential pulse signal is strictly aligned with this sampling time point, ensuring the timing synchronization between the potential pulse signal and the initial trigger signal.

[0062] S104, under the event trigger timestamp, determine the laser trigger delay amount corresponding to the potential pulse signal based on the delay time parameter.

[0063] Specifically, when the system clock advances to the sampling time point corresponding to the event trigger timestamp, the potential delay control terminal determines the laser trigger delay amount corresponding to the potential pulse signal based on the delay time parameter. The laser trigger delay amount refers to the physical duration that the potential delay control terminal needs to wait after detecting the pulse edge of the potential pulse signal, and its unit can be microseconds. The laser trigger delay amount, determined by the delay time parameter, characterizes the time interval between the appearance of the pulse edge in the potential pulse signal and the time when the laser trigger pulse signal should be output, providing a timing reference for the generation of subsequent laser trigger pulse signals and ensuring a defined timing relationship between each potential pulse edge and subsequent laser trigger pulses.

[0064] S105, under the event trigger timestamp, transform the potential pulse signal based on the laser trigger delay to generate a laser trigger pulse signal; wherein, the laser trigger pulse signal is used to indicate the emission of pulsed laser.

[0065] Specifically, the potential delay control terminal transforms the potential pulse signal in conjunction with the laser trigger delay amount to generate a laser trigger pulse signal, which is then output to the pulsed laser transmitter. Transforming the potential pulse signal means using the potential pulse signal as the processing object, and through delay processing and waveform reconstruction, converting the potential pulse signal into a laser trigger pulse signal that meets the triggering requirements of the pulsed laser transmitter. The transformation process may include: delaying the potential pulse signal based on the laser trigger delay amount, so that the edge of the transformed signal is delayed by the duration specified by the laser trigger delay amount relative to the original edge of the potential pulse signal; and reconstructing the waveform of the delayed signal to meet the pulsed laser transmitter's level standard and pulse width requirements for the input trigger signal. The laser trigger pulse signal is used to instruct the pulsed laser transmitter to emit a pulsed laser. The rising edge of the laser trigger pulse signal indicates that the pulsed laser transmitter emits a single pulsed laser, which irradiates the working electrode surface of the electrochemical reaction device, exciting Raman scattered light representing the molecular structure information of the electrode surface at that delay moment.

[0066] S106, acquire the reaction current signal corresponding to the electrochemical reaction and the Raman spectrum corresponding to the electrochemical reaction under pulsed laser irradiation.

[0067] Specifically, the potential delay control terminal acquires the reaction current signal corresponding to the electrochemical reaction and the Raman spectrum corresponding to the electrochemical reaction after pulsed laser irradiation. The Raman spectrum is spectral data recorded by the spectral detector in the spectral acquisition device during acquisition, showing the change in Raman scattered light intensity with Raman shift. After the laser trigger pulse signal triggers the pulsed laser emitter to irradiate the working electrode surface, the spectral acquisition device acquires the scattered light signal, obtaining the Raman spectrum containing information about the molecular structure of the electrode surface at that delay time. The reaction current signal is the current signal flowing through the current loop between the working electrode and the counter electrode, obtained by sampling and detecting the electrochemical reaction device through the potential delay control terminal. It is used to characterize the change in the electron transfer rate on the electrode surface over time during the electrochemical reaction, reflecting the rate and progress of the electrochemical reaction on the electrode surface. The potential delay control terminal forwards the Raman spectrum and reaction current signal to the information configuration processing terminal for storage and analysis. For example, the information configuration processing terminal can plot a Raman spectrum with Raman shift as the abscissa and Raman signal intensity as the ordinate, and a current-time curve with time as the abscissa and current value as the ordinate, thus collaboratively analyzing the electrochemical reaction process from both the molecular structure and electron transfer rate perspectives. By setting multiple different delay time parameters and using the same potential waveform data, and repeatedly executing steps S101 to S106, Raman spectra and reaction current signals at different delay times can be obtained, thereby simultaneously reconstructing the complete kinetic curve of the chemical reaction on the electrode surface over time from both molecular structure information and reaction rate dimensions.

[0068] This embodiment provides a time-resolved electrochemical Raman spectroscopy method. By acquiring delay time parameters, potential waveform data, and an initial trigger signal, the method performs event trigger detection on the initial trigger signal to obtain an event trigger timestamp as a unified timing reference. Under the event trigger timestamp, the potential waveform data is converted into a potential pulse signal to initiate and control the electrochemical reaction. Based on the delay time parameters, the laser trigger delay corresponding to the potential pulse signal is determined. Based on the laser trigger delay, the potential pulse signal is transformed to generate a laser trigger pulse signal to trigger pulsed laser irradiation. The Raman spectrum corresponding to the electrochemical reaction under pulsed laser irradiation is obtained. This achieves delayed trigger control based on the potential pulse signal itself, ensuring that each potential pulse edge has a corresponding laser trigger pulse that precisely corresponds to it. This eliminates time errors caused by software scheduling delays and mechanical modulation jitter, achieving a time resolution at the microsecond level. It can effectively capture the spectral information of short-lived intermediate species in electrochemical reactions, improving the tracking accuracy of rapid electrochemical processes.

[0069] In one embodiment, event trigger detection is performed on the initial trigger signal to obtain the event trigger timestamp, including:

[0070] S201, mark the spectral acquisition trigger values ​​in the initial trigger signal that are greater than the preset threshold voltage parameter as candidate trigger values, and mark the timestamps corresponding to the candidate trigger values ​​as candidate timestamps.

[0071] Specifically, a preset threshold voltage parameter is used to distinguish between valid high-level and low-level noise in the initial trigger signal. This parameter can be set according to actual operation and is configured and loaded into the potential delay control terminal via the information configuration processing terminal. The potential delay control terminal iterates through each timestamp in the initial trigger signal, compares the spectral acquisition trigger value corresponding to that timestamp with the preset threshold voltage parameter, and marks the spectral acquisition trigger value as a candidate trigger value and the timestamp corresponding to that spectral acquisition trigger value as a candidate timestamp. The candidate trigger value represents the high-level portion of the sampling point that is initially judged to be a possible valid trigger event; the candidate timestamp records the position of the candidate trigger value on the time axis of the initial trigger signal.

[0072] S202, extract consecutive candidate timestamps from the initial trigger signal to form a candidate timestamp set.

[0073] Specifically, the potential delay control terminal performs a continuity analysis on all candidate timestamps, merging temporally adjacent candidate timestamps into the same candidate timestamp set. A consecutive candidate timestamp means that on the timeline of the initial trigger signal, there are no unmarked timestamps between two adjacent candidate timestamps; that is, the index difference between two candidate timestamps is 1. Starting from the first candidate timestamp, the potential delay control terminal sequentially checks whether the timestamp indices of adjacent candidate timestamps are consecutive. If they are consecutive, the next candidate timestamp is added to the currently constructed candidate timestamp set; if they are not consecutive, the construction of the current candidate timestamp set ends, and the construction of the next candidate timestamp set begins with the newly appearing candidate timestamp. The mathematical form of a candidate timestamp set can be a sequence of timestamps. ,in This is the starting timestamp of the candidate timestamp set. This represents the number of timestamps contained in the candidate timestamp set.

[0074] S203, identify the number of candidate timestamps in each candidate timestamp set, obtain the number of consecutive timestamps in each candidate timestamp set, and mark the candidate timestamp set with the number of consecutive timestamps greater than the preset debouncing value as a valid trigger set.

[0075] Specifically, the preset debouncing value is used to distinguish between the sustained high-level period of a real trigger event and the instantaneous pulse of interference glitches. It can be determined based on the typical jitter width of the initial trigger signal output by the spectral acquisition device and the sampling frequency of the system clock of the spectral acquisition device. This value is set via the information configuration processing terminal and loaded into the potential delay control terminal before the experiment. For example, if the sampling period of the system clock of the spectral acquisition device is 10 nanoseconds and the expected maximum jitter width is 100 nanoseconds, the preset debouncing value can be set to 10. For each candidate timestamp set, the potential delay control terminal counts the number of candidate timestamps contained in the set, obtaining the number of consecutive timestamps in that candidate timestamp set. The number of consecutive timestamps characterizes the duration of the high-level period corresponding to that candidate timestamp set; a larger number of consecutive timestamps indicates that the high-level period lasts longer on the time axis. The potential delay control terminal compares the number of consecutive timestamps in each candidate timestamp set with a preset debouncing value. If the number of consecutive timestamps is greater than the preset debouncing value, it indicates that the high-level duration corresponding to the candidate timestamp set is long enough and can be determined as a high-level segment generated by a real trigger event. The candidate timestamp set is then marked as a valid trigger set. The valid trigger set represents the sequence of consecutive high-level segments in the initial trigger signal that are determined to be real trigger events.

[0076] S204, determine the earliest timestamp in each valid trigger set as the event trigger timestamp.

[0077] Specifically, after filtering out the valid trigger sets, the potential delay control terminal selects the timestamp with the smallest timestamp value among all valid trigger sets, i.e., the earliest timestamp in the valid trigger set, as the event trigger timestamp, which can be denoted as: The event trigger timestamp corresponds to the moment when the high-level segment of the valid spectral acquisition start in the initial trigger signal first appears, indicating the moment when the spectral acquisition exposure cycle officially begins. In the timestamp coordinate system of the initial trigger signal, this event trigger timestamp serves as the unified time reference for all subsequent timing synchronization operations performed by the potential delay control terminal. The system clock of the potential delay control terminal aligns the moment when the timestamp in the initial trigger signal is 0 with a certain moment of its own system clock, thus determining the event trigger timestamp. The sampling time point corresponds uniquely to the system clock of the potential delay control terminal. The output of subsequent potential pulse signals and the calculation of delay time are all performed starting from the sampling time point of this system clock.

[0078] This embodiment provides a time-resolved electrochemical Raman spectroscopy method. It marks spectral acquisition trigger values ​​in the initial trigger signal that exceed a preset threshold voltage parameter as candidate trigger values ​​and their candidate timestamps. Continuous candidate timestamps are extracted to form a candidate timestamp set. The number of continuous timestamps in each set is identified, and sets with a number greater than a preset de-jitter value are marked as valid trigger sets. The earliest timestamp in each valid trigger set is determined as the event trigger timestamp. This effectively filters out instantaneous glitches caused by contact jitter and electromagnetic interference during the transmission of the initial trigger signal, ensuring that the event trigger timestamp accurately reflects the true moment when the spectral acquisition device begins exposure and acquisition. This provides a reliable timing reference for subsequent potential pulse signal generation and delay time calculation.

[0079] In one embodiment, the potential waveform data includes the potential amplitude and the corresponding duration. Based on the event trigger timestamp and using the initial trigger signal as a reference, the potential waveform data is converted to obtain a potential pulse signal, including:

[0080] S301, using the event trigger timestamp as the starting point, transforms the potential waveform data to obtain a potential pulse signal, wherein the expression of the potential pulse signal is:

[0081]

[0082]

[0083] In the formula, It is any timestamp in the potential pulse signal. It is the timestamp in the potential pulse signal The corresponding voltage amplitude, It is the potential amplitude in the potential waveform data. It is the event trigger timestamp. It is the duration corresponding to the potential amplitude in the potential waveform data.

[0084] Specifically, potential waveform data includes potential amplitude. and the duration corresponding to the potential amplitude Composition. Potential amplitude This indicates the voltage applied to the electrochemical reaction apparatus, measured in volts. Its value can be determined based on the driving voltage required for the electrochemical reaction. For example, for the oxidation of potassium ferrocyanide, the potential amplitude can be set to 0.4V. Duration This indicates the duration the voltage amplitude is maintained during the output process, in microseconds. Its value can be determined based on the required duration of the electrochemical reaction; for example, the duration can be set to 200 microseconds. After determining the event trigger timestamp, the potential delay control terminal uses this timestamp as the starting point to read the potential amplitude and duration from the potential waveform data. Through digital-to-analog conversion and power amplification, it then... Internal continuous output voltage value A single square wave signal, i.e., a potential pulse signal. The potential pulse signal is used to indicate the start-up and control of the electrochemical reaction in the electrochemical reaction device. By applying the potential pulse signal between the working electrode and the counter electrode, the electrochemical reaction is triggered on the surface of the working electrode. Under the system clock of the potential delay control terminal, the event trigger timestamp uniquely corresponds to a sampling time point of the system clock, and the output start edge of the potential pulse signal is strictly aligned with this sampling time point.

[0085] This embodiment provides a time-resolved electrochemical Raman spectroscopy method. By using the event trigger timestamp as the starting point, it reads the potential amplitude and duration from the potential waveform data, and generates a single square wave signal with a constant potential amplitude as a potential pulse signal within a specified time interval. This achieves precise timing control of the potential pulse signal, ensuring that the driving voltage applied to the electrochemical reaction device is strictly synchronized with the spectral acquisition trigger event in time. Furthermore, the voltage amplitude and duration can be flexibly configured according to the needs of different electrochemical reactions, improving the accuracy of the reaction driving timing and the programmability of experimental conditions in electrochemical Raman spectroscopy.

[0086] In one embodiment, determining the laser triggering delay amount corresponding to the potential pulse signal based on the delay time parameter under the event triggering timestamp includes:

[0087] S401, based on the delay time parameter and the preset potential pulse signal time accuracy parameter, calculates the edge delay unit number, where the expression for the edge delay unit number is:

[0088]

[0089] In the formula, It is the number of edge delay units. It is a delay time parameter. It is a parameter for the timing accuracy of the potential pulse signal. It is a rounding down process.

[0090] Specifically, after determining the event trigger timestamp, the potential delay control terminal calculates the number of edge delay units based on the aforementioned formula, according to the delay time parameter and the preset potential pulse signal time precision parameter. The preset potential pulse signal time precision parameter characterizes the minimum physical duration between two adjacent resolvable time points in the potential pulse signal, and its unit can be microseconds. The value of the preset potential pulse signal time precision parameter can be determined based on the update rate of the waveform generator in the potential delay control terminal. For example, if the update rate of the waveform generator is 100MHz, the interval between adjacent resolvable time points is 0.01 microseconds, and the preset potential pulse signal time precision parameter can be set to 0.01 microseconds. The preset potential pulse signal time precision parameter can be pre-set and loaded into the potential delay control terminal through the information configuration processing terminal before the experiment. The number of edge delay units is a dimensionless integer representing the number of time units that need to be delayed after detecting the pulse edge of the potential pulse signal at the given time precision. The number of edge delay units is obtained by dividing the delay time parameter by the preset potential pulse signal time accuracy parameter and then rounding down. The rounding down process ensures that the actual waiting time does not exceed the preset delay time parameter, and the number of delay units is an integer, which facilitates the digital circuit to perform counting operations.

[0091] S402 calculates the laser trigger delay by multiplying the edge delay unit number and the potential pulse signal time accuracy parameter.

[0092] Specifically, after calculating the edge delay units, the potential delay control terminal multiplies these units by a preset potential pulse signal timing accuracy parameter to obtain the laser trigger delay. The expression for the laser trigger delay is as follows: The unit can be microseconds, representing the actual physical time the potential delay control terminal needs to wait after detecting the pulse edge of the potential pulse signal. For example, if the delay time parameter is 60 microseconds and the potential pulse signal time accuracy parameter is 0.01 microseconds, then the edge delay units are... The laser triggering delay is Microseconds. By converting the delay time parameter into a number of delay units under the time precision of the potential pulse signal itself, and then multiplying it by the time precision parameter to determine the laser trigger delay, the delay duration is directly related to the timing system of the potential pulse signal. After detecting each pulse edge in the potential pulse signal, the potential delay control terminal uses this laser trigger delay as the waiting time, providing a precise timing reference for the generation of subsequent laser trigger pulse signals.

[0093] This embodiment provides a time-resolved electrochemical Raman spectroscopy method. It calculates the number of edge delay units based on a delay time parameter and a preset potential pulse signal timing accuracy parameter. The operator-set physical delay time is converted into an integer number of steps within the timing accuracy of the potential pulse signal itself. The laser trigger delay is then calculated by multiplying the edge delay units with the potential pulse signal timing accuracy parameter. This establishes a precise temporal correspondence between the pulse edge and the laser trigger pulse within the timing system of the potential pulse signal. This ensures that the delay time calculation is unaffected by software scheduling jitter, guaranteeing that the laser trigger pulse is accurately output at the preset delay time relative to the potential pulse edge. This provides a precise timing control basis for acquiring microsecond-level time-resolved electrochemical Raman spectra.

[0094] In one embodiment, under the event trigger timestamp, the potential pulse signal is transformed based on the laser trigger delay to generate a laser trigger pulse signal, including:

[0095] S501, based on the laser trigger delay, performs delay processing on the potential pulse signal to obtain a delayed potential pulse signal.

[0096] Specifically, after determining the laser trigger delay, the potential delay control terminal performs synchronous delay processing on the potential pulse signal to obtain a delayed potential pulse signal. Synchronous delay processing refers to the potential delay control terminal shifting the complete waveform of the potential pulse signal along the time axis, with the shift duration equal to the physical duration specified by the laser trigger delay. Specifically, the potential delay control terminal internally uses a preset potential pulse signal time accuracy parameter as a clock reference and continuously samples the potential pulse signal. When a pulse edge of the potential pulse signal is detected, it counts according to the edge delay unit based on the clock reference. When the count reaches the edge delay unit, the corresponding potential pulse signal waveform is extracted, thus obtaining a delayed potential pulse signal that has been delayed along the time axis by the duration specified by the laser trigger delay. The delayed potential pulse signal retains the complete waveform characteristics of the potential pulse signal, including the potential amplitude and duration; only the position of the overall waveform on the time axis has been shifted relative to the original potential pulse signal. By performing synchronous delay processing on the potential pulse signal, the timing information of each pulse edge in the potential pulse signal is completely preserved and delayed as a whole, providing a timing-accurate reference signal for subsequent waveform reconstruction.

[0097] S502 performs edge locking on the delayed potential pulse signal to obtain the reference trigger edge signal.

[0098] Specifically, after receiving the delayed potential pulse signal, the potential delay control terminal performs edge-locking processing to obtain a reference trigger edge signal. Edge-locking processing refers to the potential delay control terminal resampling and latching the pulse edges in the delayed potential pulse signal using its own system clock as a time reference, locking the timing information of the edges to the system clock domain. Specifically, the potential delay control terminal uses the system clock as the sampling clock. When it detects an edge transition in the delayed potential pulse signal, it latches and outputs the transition at the next valid edge of the system clock, thus obtaining a reference trigger edge signal synchronized with the system clock and with significantly suppressed jitter. The position of each edge of the reference trigger edge signal on the time axis is determined by the accuracy of the system clock and is independent of jitter that may be introduced during the generation and transmission of the delayed potential pulse signal. After synchronous delay processing, the time position of the delayed potential pulse signal is delayed relative to the potential pulse signal by the laser trigger delay amount, providing a stable and reliable timing reference for subsequent level conversion and pulse width control.

[0099] S503 performs level conversion on the reference trigger edge signal based on the preset laser trigger level amplitude to obtain the standard level trigger edge signal.

[0100] Specifically, after receiving the reference trigger edge signal, the potential delay control terminal performs level conversion on the reference trigger edge signal based on a preset laser trigger level amplitude to obtain a standard level trigger edge signal. The preset laser trigger level amplitude defines the high-level voltage value that the trigger pulse output to the pulsed laser transmitter should reach. This value can be set according to the level requirements of the trigger signal at the pulsed laser transmitter's input port, and can be pre-set and loaded into the potential delay control terminal through the information configuration processing terminal. For example, if the pulsed laser transmitter's trigger input port requires a standard TTL level, the preset laser trigger level amplitude can be set to 5V. The level conversion process refers to the potential delay control terminal internally converting the high-level amplitude of the reference trigger edge signal to the voltage value specified by the preset laser trigger level amplitude, while maintaining the timing position of each edge in the reference trigger edge signal unchanged. The standard level trigger edge signal is the signal obtained after level conversion, whose high-level amplitude matches the input requirements of the pulsed laser transmitter. The timing position of each edge inherits the time accuracy and delay relationship of the reference trigger edge signal, and the high-level amplitude meets the input specifications of the pulsed laser transmitter.

[0101] S504 controls the pulse width of the standard level trigger edge signal according to the preset pulse width parameters to obtain the laser trigger pulse signal.

[0102] Specifically, after receiving the standard level trigger edge signal, the potential delay control terminal controls the pulse width of the standard level trigger edge signal according to preset pulse width parameters, generating a laser trigger pulse signal and outputting it to the pulsed laser transmitter. The preset pulse width parameters define the duration of the high level of each pulse in the laser trigger pulse signal, and can be set according to the minimum width requirement of the trigger pulse from the pulsed laser transmitter. For example, if the pulsed laser transmitter requires a trigger pulse width of not less than 20 nanoseconds, the preset pulse width parameter can be set to 20 nanoseconds. Pulse width control refers to the potential delay control terminal using the rising edge of each edge in the standard level trigger edge signal as the starting point, pulling the output signal high to the high level amplitude of the standard level trigger edge signal, maintaining it at a high level for the duration specified by the preset pulse width parameters, and then pulling it low to zero, thereby converting the standard level trigger edge signal into a laser trigger pulse signal with a standard level amplitude and a specified pulse width. The rising edge of the laser trigger pulse signal is aligned with the rising edge of the standard level trigger edge signal. Its rising edge position relative to the edge of the delayed potential pulse signal remains unchanged. Therefore, the delay time of the rising edge relative to the corresponding pulse edge in the potential pulse signal is strictly equal to the laser trigger delay. The falling edge is determined by a preset pulse width parameter. The level standard and pulse width of the laser trigger pulse signal meet the trigger input specifications of the pulsed laser transmitter, ensuring that each pulse edge in the potential pulse signal has a corresponding laser trigger pulse that precisely corresponds to it, achieving a one-to-one correspondence between the potential pulse and the laser pulse.

[0103] This embodiment provides a time-resolved electrochemical Raman spectroscopy method. By sequentially delaying, edge-locking, level-shifting, and pulse-width-controlled the potential pulse signal, the timing information of each pulse edge in the potential pulse signal is postponed by the laser trigger delay, and then subjected to jitter removal, level normalization, and pulse width shaping. This transforms the signal into a laser trigger pulse signal whose level standard and pulse width both meet the input requirements of the pulsed laser transmitter. This eliminates the impact of edge jitter and level inconsistency introduced during signal transmission on the accuracy of the laser trigger timing, ensuring that the rising edge of the laser trigger pulse signal can be accurately output at a preset delay time relative to the edge of the potential pulse. This achieves a one-to-one correspondence between the potential pulse and the laser pulse, providing a stable and reliable hardware trigger signal for the excitation of microsecond-level time-resolved electrochemical Raman spectroscopy.

[0104] To further illustrate the scheme of the embodiments in this application, a specific example is provided below: This application provides a time-resolved electrochemical Raman spectroscopy method, including the following steps:

[0105] S01, the spectral acquisition device and potential delay control terminal are started through the information configuration processing terminal. The potential waveform data in the potential delay control terminal is set to a square wave signal with a period of 2000, a frequency of 1kHz, and a duty cycle of 1:1. The electrolytic cell, working electrode, and counter electrode in the electrochemical reaction device are configured, with the working electrode and counter electrode set as gold disk microelectrodes with a diameter of 25 micrometers. The solution in the electrolytic cell is a 0.5M potassium chloride solution.

[0106] S02, before formal testing, the surface of the working electrode undergoes electrochemical activation treatment to obtain surface-enhanced Raman scattering effect. The potential waveform data is then processed by the information configuration terminal to control the potential delay, referencing... Figure 3 The potential waveform data was tested with a potential amplitude of 1.2V (relative to the Ag|AgCl reference electrode) and a duration of 10 milliseconds, and a potential amplitude of 0V (relative to the Ag|AgCl reference electrode) and a duration of 50 milliseconds. Simultaneously, the preset delay time parameter was set to 0 microseconds through the information configuration processing terminal, ensuring synchronous output of the laser trigger pulse signal and the potential pulse signal. After receiving the initial trigger signal from the spectral acquisition device, the potential delay control terminal performed event trigger detection on the initial trigger signal to obtain an event trigger timestamp. Under the event trigger timestamp, the potential waveform data was converted into a potential pulse signal and output to the electrochemical reaction device, causing the working electrode surface to cyclically step between 0V and 1.2V. This step process was repeated 50 times to obtain an activated working electrode with surface-enhanced Raman effect.

[0107] S03, After activation, the Raman spectrum of the activated working electrode surface is collected under in-situ conditions as a control. During exposure acquisition, the spectral acquisition device sends an initial trigger signal to the potential delay control terminal. After the potential delay control terminal detects the event trigger, generates the potential pulse signal, and generates the laser trigger pulse signal, the pulsed laser emitter emits a pulsed laser to irradiate the working electrode surface. The spectral acquisition device collects the Raman scattered light from the electrode surface to obtain the activated Raman spectrum. (Reference) Figure 4 The curve of Original represents the Raman spectrum before activation, and the curve of SERS represents the Raman spectrum after activation. The comparison shows that the Raman signal intensity on the working electrode surface is significantly enhanced after activation, indicating that the surface-enhanced Raman scattering effect has been successfully established.

[0108] S04, replace the solution in the electrolytic cell of the electrochemical reactor with an electrolyte solution containing potassium ferrocyanide, and re-preset the potential waveform data through the information configuration processing terminal. This potential waveform data is set as follows: potential amplitude -0.4V (relative to the mercury / mercurous sulfate reference electrode), duration 500 microseconds; potential amplitude 0V, duration 500 microseconds, cycling between -0.4V and 0V. This potential step is used to drive the oxidation reaction of potassium ferrocyanide on the working electrode surface, generating potassium ferrocyanide product. Multiple different delay time parameters are preset through the information configuration processing terminal, which can be sequentially set to 0 microseconds, 100 microseconds, 200 microseconds, 300 microseconds, 400 microseconds, etc.

[0109] S05, for each preset delay time parameter, the following processing is performed: Taking a delay time parameter of 300 microseconds as an example: the spectral acquisition device sends an initial trigger signal to the potential delay control terminal when the exposure acquisition begins; the potential delay control terminal performs event trigger detection on the initial trigger signal and obtains the event trigger timestamp; under the event trigger timestamp, the potential delay control terminal uses the event trigger timestamp as the time starting point, converts the potential waveform data into a potential pulse signal and outputs it to the electrochemical reaction device, applies a potential step from 0V to -0.4V on the working electrode surface, starts the oxidation reaction of potassium ferrocyanide, and simultaneously acquires electrochemical signals and records the current response curve; at the same time, the potential delay control terminal, based on the delay time parameter of 30 microseconds, performs the following processing: The edge delay unit is calculated using 0 microseconds and a preset potential pulse signal timing accuracy parameter. Then, the edge delay unit is multiplied by the potential pulse signal timing accuracy parameter to obtain the laser trigger delay. The potential delay control terminal performs synchronous delay processing on the potential pulse signal based on the laser trigger delay to obtain a delayed potential pulse signal. The delayed potential pulse signal is then sequentially subjected to edge locking, level conversion, and pulse width control to generate a laser trigger pulse signal, which is output to the pulsed laser emitter. The pulsed laser emitter emits a single pulsed laser to irradiate the working electrode surface. The spectral acquisition device collects the Raman scattered light from the electrode surface at this moment to obtain the Raman spectrum and corresponding electrochemical signal of the electrochemical reaction at a delay time of 300 microseconds.

[0110] S06, the Raman spectra under all preset delay time parameters are summarized and analyzed through the information configuration processing terminal. Raman shift is plotted on the x-axis and Raman signal intensity on the y-axis to obtain Raman spectra under different delay times. Based on... Figure 5 It can be observed that at a Raman shift of 2130 cm⁻¹, the Raman peak intensity gradually increases with increasing delay time. This peak is a characteristic Raman peak of potassium ferrocyanide, indicating that potassium ferricyanide is gradually oxidized to potassium ferrocyanide under the action of a potential step. Further, referring to... Figure 6The peak intensity value at a Raman shift of 2130 cm⁻¹ was extracted, and a kinetic curve was plotted with delay time as the x-axis and peak intensity as the y-axis. This visually demonstrates the evolution of potassium ferricyanide product formation on the electrode surface over time. (Refer to...) Figure 7 , Figure 7 To account for the time interval error of the pulsed laser in this specific embodiment, the time interval error jitter of the pulsed laser output by the pulsed laser emitter is 2.407 microseconds. According to the 6σ criterion, the time resolution of the measuring device and method of the present invention is 14.4 microseconds. Simultaneously, the electrochemical signals acquired under different delay time parameters can be analyzed through the information configuration processing terminal to reflect the kinetic process of the electrochemical reaction on the electrode surface from the perspective of electron transfer rate.

[0111] In the aforementioned time-resolved electrochemical Raman spectroscopy method, delay time parameters, potential waveform data, and an initial trigger signal are acquired. The initial trigger signal characterizes the mapping relationship between the spectral acquisition trigger value and the timestamp. Event trigger detection is performed on the initial trigger signal to obtain the event trigger timestamp. Under the event trigger timestamp, the potential waveform data is transformed based on the initial trigger signal to obtain a potential pulse signal. The potential pulse signal is used to indicate the initiation of the electrochemical reaction. Under the event trigger timestamp, the laser trigger delay corresponding to the potential pulse signal is determined based on the delay time parameters. Under the event trigger timestamp, the potential pulse signal is transformed based on the laser trigger delay to generate a laser trigger pulse signal. The laser trigger pulse signal is used to indicate the emission of a pulsed laser. The reaction current signal corresponding to the electrochemical reaction and the Raman spectrum corresponding to the electrochemical reaction under pulsed laser irradiation are acquired. This method achieves precise timing synchronization between the potential pulse signal and the laser trigger pulse signal at the hardware level, eliminating time errors caused by software scheduling delays and mechanical modulation jitter, enabling time resolution at the microsecond level. This effectively captures the spectral information of short-lived intermediate species in electrochemical reactions and improves the tracking accuracy of rapid electrochemical processes.

[0112] It should be understood that although the steps in the flowcharts of the embodiments described above are shown sequentially according to the arrows, these steps are not necessarily executed in the order indicated by the arrows. Unless explicitly stated herein, there is no strict order restriction on the execution of these steps, and they can be executed in other orders. Moreover, at least some steps in the flowcharts of the embodiments described above may include multiple steps or multiple stages. These steps or stages are not necessarily completed at the same time, but can be executed at different times. The execution order of these steps or stages is not necessarily sequential, but can be performed alternately or in turn with other steps or at least some of the steps or stages of other steps.

[0113] Based on the same inventive concept, this application also provides a time-resolved electrochemical Raman testing device for implementing the aforementioned time-resolved electrochemical Raman testing method. The solution provided by this device is similar to the solution described in the above method. Therefore, the specific limitations of one or more embodiments of a time-resolved electrochemical Raman testing device provided below can be found in the above-described limitations of the time-resolved electrochemical Raman testing method, and will not be repeated here.

[0114] In one exemplary embodiment, such as Figure 8 As shown, a time-resolved electrochemical Raman testing device 200 is provided, comprising:

[0115] The data acquisition module 201 is used to acquire delay time parameters, potential waveform data, and initial trigger signal; the initial trigger signal is used to characterize the mapping relationship between the spectral acquisition trigger value and the timestamp.

[0116] The timestamp detection module 202 is used to perform event trigger detection on the initial trigger signal and obtain the event trigger timestamp;

[0117] The reaction signal generation module 203 is used to convert the potential waveform data based on the initial trigger signal at the event trigger timestamp to obtain a potential pulse signal; the potential pulse signal is used to indicate the start of the electrochemical reaction;

[0118] The delay time calculation module 204 is used to determine the laser triggering delay amount corresponding to the potential pulse signal based on the delay time parameter under the event triggering timestamp;

[0119] The laser signal generation module 205 is used to transform the potential pulse signal based on the laser trigger delay amount under the event trigger timestamp to generate a laser trigger pulse signal; wherein, the laser trigger pulse signal is used to indicate the emission of pulsed laser.

[0120] The signal acquisition unit 206 is used to acquire the reaction current signal corresponding to the electrochemical reaction and the Raman spectrum corresponding to the electrochemical reaction under pulsed laser irradiation.

[0121] Furthermore, the timestamp detection module can also be used for:

[0122] The spectral acquisition trigger values ​​in the initial trigger signal that are greater than the preset threshold voltage parameter are marked as candidate trigger values, and the timestamps corresponding to the candidate trigger values ​​are marked as candidate timestamps;

[0123] Extract consecutive candidate timestamps from the initial trigger signal to form a candidate timestamp set;

[0124] Identify the number of candidate timestamps in each candidate timestamp set, obtain the number of consecutive timestamps in each candidate timestamp set, and mark the candidate timestamp set with a number of consecutive timestamps greater than the preset debouncing value as a valid trigger set;

[0125] The earliest timestamp in each valid trigger set is determined as the event trigger timestamp.

[0126] Furthermore, the potential waveform data includes the potential amplitude and the corresponding duration. The response signal generation module can also be used for:

[0127] Using the event trigger timestamp as the starting point, the potential waveform data is transformed to obtain a potential pulse signal, where the expression for the potential pulse signal is:

[0128]

[0129]

[0130] In the formula, It is any timestamp in the potential pulse signal. It is the timestamp in the potential pulse signal The corresponding voltage amplitude, It is the potential amplitude in the potential waveform data. It is the event trigger timestamp. It is the duration corresponding to the potential amplitude in the potential waveform data.

[0131] Furthermore, the delay time calculation module can also be used for:

[0132] Based on the delay time parameter and the preset potential pulse signal time accuracy parameter, the edge delay unit number is calculated, where the expression for the edge delay unit number is:

[0133]

[0134] In the formula, It is the number of edge delay units. It is a delay time parameter. It is a parameter for the timing accuracy of the potential pulse signal. It is a rounding down process;

[0135] The laser trigger delay is obtained by multiplying the edge delay unit number and the potential pulse signal timing accuracy parameter.

[0136] Furthermore, the laser signal generation module can also be used for:

[0137] Based on the laser triggering delay, the potential pulse signal is delayed to obtain a delayed potential pulse signal;

[0138] Edge-locking is performed on the delayed potential pulse signal to obtain the reference trigger edge signal;

[0139] Based on the preset laser trigger level amplitude, the reference trigger edge signal is level-converted to obtain the standard level trigger edge signal;

[0140] The standard level trigger edge signal is controlled by pulse width control according to the preset pulse width parameters to obtain the laser trigger pulse signal.

[0141] In one embodiment, a computer device is provided, including a memory and a processor, the memory storing a computer program, the processor executing the computer program to implement a time-resolved electrochemical Raman testing method as described above.

[0142] In one embodiment, a computer-readable storage medium is provided having a computer program stored thereon, which, when executed by a processor, implements the steps in the above method embodiments.

[0143] For the device embodiments, since they basically correspond to the method embodiments, the relevant parts can be referred to in the description of the method embodiments. The device embodiments described above are merely illustrative. The components described as separate parts may or may not be physically separate, and the components shown as units may or may not be physical units, that is, they may be located in one place or distributed across multiple network units. Some or all of the modules can be selected to achieve the purpose of this disclosure according to actual needs. Those skilled in the art can understand and implement this without creative effort.

[0144] The above-described embodiments are merely illustrative of several implementation methods of the embodiments of this application, and their descriptions are relatively specific and detailed. However, they should not be construed as limiting the scope of the patent application. It should be noted that those skilled in the art can make various modifications and improvements without departing from the concept of the embodiments of this application, and these modifications and improvements all fall within the protection scope of the embodiments of this application.

Claims

1. A time-resolved electrochemical Raman spectroscopy method, characterized in that, The method includes: Acquire delay time parameters, potential waveform data, and initial trigger signal; the initial trigger signal is used to characterize the mapping relationship between the spectral acquisition trigger value and the timestamp; The initial trigger signal is subjected to event trigger detection to obtain the event trigger timestamp; At the event trigger timestamp, the potential waveform data is converted based on the initial trigger signal to obtain a potential pulse signal; the potential pulse signal is used to indicate the initiation of an electrochemical reaction; Under the event trigger timestamp, the laser trigger delay amount corresponding to the potential pulse signal is determined based on the delay time parameter; At the event trigger timestamp, the potential pulse signal is transformed based on the laser trigger delay to generate a laser trigger pulse signal; wherein, the laser trigger pulse signal is used to indicate the emission of pulsed laser. The reaction current signal corresponding to the electrochemical reaction and the Raman spectrum corresponding to the electrochemical reaction under the pulsed laser irradiation are obtained.

2. The method according to claim 1, characterized in that, The step of performing event trigger detection on the initial trigger signal to obtain the event trigger timestamp includes: The spectral acquisition trigger values ​​in the initial trigger signal that are greater than a preset threshold voltage parameter are marked as candidate trigger values, and the timestamps corresponding to the candidate trigger values ​​are marked as candidate timestamps; Extract consecutive candidate timestamps from the initial trigger signal to form a candidate timestamp set; Identify the number of candidate timestamps in each candidate timestamp set, obtain the number of consecutive timestamps in each candidate timestamp set, and mark the candidate timestamp set whose number of consecutive timestamps is greater than a preset debouncing value as a valid trigger set; The earliest timestamp in each of the valid trigger sets is determined as the event trigger timestamp.

3. The method according to claim 1, characterized in that, The potential waveform data includes the potential amplitude and the duration corresponding to the potential amplitude. The step of converting the potential waveform data to obtain a potential pulse signal based on the initial trigger signal at the event trigger timestamp includes: Using the event trigger timestamp as the starting point, the potential waveform data is transformed to obtain the potential pulse signal, wherein the expression of the potential pulse signal is: In the formula, It is any timestamp in the potential pulse signal. It is the timestamp in the potential pulse signal The corresponding voltage amplitude, It is the potential amplitude in the potential waveform data. It is the event trigger timestamp. It is the duration corresponding to the potential amplitude in the potential waveform data.

4. The method according to claim 1, characterized in that, Determining the laser triggering delay amount corresponding to the potential pulse signal based on the delay time parameter under the event triggering timestamp includes: Based on the delay time parameter and the preset potential pulse signal time accuracy parameter, the edge delay unit number is calculated, wherein the expression for the edge delay unit number is: In the formula, It is the number of edge delay units. It is a delay time parameter. It is a parameter for the timing accuracy of the potential pulse signal. It is a rounding down process; The laser trigger delay is obtained by multiplying the edge delay unit number and the potential pulse signal timing accuracy parameter.

5. The method according to claim 1, characterized in that, The step of transforming the potential pulse signal based on the laser trigger delay amount at the event trigger timestamp to generate a laser trigger pulse signal includes: Based on the laser triggering delay, the potential pulse signal is delayed to obtain a delayed potential pulse signal; Edge-locking is performed on the delayed potential pulse signal to obtain the reference trigger edge signal; Based on a preset laser trigger level amplitude, the reference trigger edge signal is level-converted to obtain a standard level trigger edge signal; The standard level trigger edge signal is pulse-width controlled according to preset pulse width parameters to obtain the laser trigger pulse signal.

6. A time-resolved electrochemical Raman spectroscopy apparatus, characterized in that, The device includes: The data acquisition module is used to acquire delay time parameters, potential waveform data, and initial trigger signal; the initial trigger signal is used to characterize the mapping relationship between the spectral acquisition trigger value and the timestamp. The timestamp detection module is used to perform event trigger detection on the initial trigger signal to obtain the event trigger timestamp; A reaction signal generation module is used to convert the potential waveform data based on the initial trigger signal at the event trigger timestamp to obtain a potential pulse signal; the potential pulse signal is used to indicate the initiation of an electrochemical reaction; The delay time calculation module is used to determine the laser triggering delay amount corresponding to the potential pulse signal based on the delay time parameter under the event triggering timestamp; A laser signal generation module is used to transform the potential pulse signal based on the laser trigger delay amount at the event trigger timestamp to generate a laser trigger pulse signal; wherein, the laser trigger pulse signal is used to indicate the emission of pulsed laser. The signal acquisition unit is used to acquire the reaction current signal corresponding to the electrochemical reaction and the Raman spectrum corresponding to the electrochemical reaction under the pulsed laser irradiation.

7. A computer device comprising a memory and a processor, wherein the memory stores a computer program, characterized in that, When the processor executes the computer program, it implements the steps of the method according to any one of claims 1 to 5.

8. A computer-readable storage medium having a computer program stored thereon, characterized in that, When the computer program is executed by a processor, it implements the steps of the method according to any one of claims 1 to 5.

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