CN108776166A - A kind of spectrum modulation Hadamard transform ionic migration spectrometer - Google Patents
A kind of spectrum modulation Hadamard transform ionic migration spectrometer Download PDFInfo
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Abstract
The present invention proposes that a kind of spectrum modulates Hadamard transform ionic migration spectrometer, including ionization source, reaction zone, ion gate, spectrum modulation Hadamard transform door control unit, migration area, ion signal probe unit and spectrum modulation Hadamard transformed signals processing unit.Spectrum modulation Hadamard transform door control unit generates Hadamard transform ion gate sequence by pseudo-random sequence generator module first, then it is converted into spectrum modulation Hadamard transform ion through spectrum modulation Hadamard code modulation module and gates pulse train, access ion gate both ends after boosted module conversion, realize the spectrum modulation Hadamard transform control to ion gate, obtained spectrum modulation Hadamard transform Ion transfer stack spectral obtains spectrum modulation Hadamard transform Ion transfer reduction spectrum through reading, handling and restore.The present invention can eliminate phenomena such as ghost peak, distorted signals and strength reduction of conventional Hadamard transform ion mobility spectrometry, improve the signal-to-noise ratio of Hadamard transform ion mobility spectrometry, improve the analysis and identification ability of ion mobility spectrometry.
Description
Technical field
The invention belongs to analytical instrument and detection field, and in particular to a kind of spectrum modulation Hadamard transform ion mobility spectrometry
Instrument.
Background technology
Signal-to-noise ratio and sensitivity are to weigh the important technology index of ionic migration spectrum detection performance, 2006, scientific research personnel
Hadamard transform multiplexing technique is introduced ion mobility spectrometry for the first time, has developed Hadamard transform Ion mobility spectrometry, it should
Technology improves ion mobility spectrometry using the opening and closing of the ion gate of Hadamard transform control module control ion mobility spectrometry
Signal dutyfactor, that is, improve ion service efficiency, the signal-to-noise ratio of ion mobility spectrometry made to improve 2-10 times.
However due to modulation defect etc., there are many ghost peaks and letters in conventional Hadamard transform Ion transfer spectrum signal
Number distortion phenomenon, ion signal intensity are also substantially reduced than conventional ion mobility spectrum.Ghost peak and distorted signals phenomenon not only give object
The analysis detection of matter brings interference, also results in the reduction of ion mobility spectrometry signal-to-noise ratio, influences the property of Hadamard transform ion mobility spectrometry
Energy.
Invention content
The technical problem to be solved in the present invention is：For Hadamard transform Ion transfer spectrum signal, there are many ghost peaks, letters
Number distortion and phenomena such as ion signal strength reduction, proposes a kind of spectrum modulation Hadamard transform ionic migration spectrometer, that is, passes through spectrum
The on and off of Hadamard transform door control unit control ion mobility spectrometry ion gate is modulated, the Hadamard transform ion for obtaining separation moves
Stack spectral is moved, recycles spectrum modulation Hadamard transformed signals processing unit to be read out, handle to these stack spectrals and reduction, obtains
Modulation Hadamard transform Ion transfer reduction spectrum must be composed, the ghost peak and letter in conventional Hadamard transform ion mobility spectrometry are effectively eliminated
Phenomena such as number distortion, ion signal intensity, the final signal-to-noise ratio for improving ion mobility spectrometry and sensitivity are improved, Hadamard is promoted and becomes
Analysis and the recognition capability for changing ion mobility spectrometry, further widen the application range of the technology.
The present invention solve the technical solution that uses of above-mentioned technical problem for：A kind of spectrum modulation Hadamard transform ion mobility spectrometry
Instrument, it is by ionization source, reaction zone, ion gate, spectrum modulation Hadamard transform door control unit, migration area, ion signal probe unit
With spectrum modulation Hadamard transformed signals processing unit composition；Wherein, the reactive ion that ionization source generates enters under electric field action
After reaction zone, and ion-molecule reaction occurs for detection substance, obtains product ion, and before converging in ion gate；Spectrum modulation hada
Hadamard transform door control unit generates spectrum modulation Hadamard transform gate sequence, and reconvert passes through conducting wire and ion at gating pulse
The spectrum modulation multiplexing control to ion gate is realized in door connection；Ion in reaction zone modulates multiplexing control in this spectrum
With impulse form by ion gate under molding formula, into migration area, ion signal probe unit is reached under electric field action, is realized
The detection of ion signal obtains spectrum modulation Hadamard transform Ion transfer stack spectral, and at spectrum modulation Hadamard transformed signals
Unit is managed through data processing, transformation and reduction, obtains spectrum modulation Hadamard transform Ion transfer reduction spectrum；Hada is modulated using spectrum
Hadamard transform Ion mobility spectrometry, the multichannel quasi-molecular ions that can be effectively isolated in conventional Hadamard transform ion mobility spectrometry are eliminated normal
Advise Hadamard multiplexing technique in modulation defect, solve signal in ghost peak and distortion phenomenon, improve Hadamard transform from
The signal-to-noise ratio and qualitative analysis ability of sub- migration spectrum.
Further, the ionization source can be photo-ionisation ionization source, radioactive ionization gauge source, corona discharge ionization source, etc.
Gas ions ionization source, electron spray ionisation source or film-type ionization source.
Further, the ion gate can be Bradbury-Nielson types, can also be Tyndall-Powell
Type ion gate.
Further, spectrum modulation Hadamard transform door control unit is modulated by pseudo-random sequence generator module, spectrum
Hadamard code modulation module and boost module composition, pseudo-random sequence generator module first generate conventional Hadamard transform ion
Gate sequence obtains spectrum modulation Hadamard transform ion gate pulse train, most afterwards through rising after composing modulating-coding resume module
Die block completes conversion of the Transistor-Transistor Logic level to high level, and the spectrum tune to ion gate is realized at transformed level access ion gate both ends
System control.
Further, it after ion signal probe unit detects ion signal, obtains spectrum modulation Hadamard transform ion and moves
Stack spectral is moved, and is sent into spectrum modulation Hadamard transformed signals processing unit and is further processed.
Further, the spectrum modulates high-speed data of the Hadamard transformed signals processing unit by synchronized-pulse control
Capture card completes acquisition and the A/D conversions of multichannel spectrum modulation Hadamard transform Ion transfer stack spectral, recycles upper computer software
Reading, processing and the reduction of data are completed, spectrum modulation Hadamard transform ion mobility spectrometry is obtained.
In one embodiment of the invention, the ionization source, using corona discharge ionization source, the ion of detection is
Reactive ion.
In one embodiment of the invention, the ion gate, using Bradbury-Nielson type ion gates, from
Cervical orifice of uterus is connected with spectrum modulation Hadamard transform door control unit.
In one embodiment of the invention, the spectrum modulates Hadamard transform door control unit by pseudo-random sequence generator
Module, spectrum modulation Hadamard code modulation module and boost module composition complete the spectrum modulation multiplexing control of ion gate.
In one embodiment of the invention, pseudo-random sequence generator is completed by FPGA, in FPGA, first by
Verilog softwares construct one 8 longest linear feedback shift registers, to obtain 255 pseudo-random sequences, wherein
Contain 128 1,127 0；Then initial pseudo-random sequence is become using spectrum modulating coder to compose modulating-coding sequence, most
Boost module is utilized afterwards, obtained spectrum modulating-coding sequence (Transistor-Transistor Logic level), which is converted into ion, gates pulse voltage signal, to
Realize the spectrum modulation control of ion signal.
In one embodiment of the invention, it is folded to obtain spectrum modulation ion mobility spectrometry for the ion signal probe unit
Add spectrum, and is transferred to spectrum modulation Hadamard signal processing unit and is further processed.
In one embodiment of the invention, the spectrum modulation Hadamard transform processing unit, which is first sent to collection terminal, acquires
Beginning and end lock-out pulse completes spectrum modulation Hadamard transform multichannel by the high-speed data acquisition card under synchronized-pulse control
Data acquisition, amplification, A/D conversions and the inversion process of stack spectral.
The advantages of the present invention over the prior art are that：
(1) present invention is a kind of spectrum modulation Hadamard transform ionic migration spectrometer, is produced by the programming software of FPGA first
Modulation sequence of the pseudo-random number sequence code of raw certain digit as Hadamard transform, the sequence are compiled through composing modulating-coding module
Spectrum modulation Hadamard gating pulse sequence is obtained after code, then is completed after boosting by boost module, and ion gate both ends are applied to.
(2) present invention controls the ion gate of ionic migration spectrometer using spectrum modulation Hadamard transform door control unit, making
Ionic migration spectrometer energy effective guarantee high ion flux, improves signal dutyfactor.
(3) present invention controls the ion gate of ionic migration spectrometer using spectrum modulation Hadamard transform door control unit, making
Ionic migration spectrometer can also eliminate ghost peak and distorted signals phenomenon in conventional Hadamard transform ion mobility spectrometry, improve hada
The signal-to-noise ratio detection sensitivity of Hadamard transform ion mobility spectrometry.
Description of the drawings
Fig. 1 is that the spectrum of the present invention modulates Hadamard ion mobility spectrometer configuration schematic diagram.
Fig. 2 is that the gate sequence of conventional Hadamard transform ionic migration spectrometer and gating pulse, stack spectral are composed with reduction,
In, Fig. 2 (a) is the gate sequence and gating pulse of conventional Hadamard transform ionic migration spectrometer, and Fig. 2 (b) is 255 pseudorandoms
Conventional Hadamard transform ion mobility spectrometry stack spectral under Serial No., Fig. 2 (c) are the routine under 255 pseudo-random number sequences
Hadamard transform ion mobility spectrometry reduction spectrum.
Fig. 3 is that the gate sequence of spectrum modulation Hadamard transform ionic migration spectrometer and gating pulse, stack spectral are composed with reduction,
Wherein, Fig. 3 (a) is the gate sequence and gating pulse of spectrum modulation Hadamard transform ionic migration spectrometer, and Fig. 3 (b) is 255 puppets
The conventional Hadamard transform ion mobility spectrometry stack spectral of spectrum modulation under random number sequences, Fig. 3 (c) are 255 pseudorandom number sequences
Spectrum modulation Hadamard transform ion mobility spectrometry reduction spectrum under row.
Reference numeral meaning is in figure：1 is ionization source, and 2 be reaction zone, and 3 be ion gate, and 4 be spectrum modulation Hadamard transform
Gate is single, and 5 be migration area, and 6 be ion signal probe unit, and 7 be spectrum modulation Hadamard transformed signals processing unit, 8 for it is pseudo- with
Machine Sequencer block, 9 be spectrum modulation Hadamard code modulation module, and 10 be boost module.
Specific implementation mode
Below in conjunction with attached drawing, to the specific reality of the present invention by taking 255 spectrum modulation Hadamard transform ionic migration spectrometers as an example
The mode of applying is described in detail.
As shown in Figure 1, a kind of spectrum modulates Hadamard ionic migration spectrometer, it include ionization source 1, reaction zone 2, ion gate 3,
Spectrum modulation Hadamard transform door control unit 4, migration area 5, ion signal probe unit 6 and spectrum modulation Hadamard transformed signals processing
Unit 7 forms.Ionization source 1 generate reactive ion under electric field action enter reaction zone 2, occur herein with tested substance from
Product ion is obtained by the reaction in son-molecule, and before converging in ion gate 3.Spectrum modulation Hadamard transform door control unit 4 by conducting wire and
Ion gate 3 connects, and the pseudo-random sequence generator module of spectrum modulation Hadamard transform door control unit 4 first generates conventional Hadamard
Ion gate sequence is converted, spectrum modulation Hadamard transform ion gate pulse train is obtained after composing modulating-coding resume module,
Last boosted module completes the conversion that Transistor-Transistor Logic level arrives high level, 3 both ends of transformed level access ion gate, realization to from
The spectrum modulation control of cervical orifice of uterus 3.Ion in reaction zone 2 is in the case where this spectrum modulates multiplexing control control model with impulse form
By ion gate 3, into migration area 5, ion signal probe unit 6 is reached under electric field action, realizes the detection of ion signal,
In the case where this spectrum modulates ion gate-mode, ion, by forming the ion packet of isolation after ion gate 3, is being moved with impulse form
It moves under electric field action, ion packet is migrated to ion signal probe unit 6, is converted through Current amplifier, acquisition, A/D, and spectrum modulation is formed
Hadamard transform Ion transfer be superimposed spectrum signal, the signal again through spectrum modulation Hadamard transformed signals processing unit read after again into
The inverse Hadamard transform of row is handled and is restored, and obtains spectrum modulation Hadamard transform Ion transfer reduction spectrum.It can be effective using this method
The ghost peak and distorted signals phenomenon for eliminating conventional Hadamard transform ion mobility spectrometry, improve ion signal intensity, obtain signal-to-noise ratio
Hadamard transform ion mobility spectrometry is modulated with the higher spectrum of sensitivity.
For traditional Hadamard transform ionic migration spectrometer, as shown in Fig. 2 (a), when the pseudorandom sequence of control ion gate
Include 128 1 and 127 0 when being classified as 255, in this sequence；Wherein each " 1 " indicates that ion gate pulse is high level,
Ion gate is opened once, i.e., ion enters migration area with impulse form by ion gate, and each " 0 " then indicates ion gate pulse
For low level, ion gate is closed once, and ion stream is ended.255 pseudo-random sequences are common to be taken the form of
" 110111011100101 ... ", that is, there are multiple " 1 " continuous the case where occurring in sequence, when ion gate sequence is
When multiple company " 1 ", ion gate can keep prolonged opening state, obtain the Hadamard transform Ion transfer as shown in Fig. 2 (b)
The linear superposition at superposed signal peak (multiplex signal) and nonideal, multiple independent quasi-molecular ions.But in subsequent signal
Processing stage, and ideal superposed signal data processing is treated as at this nonideal superposed signal peak, it obtains such as Fig. 2 (c) institutes
The Hadamard transform Ion transfer reduction spectrum shown.It is seen that in addition to the reaction that signal strength is 909 at 10.40ms
Outside quasi-molecular ions, three more apparent ghost peaks are found at 3.85ms, 20.25ms and 29.95ms.According to ion mobility spectrometry noise
The calculation formula of ratio：
Wherein SNR is signal-to-noise ratio, and H is the intensity at ion signal peak, and σ is the average deviation of baseline, can calculate conventional hada
Hadamard transform ion mobility spectrometry signal-to-noise ratio is 36.
As shown in Fig. 3 (a), spectrum modulation Hadamard transform ionic migration spectrometer and traditional Hadamard transform ionic migration spectrometer
Difference lies in：Spectrum modulation Hadamard transform ionic migration spectrometer generates 255 pseudorandoms by pseudo-random sequence generator first
Conventional 255 pseudo-random sequences are isolated into spectrum modulation Hadamard multiplexing gate by pulse train through composing modulating-coding module
Pulse train is respectively inserted into one " 0 " before and after each " 1 " and " 0 " so that continuous " 1 " is isolated, then boosted mould
TTL type gating pulse sequences are boosted and gate pulse train at ion by block, are finally accessed ion gate both ends, are completed to ion
The spectrum modulation Hadamard of door multiplexes coding-control.In this control model, as shown in Fig. 3 (b), each sequence " 1 "
Generate a width independent migration spectral peak.In 255 gate sequences, obtained superposed signal peak (multiplex signal) is exactly
The linear superposition of multiple independent ion spectral peaks most reads afterwards through signal processing unit, takes and obtained such as Fig. 3 with after inversion process
(c) Ion transfer reduction spectrum spectrum shown in.As can be seen from Figure 3, spectrum modulation Hadamard transform ion mobility spectrometry detects anti-
Quasi-molecular ions is answered to be still at 10.40ms, signal strength 1565 is conventional Hadamard transform ion mobility spectrometry signal strength
1.72 times, ghost peak eliminate, background noise be improved significantly.Using formula (1), spectrum modulation Hadamard transform ion can be calculated and moved
The signal-to-noise ratio for moving spectrum is 247, is 6.86 times of conventional Hadamard transform ion mobility spectrometry signal-to-noise ratio, realizes and further increase Kazakhstan
Up to the function of Hadamard transform ion mobility spectrometry signal-to-noise ratio and ion signal intensity, the analysis of Hadamard transform ion mobility spectrometry is improved
Recognition capability.
Above example is not intended to limit the scope of the present invention just for the sake of the description purpose of the present invention.The present invention's
Range is defined by the following claims.The various equivalent alterations and modifications for not departing from spirit and principles of the present invention and making,
It should cover within the scope of the present invention.
Description of the invention does not elaborate and partly belongs to techniques well known.
Claims (6)
1. a kind of spectrum modulates Hadamard transform ionic migration spectrometer, it is characterised in that：It by ionization source (1), reaction zone (2), from
Cervical orifice of uterus (3), spectrum modulation Hadamard transform door control unit (4), migration area (5), ion signal probe unit (6) spectrum modulation Hadamard
Signal processing unit (7) is converted to form；Wherein, the reactive ion that ionization source (1) generates enters reaction zone (2) under electric field action
Afterwards, and ion-molecule reaction occurs for detection substance, obtains product ion, and before converging in ion gate (3)；Spectrum modulation Hadamard
It converts door control unit (4) and generates spectrum modulation Hadamard transform gate sequence, reconvert passes through conducting wire and ion at gating pulse
The spectrum modulation multiplexing control to ion gate is realized in door (3) connection；Ion in reaction zone is modulated in this spectrum to be multiplexed
With impulse form by ion gate (3) under control model, into migration area (5), ion signal detection is reached under electric field action
Unit (6), realizes the detection of ion signal, obtains spectrum modulation Hadamard transform Ion transfer stack spectral, and modulate hada in spectrum
Hadamard transform signal processing unit (7) obtains spectrum modulation Hadamard transform Ion transfer reduction through data processing, transformation and reduction
Spectrum；Hadamard transform Ion mobility spectrometry is modulated using spectrum, can be effectively isolated in conventional Hadamard transform ion mobility spectrometry
Multichannel quasi-molecular ions eliminates the modulation defect in conventional Hadamard multiplexing technique, solves the ghost peak and distortion phenomenon in signal,
Improve the signal-to-noise ratio and qualitative analysis ability of Hadamard transform ion mobility spectrometry.
2. spectrum according to claim 1 modulates Hadamard transform ionic migration spectrometer, it is characterised in that：The ionization source
(1) it can be photo-ionisation ionization source, radioactive ionization gauge source, corona discharge ionization source, plasma ionization source, electron spray ionisation source
Or film-type ionization source.
3. spectrum according to claim 1 modulates Hadamard transform ionic migration spectrometer, it is characterised in that：The ion gate
(3) it can be Bradbury-Nielson types, can also be Tyndall-Powell type ion gates.
4. spectrum according to claim 1 modulates Hadamard transform ionic migration spectrometer, it is characterised in that：The spectrum modulation
Hadamard transform door control unit (4) by pseudo-random sequence generator module (8), spectrum modulation Hadamard code modulation module (9) and
Boost module (10) forms, and pseudo-random sequence generator module (8) generates conventional Hadamard transform ion gate sequence, warp first
Spectrum modulation Hadamard code modulation module (9) is converted into spectrum modulation Hadamard transform ion gate pulse train, last boosted
Module (10) completes conversion of the Transistor-Transistor Logic level to high level, and transformed level access ion gate both ends are completed to ion gate (3)
Spectrum modulation control.
5. spectrum according to claim 1 modulates Hadamard transform ionic migration spectrometer, it is characterised in that：Ion signal detects
After unit (6) detects ion signal, spectrum modulation Hadamard transform Ion transfer stack spectral is obtained, and is sent into spectrum modulation Hadamard
Transformation signal processing unit (7) is further processed.
6. spectrum according to claim 1 modulates Hadamard transform ionic migration spectrometer, it is characterised in that：The spectrum modulation
Hadamard transformed signals processing unit (7) completes multichannel spectrum modulation Hadamard by the high-speed data acquisition card of synchronized-pulse control
Acquisition and the A/D conversions for converting Ion transfer stack spectral, recycle upper computer software to complete reading, processing and the reduction of data,
Obtain spectrum modulation Hadamard transform Ion transfer reduction spectrum.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN110146585A (en) * | 2019-06-22 | 2019-08-20 | 湘潭大学 | Prediction and the method for eliminating hadamard transformation Ion transfer spectral transformation ghost peak |
| CN114388333A (en) * | 2022-01-13 | 2022-04-22 | 湘潭大学 | Method for improving signal-to-noise ratio of ion mobility spectrometer and ion mobility spectrometer |
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Cited By (4)
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| CN110146585A (en) * | 2019-06-22 | 2019-08-20 | 湘潭大学 | Prediction and the method for eliminating hadamard transformation Ion transfer spectral transformation ghost peak |
| CN110146585B (en) * | 2019-06-22 | 2021-08-17 | 湘潭大学 | Method for predicting and eliminating Hadamard transform ion mobility spectrometry transform false peak |
| CN114388333A (en) * | 2022-01-13 | 2022-04-22 | 湘潭大学 | Method for improving signal-to-noise ratio of ion mobility spectrometer and ion mobility spectrometer |
| CN114388333B (en) * | 2022-01-13 | 2023-06-20 | 湘潭大学 | Method for improving signal-to-noise ratio of ion mobility spectrometer and ion mobility spectrometer |
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