CN102789952A - Time-of-flight mass spectrometer electronics reading method based on pulse front edge time measurement and amplitude correction algorithm - Google Patents
Time-of-flight mass spectrometer electronics reading method based on pulse front edge time measurement and amplitude correction algorithm Download PDFInfo
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Abstract
The invention discloses a time-of-flight mass spectrometer electronics reading method which can improve time resolution and a quantitative performance of a time-of-flight mass spectrometer at the same time and is different from an electronics reading scheme of a traditional time-of-flight mass spectrometer by an ADC (Analog to Digital Converter) waveform sampling or a TDC (Time to Digital Converter) pulse time measuring. The pulse front edge time measurement and a pulse forming sampling scheme are combined; the front edge time measured by the TDC is corrected by amplitude information obtained by a middle and low speed ADC for sampling a formed pulse, so that a time resolution effect is obviously improved, and the quantitative performance of an apparatus is improved. According to the reading method, an expensive high-speed ADC (over 1G SPS (samples per second) ) chip is replaced by a pulse forming circuit and the middle and low-speed ADC (about 100M of SPS); a constant fraction discriminator (CFD) circuit in a traditional time-of-flight mass spectrometer reading electronics is replaced by utilizing direct pulse front edge screening, and apparatus cost is reduced when a performance is improved.
Description
Technical field
The invention belongs to the time-of-flight mass spectrometer field; Be particularly related to and a kind of leading-edge pulse time measured and amplitude-time correction algorithm combines; Can improve time-of-flight mass spectrometer time resolution and quantitative performance simultaneously, and the electronics reading method of escapable cost.
Background technology
Time-of-flight mass spectrometer has application widely as a kind of high-end analytical instrument in fields such as environmental monitoring, food security, biology, pharmacy.A most important index estimating the time-of-flight mass spectrometer performance is its resolution, and this resolution index also directly depends on the time measurement precision of instrument read-out electronics except relevant with physical Design, machining.
The read-out electronics of common time-of-flight mass spectrometer, often adopt one of following two kinds of schemes:
First kind is with fast preamplifier the pulse of ion detector output to be amplified earlier, utilizes ADC to the direct waveform sampling of pulse after amplifying then, and pulse arrival time gravity model appoach capable of using draws.The advantage of this scheme is the waveform that can directly measure original pulse, helps cancelling noise, and has improved the quantitative analysis performance and the sensitivity index of instrument.But, therefore, must adopt the high-resolution ADC of high speed if think further to improve the resolution of instrument because pulse arrival time is directly calculated by the ADC sampled data.For example, if make time-of-flight mass spectrometer reach 10000 resolution, the sample rate of ADC will reach 1G SPS at least.And the employing of high sampling rate ADC; Must be accompanied by the problem of high-speed data (greater than 1G Byte/s) buffer memory and transmission; Not only make the electronics design become more complicated, also brought the problem of power consumption and heat radiation, be unfavorable for instrument being developed toward low-power consumption, low cost, portable direction in future.More serious is, is subject to the deficiency of domestic semiconducter process and design experiences, and almost domestic used ADC chip all need be from external import.And the ADC chip of high sampling rate not only costs an arm and a leg, and more owing to can be applicable to key areas such as national defence, often when buying, faces the problem of embargo.Therefore, depend merely on the electronics readout scheme that ADC carries out waveform sampling, because the restriction of the price of high-speed ADC, buying, R&D costs must limit the autonomous industrialization of high-resolution time-of-flight mass spectrometer if adopt.
Second kind is that the analog signal of with constant proportion timing circuit (CFD) ion detector being exported earlier is converted into digit pulse, and sharp then TDC directly measures the time of advent of pulse.Adopt current domestic mature technology, be easier to realize that time resolution is better than the TDC of 1ns, therefore adopt second kind of scheme, under the prerequisite that has realized higher time performance, saved ADC.But shortcoming be TDC as digital device, can only learn having or not of certain pulse of ion source output constantly, and write down its time of advent, and can't measure the shape or the amplitude (wherein comprising ion populations information) of pulse.Even for example have the identical ion of two or more mass-to-charge ratioes at short notice (for example 1ns) arrive ion detector simultaneously, the counting of TDC still is 1, thus the quantitative performance and the sensitivity that cause instrument are not as first kind of scheme.Another shortcoming of scheme two is then from the CFD circuit.The use of CFD; Though can eliminate the time error that the amplitude autokinetic effect brings; But it need carry out simulated modulation such as anti-phase amplification, delay, summation to the high-speed pulse signal of ion detector output, converts digit pulse to through high-speed comparator again, just delivers to TDC then and carries out time measurement.And each grade simulated modulation circuit all means the loss of signal bandwidth and signal to noise ratio, and the introducing of new time error.Along with the progress of digital technology in recent years; Utilize TDC can realize increasingly high time precision (TDC that realizes such as the commercial fpga chip of the employing of latest domestic can reach the time resolution that is better than 100ps); Therefore; The time figureization of pulse is shifted to an earlier date as far as possible, the simulation process process is simplified as far as possible, could effectively bring into play the precision advantage of TDC.Thereby CFD circuit in second scheme, can form restriction to the performance of high-end flight mass spectrum instrument.
The read-out electronics of existing time-of-flight mass spectrometer basically all is based on above-mentioned dual mode, though can realize function to a certain extent, the shortcoming that can not be ignored is arranged all, has limited the application of time-of-flight mass spectrometer, and autonomous industrialization.
Summary of the invention
The object of the invention one is; To having the deficiency that time-of-flight mass spectrometer is depended merely on ADC or depended merely on the TDC readout scheme now; Propose a kind of new departure that the leading-edge pulse time measurement is combined with the pulse shaping sampling, low speed ADC and TDC during it adopts simultaneously are when improving instrument performance; Simplify reading circuit structure, reduced cost.
The object of the invention two is, on the basis of purpose one, has proposed a kind of pulse amplitude information of in the time-of-flight mass spectrometer read-out system, utilizing, the method that TDC leading edge time measurement result is carried out online correction.Adopt this method can overcome the amplitude-time autokinetic effect of lead edge timing, improve final time measurement precision.
For achieving the goal one, the present invention proposes a kind of new departure that the leading-edge pulse time measurement is combined with the pulse shaping sampling, and described treatment step is:
Step a at first will utilize preamplifier to amplify from the detector signal of ion detector (normally microchannel plate), and the signal after will amplifying is then delivered to the electronics data collecting card through radio frequency cable.
Step b behind the signal arrival electronics data collecting card of preceding putting, carries out amplifying at 1: 1 through analogue buffer (Buffer) earlier;
Step c is divided into two-way output with the signal after the amplification among the step b, and one the road earlier through forming circuit, and low speed ADC carries out waveform sampling in delivering to then, and another Lu Xianjing comparator converts digit pulse to, delivers to TDC then.Wherein, the about 100M SPS of the sample rate of middling speed ADC, the time constant of forming circuit is about 100ns.The temporal resolution of the TDC that is adopted is about 500ps or higher.
Steps d, the data of ADC and TDC are sent among the DSP on the data collecting card and handle, and result is delivered in the PC through usb bus.
For achieving the goal two, the present invention proposes a kind ofly at time-of-flight mass spectrometer read-out system amplitude time correction algorithm, described step is:
Step e; Under the time-of-flight mass spectrometer typical work condition; To typical sample, utilize above-mentioned leading-edge pulse time to measure the electronics reading method that combines with the pulse shaping sampling, measure the leading edge time of microchannel plate output signal and the Wave data behind the pulse shaping.Utilize the method for digital peak-seeking, Wave data is analyzed, obtain the peak amplitude of shaped pulse, then leading edge time is preserved into file with amplitude data.
Step f analyzes the data file, finds a certain typical ion peak position in the sample, and its pairing many group time datas and amplitude data are carried out match, must appear the relation curve of threshold time and pulse amplitude, forms and revises look-up table.
Step g writes this lookup file in the Flash chip on the data collecting card, is loaded into automatically among the program RAM after each system powers on.
Step h after ADC samples signal waveform, carries out digital peak-seeking in DSP, to this peak value, in look-up table, find the time corresponding correction value then.On the numerical value that TDC records, add this correction value then.
The present invention compared with prior art, its advantage is:
1) guaranteeing regularly and under the prerequisite of quantitative performance, utilizing middling speed ADC chip to substitute the high-speed ADC chip in the existing high-end time-of-flight mass spectrometer, both reduces cost, simplified circuit design again, reduced power consumption.The embargo problem that has been faced when having avoided the buying of high-speed ADC chip simultaneously helps the production domesticization of high-end time-of-flight mass spectrometer.
2) utilize direct lead edge timing mode to substitute the constant proportion timing mode in traditional time-of-flight mass spectrometer readout scheme, simplified the analog front end circuit design.Simultaneously, because the application of amplitude correction algorithm, compensated time that lead edge timing causes error of moving about, thereby made full use of digitlization advantage and the potentiality of TDC, and helped followingly, made instrument toward high extreme direction upgrading along with the TDC development of technology.
3) in DSP, realize real-time searching table correction algorithm, guaranteed the real-time analysis and the handling property of instrument, shortened the analysis time of sample.
Description of drawings
Fig. 1 system construction drawing
Fig. 2 ADC process chart that combines with TDC
Fig. 3 amplitude-time is revised flow chart
Pulse amplitude that Fig. 4 emulation obtains and mistake threshold time relation curve
Electronics time resolution before and after the correction that Fig. 5 emulation obtains
Embodiment
To combine the accompanying drawing in the embodiment of the invention below, the technical scheme in the embodiment of the invention is carried out clear, intactly description, obviously, described embodiment only is a part of embodiment of the present invention, rather than whole embodiment.Based on embodiments of the invention, the every other embodiment that those of ordinary skills are obtained under the prerequisite of not making creative work belongs to the scope that the present invention protects.
As shown in Figure 1, be system configuration sketch map of the present invention, comprise following a few part in the shown system: MCP is a detector signal; Buffer is the analogue buffer module; Shaper is the forming circuit module; ADC is the analog to digital converter module; TDC time-to-digit converter module;
The object of the invention one is; To having the deficiency that time-of-flight mass spectrometer is depended merely on ADC or depended merely on the TDC readout scheme now; Propose a kind of new departure that the leading-edge pulse time measurement is combined with the pulse shaping sampling, low speed ADC and TDC during it adopts simultaneously are when improving instrument performance; Simplify reading circuit structure, reduced cost.
The object of the invention two is, on purpose one basis, has proposed a kind of pulse amplitude information of in the time-of-flight mass spectrometer read-out system, utilizing, the method that TDC leading edge time measurement result is carried out online correction.Adopt this method can eliminate the amplitude autokinetic effect of lead edge timing, improve the time measurement precision.
For achieving the goal one, the concrete steps of enforcement can be summarized as follows:
From the consideration of simplifying circuit design, improving temporal resolution, it is regularly more excellent than adopting constant proportion to adopt the forward position examination.But it is exactly the time autokinetic effect that a required problem that overcomes is screened in the forward position, and promptly the pulse signal of different amplitudes is crossed the threshold time difference, can the life period error after screening through the forward position.Have only this error is revised, just can embody the advantage of forward position examination and high accuracy TDC.Second purpose of the present invention is the shape information of utilizing ADC to adopt, and the leading edge time information that TDC measures is revised, and the error with subduction time autokinetic effect truly improves final time resolution.
For achieving the goal two, the concrete steps of enforcement can be summarized as follows:
Fig. 4 is according to above-mentioned implementation step, utilizes the emulation of Matlab software modeling, MCP pulse amplitude that obtains and mistake threshold time relation curve.The emulation experiment condition of setting: the TDC time resolution is 100ps; The threshold value that screen in the forward position is 200mV; The amplitude measurement overall error that is caused by pulse shaping, waveform sampling and digital peak-seeking process is the even distribution in+/-5% scope; The about 3ns of MCP pulse front edge after preposition amplification, the MCP pulse amplitude is the even distribution of 220mV～1200mV, the random sampling number of times is 1000 times.
The sampled point that " samples " among Fig. 4 obtains for emulation, " Fit curve " are according to 1000 sampled points, carry out 5 order polynomial matches, the fair curve that obtains.Can find out from the distribution of sampled point, cross threshold time and be with the increase of pulse amplitude and reduce trend, and along with amplitude increases to a certain degree, this reduce trend and also slows down gradually, effect that Here it is so-called " time moves about ".To the sampled point of big statistic, the amplitude-time that the obtains matched curve of moving about generates with the look-up table of pulse amplitude numerical value as the addressing address then, promptly can be used for the TDC data are revised, and with the make-up time error of moving about, improves final time resolution.
Fig. 5 utilizes the matched curve among Fig. 4 to generate look-up table for adopting same Matlab modeling and simulating method, the MCP leading edge time data that TDC records is revised the time explanation result before and after the emulation that obtains.Carried out 1000 sampling equally, the about 0.23ns of electronics time resolution (root-mean-square value) before obtaining revising, the about 0.03ns of revised electronics time resolution (root-mean-square value), effect is remarkable, proves that this modification method is fully feasible.
Through experiment with analyze, the present invention compared with prior art, it is advantageous that following some:
1) guaranteeing regularly and under the prerequisite of quantitative performance, utilizing middling speed ADC chip to substitute the high-speed ADC chip in the existing high-end time-of-flight mass spectrometer, both reduces cost, simplified circuit design again, reduced power consumption.The embargo problem that has been faced when having avoided the buying of high-speed ADC chip simultaneously helps the production domesticization of high-end time-of-flight mass spectrometer.
2) utilize direct lead edge timing mode to substitute the constant proportion timing mode in traditional time-of-flight mass spectrometer readout scheme, simplified the analog front end circuit design.Simultaneously, because the application of amplitude correction algorithm, compensated time that lead edge timing causes error of moving about, thereby made full use of digitlization advantage and the potentiality of TDC, and helped followingly, made instrument toward high extreme direction upgrading along with the TDC development of technology.
3) in DSP, realize real-time searching table correction algorithm, guaranteed the real-time analysis and the handling property of instrument, shortened the analysis time of sample.
The above description of this invention is illustrative, and nonrestrictive, and those skilled in the art is understood, and within spirit that claim limits and scope, can carry out many modifications, variation or equivalence to it, but they will fall in protection scope of the present invention all.
Claims (9)
1. measure the time-of-flight mass spectrometer electronics reading method with the amplitude correction algorithm based on leading-edge pulse time for one kind, it mainly comprises: with the method that leading-edge pulse time is measured and pulse shaping is sampled the method that combines and the time measurement result carried out online correction.
Above-mentioned that the leading-edge pulse time measurement is following with the method step that the pulse shaping sampling combines:
Step a at first will utilize preamplifier to amplify from the detector signal of ion detector (normally microchannel plate), and the signal after will amplifying is then delivered to the electronics data collecting card through radio frequency cable.
Step b behind the signal arrival electronics data collecting card of preceding putting, carries out amplifying at 1: 1 through analogue buffer (Buffer) earlier;
Step c is divided into two-way output with the signal after the amplification among the step b, and one the road earlier through forming circuit, and low speed ADC carries out waveform sampling in delivering to then, and another Lu Xianjing comparator (also being referred to as discriminator) converts digit pulse to, delivers to TDC then.Wherein, the sample rate of middling speed ADC is (for example 100M SPS) below the 1G SPS, and the time constant of forming circuit is tens of to hundreds of nanoseconds (for example 100ns).The temporal resolution of the TDC that is adopted is about tens of to hundreds of psecs (for example 100ps).
Steps d, the data of ADC and TDC are sent among the DSP on the data collecting card and handle, and result is delivered in the PC through usb bus.
The method step that measurement result is carried out online correction is following:
Step e under the time-of-flight mass spectrometer typical work condition, to typical sample, utilizes above-mentioned leading-edge pulse time to measure the electronics reading method that combines with the pulse shaping sampling, measures the leading edge time and the impulse waveform of microchannel plate output signal.Utilize the method for digital peak-seeking, Wave data is analyzed, obtain the peak amplitude of shaped pulse, then leading edge time is preserved into file with amplitude data.
Step f analyzes the data file, finds a certain typical ion peak position time corresponding and amplitude data in the sample, and multi-group data is carried out match, must appear the relation curve of threshold time and pulse amplitude, forms to revise look-up table.
Step g writes this lookup file in the Flash chip on the data collecting card, is loaded into automatically among the program RAM after each system powers on.
Step h after ADC samples signal waveform, carries out digital peak-seeking in DSP, to this peak value, in the RAM look-up table, find the time corresponding correction value then.On the numerical value that TDC records, add this correction value then.
2. the time-of-flight mass spectrometer electronics reading method based on leading-edge pulse time measurement and amplitude correction algorithm as claimed in claim 1; It is characterized in that; Among the said step c, the reading method that has adopted ADC and TDC to combine, and take all factors into consideration the demand of cost and performance; Avoid adopting high-speed ADC, but adopted the middling speed ADC below the sample rate 1G SPS.
3. the time-of-flight mass spectrometer electronics reading method based on leading-edge pulse time measurement and amplitude correction algorithm as claimed in claim 1; It is characterized in that; Among the said step c, before the ADC waveform sampling, earlier ion detector is exported signal and directly deliver to forming circuit then through preposition amplification.The effect of this forming circuit is that narrow pulse signal is at a high speed become an accurate Gaussian waveform that the forward position is slow slightly, makes it to be more suitable for middling speed ADC sampling.Accurate gaussian signal peak value through after being shaped is directly proportional with the amplitude of original waveform, therefore after sampling, does not lose the amplitude information of primary signal, thereby has guaranteed the quantitative analysis ability of spectrometer.
4. the time-of-flight mass spectrometer electronics reading method based on leading-edge pulse time measurement and amplitude correction algorithm as claimed in claim 1; It is characterized in that; In the said steps d, in DSP through the method for digital peak-seeking, the peak value of the accurate Gaussian pulse after obtaining being shaped.
5. the time-of-flight mass spectrometer electronics reading method based on leading-edge pulse time measurement and amplitude correction algorithm as claimed in claim 1; It is characterized in that; Directly adopt high-speed comparator to replace traditional CFD; After screen in the forward position, convert input pulse to digital signal, deliver to TDC then and measure.The forward position discriminator circuit is simpler than constant proportion principle regularly, and it is easier to realize, thereby has guaranteed that the temporal information that signal pulse comprised do not suffer a loss, and is easy to expand, to satisfy the demand of following mass spectrometer performance upgrade.
6. the time-of-flight mass spectrometer electronics reading method based on leading-edge pulse time measurement and amplitude correction algorithm as claimed in claim 1; It is characterized in that; Among the said step f, propose a certain ion peak position is recorded many groups amplitude-time data, carry out match then; Draw the relation curve that threshold time and amplitude are crossed in pulse, set up the digital search table that is used for amplitude-time correction.
7. the time-of-flight mass spectrometer electronics reading method based on leading-edge pulse time measurement and amplitude correction algorithm as claimed in claim 1 is characterized in that the digital search table in the said step g possesses the automatic value-added tax function that powers on.
8. the time-of-flight mass spectrometer electronics reading method based on leading-edge pulse time measurement and amplitude correction algorithm as claimed in claim 1 is characterized in that, among the said step h, through look-up table the TDC data is carried out online correction.
9. the time-of-flight mass spectrometer electronics reading method based on leading-edge pulse time measurement and amplitude correction algorithm as claimed in claim 2; It is characterized in that; Guaranteeing regularly and under the prerequisite of quantitative performance, utilizing middling speed ADC chip to substitute the high-speed ADC chip in the existing high-end time-of-flight mass spectrometer.
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| CN104078302B (en) * | 2014-07-15 | 2017-01-11 | 江苏天瑞仪器股份有限公司 | Detector signal processing component capable of being adjusted by user and applicable to mass spectrometer |
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| CN109171787A (en) * | 2018-08-27 | 2019-01-11 | 苏州瑞派宁科技有限公司 | The method of sampling, device and the computer program medium of pulse signal |
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| CN109581399A (en) * | 2018-12-29 | 2019-04-05 | 西南技术物理研究所 | A kind of Larger Dynamic range Centimeter Level precision laser distance measuring method |
| CN113406181A (en) * | 2021-06-03 | 2021-09-17 | 中山大学 | Method, system, device and storage medium for measuring chemical ionization reaction time |
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