CN114112042A - Measuring method of free cluster time-resolved luminescence spectrum - Google Patents
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Abstract
The invention discloses a measuring method of a free cluster time-resolved luminescence spectrum, which comprises the steps of generating a cluster beam by a cluster source, forming a parallel beam flying along the axis of a system by a cluster ion optical focusing system, forming a single-size cluster beam by a cluster mass selector, enabling the cluster to enter a space flying freely at a selected speed by an ion accelerating system, carrying out continuous laser irradiation on the cluster by a laser irradiation window in the flying process, and measuring the luminescence intensity of the cluster by a single-photon detector. Compared with the prior art, the invention has the advantages that: the dynamic tracking measurement of the single cluster particle luminescence is realized, a large amount of single cluster particle luminescence signals can be subjected to long-time accumulation measurement, the problems of complex control and difficult experiment caused by the fact that the ion trap technology is adopted to carry out fine three-dimensional fixed point constraint through an electromagnetic field in the prior art, weak luminescence signals caused by too few samples in the ion trap and the like are solved, and the measurement conditions and the cost are greatly simplified.
Description
Technical Field
The invention belongs to the technical fields of atomic molecular physics, cluster physics basic research, nano material optical property analysis and the like, and relates to a single-size cluster time-resolved luminescence spectrum measurement technology based on dynamic constraint and flight time analysis, in particular to a measurement method of a free cluster time-resolved luminescence spectrum.
Background
Optical emission spectroscopy is an important tool for studying the properties of atoms, molecules and clusters. Since the optical emission spectra of atoms, molecules and clusters adsorbed or deposited on the surface of a solid are often very different from those of atoms, molecules and clusters in a free state, in order to study the intrinsic properties of atoms, molecules and clusters, the measurement of the optical emission spectra of particles in free flight is required. For atoms, molecules, this measurement can be done by a stable gas sample. For the cluster, a dense gas phase sample composed of single-size clusters is difficult to obtain, and free-state cluster particles tend to be difficult to track in high-speed flight and rapidly deposit on a solid surface, have short existence time in a gas phase and cannot be positioned. This makes the spectral measurement of free-clusters very difficult. The only method in the prior art at present is to use an "ion trap", namely: the Cluster Ions are confined in a finite space for a certain time to complete the fixed-point Optical excitation and spectral measurement [ Akira Terasaki, Takuya major, Chiharu Kasai, Tamotsu Kondow, et al. Generally, the constraint of cluster ions is realized through an ion trap, the kinetic energy of the cluster needs to be reduced to be lower than the thermal energy, fine three-dimensional constraint is performed through an electromagnetic field, the control is complex, and the experiment is difficult. In addition, only a small number of clusters can be trapped in the ion trap at the same time, the light emission signal is weak, and the measurement of the spectrum can be realized only by means of super-strong light sources such as synchrotron radiation. Therefore, no effective means for measuring the free cluster light emission spectrum exists so far, and particularly, no relevant measuring method report is found in the prior art for analyzing the time-resolved luminescence spectrum of the cluster excited state energy level lifetime.
Disclosure of Invention
The technical problem to be solved is as follows: in order to overcome the defects of the prior art and realize the tracking measurement of the single cluster so as to obtain the time-resolved luminescence spectrum of the free cluster, the invention provides a free cluster dynamic tracking measurement scheme based on dynamic constraint and flight time analysis. According to the scheme, the cluster beam with single size, single kinetic energy and stable strength is obtained through size selection and acceleration, the cluster particles have constant flight speed in a field-free space, and the flight time of the cluster particles accurately corresponds to the flight length. Therefore, the cluster is constrained to fly on a determined path, a light irradiation window is arranged at a specific position of the flying path, the passing cluster particles are excited by light, a series of optical measurement windows are arranged at different positions of the subsequent flying path of the cluster, and light intensity accumulation recording is carried out on each optical measurement window by means of a high-speed single photon measurement technology, the light signals measured by different windows correspond to the emitted light of the cluster under different decay time, and the decay time is the flying time of the cluster from the light excitation (irradiation) window to the optical measurement window. Under the determined optical signal accumulation recording time, the accumulated light intensity of each optical window changes along with the flight time of the cluster from the excitation window to the window, namely, the time-resolved luminescence spectrum is given.
The technical scheme is as follows: the method comprises the steps of generating cluster beams with various sizes through a cluster source, forming parallel beams flying along the axis of a system through a cluster ion optical focusing system, forming single-size cluster beams through a cluster mass selector, enabling the clusters to enter a space flying freely at a selected speed through an ion accelerating system, giving continuous laser irradiation to the clusters through a laser irradiation window in the flying process, enabling the clusters to be optically excited to enter a cluster free flying interval, arranging at least one single-photon detector moving along a cluster flying path in the interval to measure the cluster luminous intensity, and obtaining the time-resolved luminous spectrum of the clusters through the luminous intensity corresponding to the flying time of the clusters from an excitation point to each measuring point.
Preferably, the single size cluster beam stream passes through an ion acceleration system to form clusters of a determined kinetic energy.
Preferably, the cluster source is a magnetron plasma gas cluster source, an arc method gas cluster source or a high-temperature evaporation gas cluster source; the clusters are metal clusters or non-metal clusters, each cluster containing 2-200 atoms.
Preferably, the cluster ion optical focusing system is a conventional electrostatic lens composed of a three-stage to five-stage cylinder; the cluster mass selector is a conventional quadrupole mass filter, or a time-of-flight mass selector.
Preferably, the ion acceleration system is a conventional ion electrostatic acceleration electrode formed from two sheets of metal membrane.
Preferably, the kinetic energy of free flight of the clusters in the ion acceleration system is 1-30 keV.
Preferably, the laser for exciting the cluster to emit light is ultraviolet continuous laser, the laser is perpendicular to the flight path of the cluster and is focused on the cluster, and the diameter of a focal point is less than 0.5 mm.
Preferably, the single photon detector is a photomultiplier or an avalanche diode photodetector.
Preferably, the distance of free flight of the cluster from the position where the cluster is excited by the laser to the position where the luminescence of the cluster is measured is 0.5mm to 50 mm.
Preferably, the single photon detector is arranged in a manner that the detector is vertically aligned with the cluster flight path and can move along the cluster flight path. The following is described with respect to achieving vertical alignment and movement of the detector along the cluster flight path: the moving precision of a commercial optical mechanical platform can be controlled to be several microns or even smaller, the piezoelectric ceramic driven shifter can reach the moving precision of nanometers, and if a collimation diaphragm of about 0.5mm is arranged in front of a single photon detector, the precision of the mechanical system is enough. There is no technical problem in maintaining the vertical alignment of the detector with the cluster beam during the movement. There are various options, such as: arranging a series of optical fibers (the diameter is less than 0.5mm) along a cluster flight path, arranging one end of each optical fiber at a position close to a cluster beam and aligned with the cluster beam, arranging the other end of each optical fiber at a position close to a detector (whether the optical fibers are aligned can be checked by observing whether the two laser beams are vertically crossed or not by introducing a laser beam along the cluster beam flight path and from the optical fibers in advance, finely adjusting the optical fibers according to the condition), and introducing cluster luminescence into the detector; and secondly, the detector moves to each new position, the alignment condition is checked by adopting laser, and the vertical alignment of the detector and the cluster beam is ensured by finely adjusting the position of the detector.
The principle of the measuring method of the free cluster time-resolved luminescence spectrum is as follows: the cluster beam current which is generated by a cluster source, has single size and kinetic energy after size selection and acceleration and is stable in strength, wherein cluster particles have constant flight speed in a free flight interval of the cluster, and the flight time of the cluster particles has an accurate corresponding relation with the flight length. Therefore, the cluster is constrained to fly on a determined path, a laser irradiation window is arranged at a specific position of the flying path, the passing cluster particles are excited by light, a series of optical measurement windows are arranged at different positions of the subsequent flying path of the cluster, and light intensity accumulation recording is carried out on each optical measurement window by means of a high-speed single photon measurement technology, the light signals measured by the different windows correspond to the emitted light of the cluster under different decay times, and the decay time is the flying time of the cluster from the light excitation (irradiation) window to the optical measurement window. At a certain optical signal accumulation recording time, the accumulated light intensity of each optical window changes along with the flight time of the cluster from the excitation window to the point, namely, the time-resolved luminescence spectrum of a single cluster is given.
Has the advantages that: (1) according to the invention, through a cluster ion focusing, mass selection and accelerating system, the transverse momentum compensation of the cluster in the direction vertical to the beam axis is realized, the constrained motion of the cluster on the beam axis is kept, the particle state (mass and kinetic energy) of the cluster is selected, the cluster freely flies at a constant speed along a fixed path in a free space, the precise dynamic space constraint of the cluster beam is realized, and the problems of complex control, difficult experiment and the like caused by the fact that the kinetic energy of the cluster needs to be reduced below the heat energy and the precise three-dimensional constraint is carried out through an electromagnetic field in the conventional static constraint method for realizing cluster ions through an ion trap are solved. The method becomes an effective scheme for replacing an ion trap technology to realize cluster precise constraint. (2) The invention carries out optical excitation and luminescence measurement on the cluster flying freely along a determined path, realizes the quantification of the luminescence time of the cluster through the flying distance of the cluster, realizes the dynamic tracking measurement of the luminescence of single cluster particles, and can carry out long-time accumulation measurement on a large number of luminescence signals of single cluster particles. The realization of the single particle luminescence life spectrum measuring scheme overcomes the defect that only a small number of clusters can be simultaneously imprisoned in the conventional ion trap fixed-point constraint measurement, and cluster spectrum measurement can be realized only by virtue of super-strong light sources such as synchrotron radiation and the like due to weak light emission signals.
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FIG. 1 is a schematic diagram of the principle of the method for measuring the time-resolved luminescence spectrum of free clusters according to the present invention;
FIG. 2 is a practical system for a set of free-cluster time-resolved luminescence spectroscopy measurements established in accordance with the present invention;
the system comprises a cluster source 1, a cluster beam 2, a cluster ion optical focusing system 3, a cluster mass selector 4, a single-size cluster beam 5, an ion acceleration system 6, a laser irradiation window 7, a single photon detector 8, a cluster free flight interval 9, a magnetron plasma gas gathering cluster source 10, a cluster ion electrostatic focusing lens 11, a transverse flight time mass selector 12, a cluster electrostatic acceleration lens 13, a laser incidence window 14, a cluster luminescence measurement window 15 and a vacuum pump 16.
FIG. 3 is Cu measured by the method of the invention in example 25A time-resolved photoluminescence lifetime spectrum of the clusters; i isPLNormalized luminous intensity; t is time.
FIG. 4 shows Ag measured by the method of the present invention in example 34A time-resolved photoluminescence lifetime spectrum of the clusters; i isPLNormalized luminous intensity; t is time.
Detailed Description
The following examples further illustrate the present invention but are not to be construed as limiting the invention. Modifications and substitutions to methods, procedures, or conditions of the invention may be made without departing from the spirit and substance of the invention. Unless otherwise specified, the technical means used in the examples are conventional means well known to those skilled in the art.
Example 1
As shown in a schematic diagram of fig. 1, a method for measuring a time-resolved luminescence spectrum of a free cluster includes generating a cluster beam 2 having various sizes by a cluster source 1, forming a parallel beam flying along a system axis by a cluster ion optical focusing system 3, forming a single-size cluster beam 5 by a cluster mass selector 4, entering the cluster into a space flying freely at a selected speed by an ion acceleration system 6, irradiating the cluster with continuous laser through a laser irradiation window 7 during the flying process, exciting the cluster into a cluster free-flying interval 9 by light, measuring the luminescence intensity of the cluster by at least one single-photon detector 8 arranged in the interval, and obtaining the time-resolved luminescence spectrum of the cluster from the luminescence intensity corresponding to the flying time of the cluster from an excitation point to each measurement point.
The cluster beam 5 with single size forms clusters with determined kinetic energy through an ion acceleration system 6.
The cluster source 1 is a magnetron plasma gas cluster source, an arc method gas cluster source or a high-temperature evaporation gas cluster source; the clusters are metal clusters or non-metal clusters, each cluster containing 2-200 atoms.
The cluster ion optical focusing system 3 is a conventional electrostatic lens composed of a three-stage to five-stage cylinder; the cluster mass selector 4 is a conventional quadrupole mass filter, or a time-of-flight mass selector.
The ion acceleration system 6 is a conventional ion electrostatic acceleration electrode formed from two pieces of metal membrane.
The kinetic energy of the cluster free flight in the ion acceleration system 6 is 1-30 keV.
The laser for exciting the cluster to emit light is ultraviolet continuous laser, the laser is perpendicular to the flight path of the cluster and is focused on the cluster, and the diameter of a focus is less than 0.5 mm.
The single photon detector 8 is a photomultiplier or an avalanche diode photodetector.
The distance of free flight of the cluster from the position where the cluster is excited by the laser to the position where the luminescence of the cluster is measured is 0.5mm-50 mm.
The single photon detector 8 is arranged in a way that the detector is vertically aligned with the cluster flight path and can move along the cluster flight path.
Example 2
According to the method for measuring the time-resolved luminescence spectrum of the free-cluster shown in example 1 and fig. 1, a set of experimental systems for measuring the time-resolved luminescence spectrum of the free-cluster is established as shown in fig. 2, and the operation process comprises the following steps:
generating continuous cluster beams by a magnetron plasma gas cluster gathering source 10, focusing by a cluster ion electrostatic focusing lens 11 to form parallel beams flying along the axis of the cluster ion electrostatic focusing lens, selecting single-size clusters by a transverse flying time selector 12, and enabling the clusters to enter a space flying freely at a selected speed by a cluster electrostatic accelerating lens 13; in cluster free flight, a cluster beam is irradiated with continuous laser light through the laser incident window 14, so that the cluster is optically excited. The light emission intensity of the cluster is measured by the single photon detector 8 from the cluster light emission measurement window 15 at different positions on the free flight path of the cluster, so that the time-resolved light emission spectrum of the cluster, that is, the light emission intensity which changes with the flight time of the cluster from the excitation point to each measurement point, is obtained. The above process is all carried out in a vacuum environment, with a high vacuum maintained by two vacuum pumps 16.
The conventional cluster source used in this example is a magnetron plasma gas cluster source. Cu clusters are generated from a cluster source. The cluster beam is focused by a conventional electrostatic lens consisting of a three-stage cylinder. Clusters with atomic number 5 were selected by a lateral time-of-flight selector and accelerated to 30 keV. The cluster excitation adopts 375nm wavelength continuous laser, the laser is perpendicular to the flight path of the cluster and is focused on the flight path, and the focal diameter is less than 0.5 mm. The cluster luminescence measurement adopts an avalanche diode photoelectric detector, and 20 points are selected for the luminescence measurement within the range of 0.5mm-10mm from a laser excitation point on the cluster flight path. The light measurement accumulation time at each measurement point was 1000 s. FIG. 3 shows the measured Cu5Time-resolved photoluminescence lifetime spectra of clusters.
Example 3
The difference from example 2 is thatThe regular cluster source is a high-temperature evaporation gas cluster gathering source, and the Ag cluster is generated by the cluster source. The cluster beam is focused by a conventional electrostatic lens consisting of a three-stage cylinder. Clusters with atomic number 4 were selected by a lateral time-of-flight selector. The clusters are accelerated to 20keV by an electrostatic acceleration system. The method comprises the steps of adopting continuous laser excitation with the wavelength of 375nm, adopting an avalanche diode photoelectric detector for cluster luminescence measurement, vertically aligning a detector with a cluster flight path, moving along the cluster flight path, starting luminescence measurement at a position 2.0mm away from a laser excitation point on the cluster flight path, carrying out luminescence measurement with the accumulation time of 800s every time of moving 2.0mm, and measuring 25 points in total. FIG. 4 shows Ag measured4Time-resolved photoluminescence lifetime spectra of clusters.
Claims (10)
1. Method for measuring a time-resolved luminescence spectrum of a free-cluster, characterized in that the method generates a cluster beam (2) comprising various sizes by means of a cluster source (1), parallel beam current flying along the system axis is formed through a cluster ion optical focusing system (3), a single-size cluster beam current (5) is formed through a cluster mass selector (4), the cluster is then moved by an ion acceleration system (6) into a space free-flying at a selected velocity, in the flying process, continuous laser irradiation is carried out on the cluster through a laser irradiation window (7), so that the cluster is optically excited to enter a free-flying interval (9) of the cluster, a single-photon detector (8) moving along the flying direction of the cluster is arranged in the free-flying interval to measure the luminous intensity of the cluster at different positions on the flying path of the cluster, and the time-resolved luminous spectrum of the cluster is obtained according to the luminous intensity of the flying time of the cluster from an excitation point to each measuring point.
2. The method for measuring a time-resolved luminescence spectrum of free clusters according to claim 1, characterized in that a cluster beam (5) of a single size is subjected to an ion acceleration system (6) to form clusters of a determined kinetic energy.
3. The method for measuring a free-cluster time-resolved luminescence spectrum according to claim 1, wherein the cluster source (1) is a magnetron plasma gas cluster source, an arc method gas cluster source, or a high-temperature evaporation gas cluster source; the clusters are metal clusters or non-metal clusters, each cluster containing 2-200 atoms.
4. The method for measuring a time-resolved luminescence spectrum of free clusters according to claim 1, characterized in that the cluster ion optical focusing system (3) is a conventional electrostatic lens consisting of a three-to five-stage cylinder; the cluster mass selector (4) is a conventional quadrupole mass filter, or a time-of-flight mass selector.
5. The method for measuring a time-resolved luminescence spectrum of free clusters according to claim 1, characterized in that the ion acceleration system (6) is a conventional ion electrostatic acceleration electrode formed by two metal sheets.
6. The method for measuring a time-resolved luminescence spectrum of free clusters according to claim 1, characterized in that the kinetic energy of the free flight of clusters within the ion acceleration system (6) is 1-30 keV.
7. The method for measuring a free-cluster time-resolved luminescence spectrum according to claim 1, wherein the laser for exciting the cluster to emit light is an ultraviolet continuous laser, the laser is perpendicular to a flight path of the cluster and focused on the cluster, and the focal diameter is less than 0.5 mm.
8. The method for measuring a free-cluster time-resolved luminescence spectrum according to claim 1, wherein the single-photon detector (8) is a photomultiplier or an avalanche diode photodetector.
9. The method for measuring a time-resolved emission spectrum of a free cluster according to claim 1, wherein a distance of free flight of the cluster from a position where the cluster is excited by the laser to a position where emission of the cluster is measured is 0.5mm to 50 mm.
10. The method for measuring a free-cluster time-resolved luminescence spectrum according to claim 1, wherein the single-photon detector (8) is arranged in such a way that the detector is vertically aligned with and moves along the cluster flight path.
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Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5051582A (en) * | 1989-09-06 | 1991-09-24 | The United States Of America As Represented By The Secretary Of The Air Force | Method for the production of size, structure and composition of specific-cluster ions |
| CN109115660A (en) * | 2018-08-23 | 2019-01-01 | 金华职业技术学院 | A kind of particle imaging method |
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Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5051582A (en) * | 1989-09-06 | 1991-09-24 | The United States Of America As Represented By The Secretary Of The Air Force | Method for the production of size, structure and composition of specific-cluster ions |
| CN109115660A (en) * | 2018-08-23 | 2019-01-01 | 金华职业技术学院 | A kind of particle imaging method |
Non-Patent Citations (2)
| Title |
|---|
| AKIRA TERASAKI等: "Photoabsorption and Magneto‑Optical Spectroscopy of Mass‑Selected Atomic and Cluster Ions Stored in an Ion Trap", 《AIP CONFERENCE PROCEEDINGS》 * |
| 韩民: "团簇束流与团簇淀积", 《中国优秀博硕士学位论文全文数据库(博士)基础科学辑》 * |
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