CN117612928A - Accelerator mass spectrometry device based on high-charge state ion source - Google Patents
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- 238000004760 accelerator mass spectrometry Methods 0.000 title claims abstract description 33
- 150000002500 ions Chemical class 0.000 claims abstract description 135
- 238000010884 ion-beam technique Methods 0.000 claims abstract description 55
- 238000012216 screening Methods 0.000 claims abstract description 37
- 230000001133 acceleration Effects 0.000 claims abstract description 18
- 238000005259 measurement Methods 0.000 claims abstract description 16
- 238000001514 detection method Methods 0.000 claims abstract description 14
- 239000002245 particle Substances 0.000 claims abstract description 5
- 239000012535 impurity Substances 0.000 claims description 19
- 229910052792 caesium Inorganic materials 0.000 abstract description 13
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 abstract description 13
- 238000004544 sputter deposition Methods 0.000 abstract description 11
- 238000004458 analytical method Methods 0.000 abstract description 9
- 150000001450 anions Chemical class 0.000 abstract description 7
- 230000035945 sensitivity Effects 0.000 abstract description 7
- 239000000243 solution Substances 0.000 description 7
- 239000011261 inert gas Substances 0.000 description 5
- 238000000034 method Methods 0.000 description 4
- 230000005540 biological transmission Effects 0.000 description 3
- 239000012634 fragment Substances 0.000 description 3
- 238000001819 mass spectrum Methods 0.000 description 3
- 150000001793 charged compounds Chemical class 0.000 description 2
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- 239000007787 solid Substances 0.000 description 2
- 235000013619 trace mineral Nutrition 0.000 description 2
- 239000011573 trace mineral Substances 0.000 description 2
- 229910052768 actinide Inorganic materials 0.000 description 1
- 150000001255 actinides Chemical class 0.000 description 1
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- H—ELECTRICITY
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- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
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- H01J49/10—Ion sources; Ion guns
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- G—PHYSICS
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
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Abstract
The invention provides an accelerator mass spectrometry analysis device based on a high-charge state ion source, which comprises a high-charge state ion source module, a first selection module, an acceleration module, a second selection module and a detection module; the high-charge state ion source module is used for generating high-charge state ion beam current, and the first selection module is used for carrying out first-stage screening on the high-charge state ion beam current; the accelerating module is used for accelerating the high-charge state ion beam current to a preset target energy level and carrying out speed screening, and the second selecting module is used for carrying out second-stage screening on the high-charge state ion beam current; the detection module is used for carrying out particle identification and/or isotope abundance ratio measurement on the high-charge state ion beam current. The high-charge state ion beam current generated by the high-charge state ion source module has no molecular interference, can provide the beam current intensity far greater than that of the cesium sputtering anion source in the prior art, improves the measurement sensitivity, can analyze partial nuclides incapable of generating anions, and has wide application range.
Description
Technical Field
The invention relates to the technical field of accelerator mass spectrometry, in particular to an accelerator mass spectrometry device based on a high-charge state ion source.
Background
Accelerator mass spectrometry refers to a nuclear analysis technique in which accelerator is combined with mass spectrometry. Many areas of modern science and technology, such as archaeology, biomedical science, geology, and astrophysics, rely heavily on accelerator mass spectrometry.
Conventional accelerator mass spectrometers mostly employ cesium sputter negative ion sources and tandem accelerators. Although such accelerator mass spectrometers have been in development for forty-five years, certain limitations remain: in the first aspect, molecular interference exists in the cesium sputtering anion source to form an instrument background, so that the detection sensitivity of partial isotopes is restricted; in the second aspect, the beam intensity of the cesium sputtering negative ion source is weaker and is generally not more than 100 microamps, so that the event rate of experimental measurement is limited; in a third aspect, an accelerator mass spectrometer employing a cesium sputter negative ion source is incapable of analyzing a portion of a species (e.g., an inert gas isotope) because it employs a negative ion source and such species cannot generate negative ions.
Disclosure of Invention
The invention provides an accelerator mass spectrum analysis device based on a high-charge state ion source, which is used for solving the defects that an accelerator mass spectrometer adopting a cesium sputtering negative ion source in the prior art has molecular interference, weak beam intensity and incapability of analyzing part of nuclides incapable of generating negative ions, realizing thorough Bayer molecular interference, improving beam intensity and realizing measurement of nuclides incapable of generating negative ions.
The invention provides an accelerator mass spectrometry analysis device based on a high-charge state ion source, which comprises:
the device comprises a high-charge state ion source module, a first selection module, an acceleration module, a second selection module and a detection module;
the high-charge state ion source module is used for generating high-charge state ion beam current;
the input end of the first selection module is connected with the output end of the high-charge state ion source module and is used for carrying out first-stage screening on the high-charge state ion beam current according to a preset first mass-to-charge ratio resolution limit value to primarily remove impurity ions;
the input end of the acceleration module is connected with the output end of the first selection module and is used for accelerating the high-charge state ion beam after the first-stage screening to a preset target energy level and carrying out speed screening on the high-charge state ion beam based on a preset speed threshold;
the input end of the second selection module is connected with the output end of the acceleration module and is used for carrying out second-stage screening on the high-charge state ion beam current reaching the target energy level according to a preset second mass-to-charge ratio resolution limit value, and removing impurity ions again;
the input end of the detection module is connected with the output end of the second selection module and is used for carrying out particle identification and/or isotope abundance ratio measurement on the high-charge state ion beam current subjected to the second-stage screening.
According to the accelerator mass spectrometry device based on the high-charge state ion source, the high-charge state ion source module is a high-charge state electron cyclotron resonance ion source.
According to the accelerator mass spectrometry analysis device based on the high-charge state ion source, the acceleration module is a linear accelerator.
According to the accelerator mass spectrometry analysis device based on the high-charge state ion source, the linear accelerator comprises a pre-beam-forming device, a first accelerator and a second accelerator;
the input end of the pre-buncher is connected with the output end of the first selection module and is used for improving the speed selectivity of the first accelerator;
the input end of the first accelerator is connected with the output end of the pre-buncher and is used for accelerating ions in the high-charge state ion beam after the first-stage screening to a preset intermediate energy level and carrying out speed screening on the ions in the high-charge state ion beam reaching the intermediate energy level based on a preset speed threshold;
the input end of the second accelerator is connected with the output end of the first accelerator, and the output end of the second accelerator is connected with the input end of the second selection module and is used for accelerating ions in the high-charge state ion beam after speed screening to a preset target energy level.
According to the accelerator mass spectrometry device based on the high-charge state ion source, the first accelerator is a radio-frequency four-stage field accelerator, and the second accelerator is a drift tube linear accelerator.
According to the accelerator mass spectrometry analysis device based on the high-charge state ion source, the preset intermediate energy level is of the order of hundred keV of single nuclear energy.
According to the accelerator mass spectrometry device based on the high-charge state ion source, the preset target energy level is of the order of magnitude of single nuclear energy MeV.
According to the accelerator mass spectrometry device based on the high-charge state ion source, the first selection module and the second selection module are both mass-to-charge ratio selectors.
According to the accelerator mass spectrometry device based on the high-charge state ion source, the first mass-to-charge ratio resolution limit is 1/100.
According to the accelerator mass spectrometry device based on the high-charge state ion source, the second mass-to-charge ratio resolution limit value is smaller than 2/1000.
The invention provides an accelerator mass spectrometry analysis device based on a high-charge state ion source, which comprises a high-charge state ion source module, a first selection module, an acceleration module, a second selection module and a detection module, wherein the high-charge state ion source module is used for generating high-charge state ion beam current; the input end of the first selection module is connected with the output end of the high-charge state ion source module and is used for carrying out first-stage screening on the high-charge state ion beam current according to a preset first mass-to-charge ratio resolution limit value to primarily remove impurity ions; the input end of the acceleration module is connected with the output end of the first selection module and is used for accelerating the high-charge state ion beam after the first-stage screening to a preset target energy level and carrying out speed screening on the high-charge state ion beam based on a preset speed threshold; the input end of the second selection module is connected with the output end of the acceleration module and is used for carrying out second-stage screening on the high-charge state ion beam current reaching the target energy level according to a preset second mass-to-charge ratio resolution limit value, and removing impurity ions again; the input end of the detection module is connected with the output end of the second selection module and is used for carrying out particle identification and/or isotope abundance ratio measurement on the high-charge-state ion beam current subjected to the second-stage screening. The high-charge state ion beam current generated by the high-charge state ion source module has no molecular interference, can provide beam intensity far greater than that of a cesium sputtering negative ion source in the prior art, so that statistics is better, measurement sensitivity can be improved, and in addition, partial nuclides incapable of generating negative ions can be analyzed by adopting a positive ion source, so that the application range is wide.
Drawings
In order to more clearly illustrate the invention or the technical solutions of the prior art, the following description will briefly explain the drawings used in the embodiments or the description of the prior art, and it is obvious that the drawings in the following description are some embodiments of the invention, and other drawings can be obtained according to the drawings without inventive effort for a person skilled in the art.
Fig. 1 is a schematic structural diagram of an accelerator mass spectrometry device based on a high-charge state ion source.
1: a high charge state ion source module; 2: a first selection module; 3: an acceleration module; 4: a second selection module; 5: a detection module; 31: a pre-buncher; 32: a first accelerator; 33: and a second accelerator.
Detailed Description
For the purpose of making the objects, technical solutions and advantages of the present invention more apparent, the technical solutions of the present invention will be clearly and completely described below with reference to the accompanying drawings, and it is apparent that the described embodiments are some embodiments of the present invention, not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
In order to overcome the defects that in the prior art, an accelerator mass spectrometer adopting a cesium sputtering negative ion source has molecular interference, weak beam intensity and can not analyze part of nuclides incapable of generating negative ions, the invention provides an accelerator mass spectrometry device based on a high-charge state ion source, and the accelerator mass spectrometry device based on the high-charge state ion source is described below with reference to fig. 1.
As shown in fig. 1, the accelerator mass spectrometry device based on the high-charge state ion source provided by the invention comprises a high-charge state ion source module 1, a first selection module 2, an acceleration module 3, a second selection module 4 and a detection module 5.
The high-charge state ion source module 1 is used for generating high-charge state ion beam current. High charge state ions refer to substances with higher charge numbers of the ions, which lose a plurality of electrons, so that the high charge state ions have very high positive charges, and the high charge state ions have wide application fields including plasma physics, material physics, life sciences and the like. It should be appreciated that in an alternative embodiment of the present application, the high charge state ion source module 1 is not limited to generating a high charge state ion beam current that is capable of generating a multi-species multi-charge state ion beam current, but is only one of the ion beam currents that it is capable of generating.
The adoption of the ion beam current in the high charge state has at least the following advantages:
first, the traditional cesium sputtering negative ion source has molecular interference, which forms instrument background and limits detection sensitivity of partial isotopes, a stripper is needed to remove the interference of the background, and when molecular ions pass through the stripper, the molecular ions are broken down due to coulomb force, but molecular fragment ions generated in the stripping process can also cause interference and limit detection sensitivity of partial isotopes.
The high-charge state ion source module 1 can generate high-charge state ion beam current, and high-charge state ions have no interference of molecular states, so that stripping is not needed, and interference of molecular fragments generated by stripping is avoidedAnd meanwhile, the loss of beam intensity caused by stripping is avoided. The high-charge state ion source module 1 can realize the measurement of gaseous, liquid and solid samples, and can adopt a laser plasma injection mode for the solid samples to effectively reduce the memory effect. The accelerator mass spectrum analysis device provided by the invention can realize analysis of actinide samples below femtocells (fg) to generate 41 Ca full bare ion gets rid of 41 K interference of 41 Ca provides a new method for definite years.
Second, the combing intensity of the ion beam generated by the traditional cesium sputtering negative ion source is weak, generally not more than 100 microamps, and the event rate of experimental measurement is limited.
Compared with the ion beam current generated by cesium sputtering anion source, the high-charge state ion beam current generated by the high-charge state ion source module 1 is 1-2 orders of magnitude higher in beam current intensity, so that the event rate for trace element measurement is improved by 1-2 orders of magnitude.
Third, the traditional accelerator mass spectrometers adopting cesium sputtering anion sources adopt anion sources, and inert gas isotopes cannot generate anions, so that the accelerator mass spectrometers cannot analyze inert gas isotopes, and the application range is small.
The high-charge state ion source module 1 can generate the beam current of the inert gas isotope due to the adoption of the positive ion source, so that the analysis of the inert gas isotope is realized, and the application range is wider.
In an alternative embodiment of the invention, the high charge state ion source module 1 is comprised of a high charge state electron cyclotron resonance (Electron Cyclotron Resonance, ECR) ion source.
The input end of the first selection module 2 is connected with the output end of the high-charge state ion source module 1, and is used for performing first-stage screening on the high-charge state ion beam current according to a preset first mass-to-charge ratio resolution limit value, and primarily removing impurity ions. In an alternative embodiment of the invention, the first selection module 2 is a first order mass to charge ratio (M/q) selector. The input end of the first-stage M/q selector is connected with the input end of the high-charge state ECR ion source through a beam current transmission line and is used for carrying out first-stage screening on high-charge state ion beam current generated by the high-charge state ECR ion source. Specifically, in an alternative embodiment of the present invention, the mass-to-charge ratio resolution of the first stage screening (i.e., d (M/q)/(M/q), where M is the mass number of the ion, q is the charge state of the ion, and M/q is the ion mass-to-charge ratio) is 1/100, i.e., if the difference between the mass-to-charge ratios of the impurity ion and the target ion, d (M/q), divided by the value of the target ion mass-to-charge ratio (M/q), is greater than 1/100, the impurity ion is blocked, and conversely, the impurity ion will pass. By setting the mass-to-charge ratio resolution of the first stage screening to 1/100, impurity ions larger than the resolution can be filtered out, and preliminary removal of impurity ions can be realized.
The input end of the acceleration module 3 is connected with the output end of the first selection module 2, and is used for accelerating the high-charge state ion beam after the first-stage screening to a preset target energy level and carrying out speed screening on the high-charge state ion beam based on a preset speed threshold.
In an alternative embodiment of the present application, the acceleration module 3 employs a linear accelerator.
Specifically, the linear accelerator used in the present application includes a pre-beam condenser 31, a first accelerator 32, and a second accelerator 33.
The input of the pre-buncher 31 is connected to the output of the first selection module 2 for increasing the speed selectivity of the first accelerator 32. The pre-beam-forming device 31 is a pre-beam-forming device of the first accelerator 32, which is connected with the first selecting module 2 and is connected with the first accelerator 32, and is used for improving the speed selectivity of the first accelerator 32. Taking a radio frequency quaternary field (Radio Frequency Quadrupole, RFQ) accelerator as the first accelerator 32 as an example, the pre-beam accelerator 31 is upstream of the RFQ accelerator, and the ion beam is focused along the beam advancing direction (i.e., the longitudinal direction in fig. 1) after passing through the longitudinal beam focusing action of the pre-beam accelerator 31, so as to form an ion beam mass with a microstructure, and the ion beam mass drifts a distance into the RFQ accelerator. The time required for drift over a distance is different due to the different velocities of the ions in the cluster. Whereas the RFQ accelerator can only receive ions within a time window beyond which ions will not be effectively accelerated. Thus, the reverse-push can be seen that the RFQ accelerator can only receive ions within a certain speed range, which is speed selectivity. Therefore, the presence of the pre-buncher 31 helps to improve the speed selectivity of the RFQ accelerator.
The input end of the first accelerator 32 is connected to the output end of the pre-beam shaper 31, and is used for accelerating ions in the high-charge state ion beam to a preset intermediate energy level and performing speed screening on the ions in the high-charge state ion beam based on a preset speed threshold.
In an alternative embodiment of the present invention, an RFQ accelerator is selected as the first accelerator 32, where the RFQ accelerator is capable of accelerating target ions in the high-charge-state ion beam after being screened by the first selection module 2 to a preset intermediate energy level, preferably, the preset intermediate energy level is on the order of hundred keV of single nuclear energy. In addition, the RFQ accelerator can also be used as an ion speed selector at the same time, namely, ions accelerated by the RFQ accelerator are all in a preset energy spread, and ions beyond the energy spread are lost.
The input end of the second accelerator 33 is connected to the output end of the first accelerator 32, and the output end is connected to the input end of the second selection module 4, so as to accelerate the ions in the high-charge state ion beam after speed screening to a preset target energy level.
In an alternative embodiment of the present invention, a Drift Tube Linac (DTL) accelerator is selected as the second accelerator 33. The input end of the DTL accelerator is connected with the RFQ accelerator through a beam transmission line, and the input end of the DTL accelerator is connected with the second selection module 4 through the beam transmission line. The DTL accelerator is capable of accelerating ions in a high charge state ion beam to a preset target energy level, preferably on the order of MeV, which is the single nuclear energy.
Through the small-size linear accelerator structure that adopts "pre-buncher + RFQ accelerator + DTL accelerator", compare with the serial accelerator or other high-pressure type accelerators that traditional accelerator mass spectrometer adopted, the linear accelerator that this application adopted possesses strong speed selectivity, can promote the sensitivity of accelerator mass spectrum, in addition, the ion energy that the linear accelerator that this application adopted can accelerate is higher, especially to the heavier nuclide of quality, more is favorable to ion identification, suppresses the interference of impurity nuclide ion.
The input end of the second selection module 4 is connected with the output end of the acceleration module 3, and is used for performing second-stage screening on the high-charge state ion beam current reaching the target energy level according to a preset second mass-to-charge ratio resolution limit value, and removing impurity ions again.
In an alternative embodiment of the invention, the second selection module 4 is a second stage mass to charge ratio (M/q) selector. The second stage M/q selector is used for carrying out second stage screening on the high-charge state ion beam current. Specifically, in an alternative embodiment of the present invention, the mass-to-charge ratio resolution of the second stage screening is less than 2/1000, i.e., if the difference d (M/q) between the mass-to-charge ratio of the impurity ions and the target ions divided by the value of the mass-to-charge ratio of the target ions (M/q) is equal to or greater than the mass-to-charge ratio resolution (e.g., equal to or greater than 2/1000), the impurity ions are blocked, and vice versa, the impurity ions will pass. By setting the mass-to-charge ratio resolution of the second stage screening to be less than 2/1000, impurity ions greater than this resolution can be filtered out, enabling further removal of impurity ions.
The input end of the detection module 5 is connected with the output end of the second selection module 4, and is used for carrying out particle identification and/or isotope abundance ratio measurement on the high-charge-state ion beam current subjected to the second-stage screening.
In summary, the accelerator mass spectrometry device based on the high-charge state ion source provided by the invention can thoroughly get rid of molecular interference, and the generated high-charge state positive ions do not need to be stripped, so that the interference of molecular fragments generated by stripping is avoided. In addition, the linear accelerator has the advantages of good ion speed selectivity and high acceleration energy, so that the measurement sensitivity can be effectively improved, compared with a traditional cesium sputtering negative ion source, the beam intensity generated by a high-charge ECR ion source is 1-2 orders of magnitude higher, positive ions do not need to be stripped, the beam intensity loss caused by stripping is avoided, and the event rate for trace element measurement is improved by 1-2 orders of magnitude; the use of a highly charged ECR ion source has significant advantages in the measurement of partial species, such as inert elemental measurements, 41 ca measurementAnd the mass spectrometer is expected to become a key instrument for research and application in the multidisciplinary field.
The apparatus embodiments described above are merely illustrative, wherein the elements illustrated as separate elements may or may not be physically separate, and the elements shown as elements may or may not be physical elements, may be located in one place, or may be distributed over a plurality of network elements. Some or all of the modules may be selected according to actual needs to achieve the purpose of the solution of this embodiment. Those of ordinary skill in the art will understand and implement the present invention without undue burden.
From the above description of the embodiments, it will be apparent to those skilled in the art that the embodiments may be implemented by means of software plus necessary general hardware platforms, or of course may be implemented by means of hardware. Based on this understanding, the foregoing technical solution may be embodied essentially or in a part contributing to the prior art in the form of a software product, which may be stored in a computer readable storage medium, such as ROM/RAM, a magnetic disk, an optical disk, etc., including several instructions for causing a computer device (which may be a personal computer, a server, or a network device, etc.) to execute the method described in the respective embodiments or some parts of the embodiments.
Finally, it should be noted that: the above embodiments are only for illustrating the technical solution of the present invention, and are not limiting; although the invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical scheme described in the foregoing embodiments can be modified or some technical features thereof can be replaced by equivalents; such modifications and substitutions do not depart from the spirit and scope of the technical solutions of the embodiments of the present invention.
Claims (10)
1. An accelerator mass spectrometry apparatus based on a high charge state ion source, comprising: the device comprises a high-charge state ion source module, a first selection module, an acceleration module, a second selection module and a detection module;
the high-charge state ion source module is used for generating high-charge state ion beam current;
the input end of the first selection module is connected with the output end of the high-charge state ion source module and is used for carrying out first-stage screening on the high-charge state ion beam current according to a preset first mass-to-charge ratio resolution limit value to primarily remove impurity ions;
the input end of the acceleration module is connected with the output end of the first selection module and is used for accelerating the high-charge state ion beam after the first-stage screening to a preset target energy level and carrying out speed screening on the high-charge state ion beam based on a preset speed threshold;
the input end of the second selection module is connected with the output end of the acceleration module and is used for carrying out second-stage screening on the high-charge state ion beam current reaching the target energy level according to a preset second mass-to-charge ratio resolution limit value, and removing impurity ions again;
the input end of the detection module is connected with the output end of the second selection module and is used for carrying out particle identification and/or isotope abundance ratio measurement on the high-charge state ion beam current subjected to the second-stage screening.
2. The high charge state ion source based accelerator mass spectrometry apparatus of claim 1, wherein the high charge state ion source module is a high charge state electron cyclotron resonance ion source.
3. The high charge state ion source based accelerator mass spectrometry apparatus of claim 1, wherein the acceleration module is a linear accelerator.
4. The high charge state ion source based accelerator mass spectrometry apparatus of claim 3, wherein the linac comprises a pre-beam former, a first accelerator and a second accelerator;
the input end of the pre-buncher is connected with the output end of the first selection module and is used for improving the speed selectivity of the first accelerator;
the input end of the first accelerator is connected with the output end of the pre-buncher and is used for accelerating ions in the high-charge state ion beam after the first-stage screening to a preset intermediate energy level and carrying out speed screening on the ions in the high-charge state ion beam reaching the intermediate energy level based on a preset speed threshold;
the input end of the second accelerator is connected with the output end of the first accelerator, and the output end of the second accelerator is connected with the input end of the second selection module and is used for accelerating ions in the high-charge state ion beam after speed screening to a preset target energy level.
5. The high charge state ion source based accelerator mass spectrometry apparatus of claim 4, wherein the first accelerator is a radio frequency four-stage field accelerator and the second accelerator is a drift tube linear accelerator.
6. The high charge state ion source based accelerator mass spectrometry apparatus of claim 4, wherein the predetermined intermediate energy level is on the order of hundred keV for single nuclei.
7. The high charge state ion source based accelerator mass spectrometry apparatus of claim 4, wherein the predetermined target energy level is on the order of MeV.
8. The high charge state ion source based accelerator mass spectrometry apparatus of claim 1, wherein the first selection module and the second selection module are both mass to charge ratio selectors.
9. The high charge state ion source based accelerator mass spectrometry apparatus of any of claims 1-8, wherein the first mass to charge ratio resolution limit is 1/100.
10. The high charge state ion source based accelerator mass spectrometry apparatus of any of claims 1-8, wherein the second mass to charge ratio resolution limit is less than 2/1000.
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