CN113257847B - Perovskite anisotropy enhanced high-resolution gamma ray imaging method - Google Patents
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Abstract
The invention discloses a perovskite anisotropy enhanced high-resolution gamma ray imaging method. The perovskite single crystal structure is regulated and controlled by a process treatment method, so that the transverse carrier mobility of the perovskite single crystal structure is reduced, and the service life of carriers is shortened. In the gamma ray detection imaging process, a photogenerated carrier is transported from a top electrode to a bottom electrode under the action of a longitudinal electric field to form a detection signal. The photo-generated carriers are subjected to the action of the edge field at the same time, so that lateral diffusion is generated. However, since the photo-generated carrier mobility-lifetime product of lateral diffusion becomes small, the probability of recombination of photo-generated electrons and holes participating in lateral diffusion increases. A large amount of laterally diffused photo-generated electrons and holes are recombined before reaching the collecting electrode, so that crosstalk charge signals of adjacent pixels are reduced, and the imaging spatial resolution of gamma rays is finally improved.
Description
Technical Field
The invention belongs to the field of high-spatial-resolution gamma ray imaging methods, and particularly relates to a perovskite anisotropy-enhanced high-resolution gamma ray imaging method.
Background
Gamma-ray detection has important application in the fields of nuclear medicine, aerospace, industrial nondestructive detection and the like, and is one of peopleEfforts have been directed toward developing high performance gamma ray detectors. Since gamma-ray photons are high in energy and penetration, gamma-ray detecting active materials need to have a high average atomic number (Z) and thickness to sufficiently absorb gamma photons. High purity semiconductor single crystals are generally selected as radiation detection active materials, and gamma-ray detection using high purity Ge (HPGe) has been proposed in the 70 s to achieve good energy resolution. But because of its small bandgap, liquid nitrogen cooling is required. For detecting gamma rays at room temperature, compound semiconductor crystals such as CdTe and Cd are used as active materials for gamma ray detection 1- x Zn x Te (CZT), tlBr, etc. These gamma ray detectors have found commercial use. However, the existing compound semiconductor gamma-ray detector has the problems of complex preparation technology, high cost, incompatibility of the sensing unit and the readout circuit process, difficulty in considering energy resolution, spatial resolution, sensitivity, working temperature, cost and the like in gamma-ray detection imaging.
Because gamma ray detection requires a very thick photon absorber, gamma ray imaging has a lower spatial resolution than lower energy photon (e.g., visible light, X-rays, etc.) imaging resolution. The reduction in spatial resolution during gamma imaging is illustrated in fig. 1. In the indirect detection of fig. 1 (a), gamma ray photons 21 are incident on a scintillator 22 to produce scintillating fluorescence 23 (visible light), which is then converted into an electrical signal by a conventional visible light detector 24. However, due to the scattering phenomenon of visible light, the scintillating fluorescence 23 scatters in the scintillator 22, resulting in an expansion 25 of the fluorescence spot, and finally, a reduction in the spatial resolution of the indirect detection gamma-ray imaging. In the gamma ray direct detection structure shown in fig. 1 (b), the detection active material layer 26 absorbs gamma ray photons 21, and directly converts them into photogenerated carriers 15 (electron/hole pairs). A bias photo-generated carrier 15 is arranged between the common electrode 4 and the pixel electrode 5 and drifts up and down by the action of an external electric field to form a detection electric signal. Although the direct detection of gamma rays avoids the scattering effect of scintillation fluorescence, due to the fringe field existing between the upper electrode and the lower electrode, the photogenerated carriers 15 can generate lateral diffusion under the effect of the fringe field, resulting in charge crosstalk 27 between adjacent pixel electrodes, and finally reducing the imaging resolution of gamma rays.
The perovskite material has excellent photoelectric performance, and has very good application prospects in the fields of photovoltaic solar cells, UV/Vis/NIR photoelectric detection, light-emitting diodes and the like. The perovskite monocrystal has wide band gap (about 3.1 ev), contains heavy elements such as lead, halogen and the like, and has carrier mobility as high as 600cm 2 V -1 S -1 The advantages are long service life of carriers reaching several microseconds, ionization energy reaching 3-5 eV, and low cost. In addition, halogen perovskites also have very good radiation resistance properties compared to other semiconductors. Research shows that the formation energy of deep level carrier traps in many halogen perovskite crystals is very large, so that point defects caused by irradiation are mostly shallow level traps. The tolerance of the defects improves the irradiation resistance of perovskite crystals. Because of the above-mentioned advantages of perovskite crystals, it is considered as a next generation gamma ray direct detection material. Perovskite crystals are sequentially applied to the field of high-energy ray detection by research teams at home and abroad from 2015, and important research results are obtained. These results show that the quantum efficiency of gamma photon detection can be improved by optimizing the elemental composition and preparation process of perovskite crystals. Meanwhile, it is proposed to suppress the fringe field by optimally designing the electrode structure, thereby improving the spatial resolution of gamma-ray imaging. A typical technical solution is proposed by the j.s.huang group of us University of North Carolina, which uses conventional top and bottom electrodes, to generate a fringe field in the detector that causes lateral diffusion of photogenerated carriers. The S.Huang research group divides the top electrode into two parts by arranging an isolating ring on the top electrode, and the electrode can inhibit the edge field and reduce the lateral diffusion of photo-generated carriers. However, as the thickness of perovskite crystals increases, the ratio of the spacer ring dimension to the crystal thickness becomes progressively smaller, and the spacer ring's effect of suppressing the fringe field is also impaired.
The invention provides a direct detection high-resolution gamma-ray imaging method by utilizing the structural characteristics of perovskite materials and the advantages of a solution method preparation process, which can effectively solve the problem that an electrode structure inhibits the edge field from being insensitive.
Disclosure of Invention
The invention aims to provide a perovskite anisotropy enhanced high-resolution gamma ray imaging method for solving the technical problems.
In order to solve the technical problems, the specific technical scheme of the invention is as follows:
a method of perovskite anisotropy enhanced high resolution gamma ray imaging comprising the steps of:
step one, adopting a process method to treat the perovskite crystal so that anisotropy of the structure and the electrical property of the perovskite crystal appears;
and secondly, utilizing the anisotropy of the perovskite crystal to enable photo-generated carriers generated by gamma ray photons to be transmitted longitudinally and rapidly, forming effective detection electric signals, enabling the photo-generated carriers to be low in transverse transmission speed and short in carrier service life, reducing transverse charge crosstalk between adjacent electrodes, and improving gamma ray imaging resolution.
Further, the perovskite crystal has a thickness of more than 1 cm, is used as an absorption and conversion layer of gamma photons, and improves the gamma ray detection sensitivity by utilizing the absorption coefficient of the perovskite crystal to gamma photons and the carrier transport property of the perovskite crystal.
Further, the process method is a template method, comprising the following steps:
step 1, growing perovskite crystals in a vacuum freeze-drying experimental device by adopting a variable temperature method or a reverse temperature method;
step 2, forming a penetrating hollow pore canal in the perovskite crystal by controlling the pressure of a growth system;
and 3, taking out the perovskite crystal in the step 2, immersing the perovskite crystal in a precursor liquid at normal temperature and normal pressure, growing the perovskite crystal for the second time by a temperature changing method or an inverse temperature method, filling the hollow pore canal of the first time growing template with the perovskite crystal grown for the second time, and forming the anisotropic perovskite crystal by the template grown for the first time and the perovskite crystal column grown for the second time.
Further, the process method is a directional irradiation method, comprising the following steps:
step 1, preparing an ultra-thick perovskite single crystal by adopting a conventional reverse temperature or variable temperature method, and arranging a mask plate prepared by heavy metals at the top end of the perovskite single crystal;
and 2, processing the perovskite crystal by using high-dose-rate radiation through the mask.
Further, the process is a heteroepitaxy process in which a heterometal salt is added to the precursor solution during the growth of the crystal in solution to form heteroepitaxial channels in the crystal.
The perovskite anisotropy enhanced high-resolution gamma ray imaging method has the following advantages:
1. the invention utilizes the anisotropy of perovskite crystals, and increases the recombination probability of transverse diffusion electron/hole pairs by reducing the mobility of transverse carriers and shortening the service life of carriers, thereby reducing the signal crosstalk between pixel electrodes. The scheme solves the problems that in the conventional gamma ray detection structure, the structure change of the end surface electrode is insensitive to the regulation and control of the edge field, and the crosstalk of the adjacent pixel electrode is not enough. In addition, as the thickness of perovskite crystal increases, the suppression effect of anisotropic electrical performance on transverse diffusion carrier signal crosstalk is more enhanced, and the conventional gamma-ray detection structure is opposite to the suppression effect.
2. In the technical scheme provided by the invention, the longitudinal carrier transmission performance of the perovskite crystal is basically maintained unchanged. Therefore, other properties of gamma ray detection, such as detection sensitivity, energy resolution, and response speed, can be maintained substantially unchanged while reducing signal crosstalk caused by lateral carrier diffusion.
Drawings
FIG. 1 is a schematic diagram of a conventional gamma ray detection structure;
FIG. 1 (a) is a schematic diagram of fluorescence scattering in an indirect detection structure;
FIG. 1 (b) is a schematic diagram of lateral carrier diffusion caused by a fringe field in a direct-detection structure;
FIG. 2 (a) is a schematic diagram of growing perovskite crystals with higher defect density in a vacuum freeze-drying environment and forming hollow channels;
FIG. 2 (b) is a schematic view of a perovskite crystal with low defect density grown for the second time at normal pressure, and a perovskite crystal column is formed along a hollow pore canal;
FIG. 2 (c) is a schematic diagram of a gamma ray imaging device with top and bottom pixelated electrodes;
FIG. 3 (a) is a schematic illustration of the application of high dose rate gamma radiation to perovskite crystals through a heavy metal reticle;
FIG. 3 (b) is a schematic diagram showing the enhancement of anisotropy due to perovskite crystal lattice distortion after high dose rate gamma ray irradiation;
FIG. 4 is a schematic diagram of enhancing the anisotropy of perovskite crystals by suppressing epitaxy;
FIG. 5 is a schematic diagram showing the reduction of spatial resolution caused by lateral diffusion of carriers in a conventional gamma-ray detection imaging structure;
fig. 6 is a schematic diagram of the principle of the invention for increasing the lateral diffusion photo-generated carrier recombination by anisotropic perovskite crystals.
The figure indicates: 1. a first perovskite crystal; 2. a hollow duct; 3. perovskite crystal columns; 4. a common electrode; 5. a pixel electrode; 6. a line of radiation; 7. masking plate; 8. a second perovskite crystal; 9. lattice distortion; 10. a third perovskite crystal; 11. a heteroepitaxial channel; 12. gamma photons; 13. a fourth perovskite crystal; 14. a fringe electric field; 15. photo-generated carriers; 16. a row driving circuit; 17. an analog-to-digital converter; 18. an input channel; 19. an output channel; 20. a fifth perovskite crystal; 21. gamma ray photons; 22. a scintillator; 23. flashing fluorescence; 24, a step of detecting the position of the base; a visible light detector; 25. expanding fluorescent light spots; 26. an active material layer; 27. charge crosstalk.
Detailed Description
For a better understanding of the objects, structures and functions of the present invention, a method of perovskite anisotropy enhanced high resolution gamma ray imaging is described in further detail below with reference to the accompanying drawings.
The invention first prepares anisotropic perovskite crystals. The anisotropic perovskite crystal has high longitudinal carrier mobility and long carrier life; the perovskite crystal has small transverse carrier mobility and short carrier life. And respectively depositing a top electrode and a bottom electrode on the upper end face and the lower end face of the anisotropic perovskite crystal by a vapor deposition method and the like, and applying bias voltages to the top electrode and the bottom electrode to form a bias electric field. When gamma photons are incident, they are absorbed by the anisotropic perovskite crystal, generating photogenerated carriers (electron/hole pairs). The photo-generated electron/hole pairs form drifting movement under the action of the bias electric field, and as the anisotropic perovskite crystal has high longitudinal carrier mobility and long carrier service life, the probability of generating recombination in the longitudinal photo-generated carriers is small, and most of photo-generated carriers can be received by the electrodes to form detection electric signals. In addition to the longitudinal drift motion, the photogenerated carriers are subjected to fringing electric fields, which also produce lateral diffusion. Because the anisotropic perovskite crystal has low transverse carrier mobility and short service life, the probability of generating recombination between laterally diffused photogenerated electrons and photogenerated holes is high, and the number of crosstalk photogenerated carriers received by adjacent electrodes is reduced, so that the resolution of gamma ray imaging can be improved.
The first example employs a templating process to prepare anisotropic perovskite crystals. As shown in fig. 2 (a), first perovskite crystal 1 was grown by a temperature-changing method or an inverse temperature method in an experimental apparatus for vacuum freeze-drying. Since the saturation concentration of the perovskite precursor liquid is relatively low at a low pressure, the growth rate of the first perovskite crystal 1 is relatively fast. However, the grown first perovskite crystal 1 has more defects, small carrier mobility and short carrier life. By controlling the pressure of the growth system, a plurality of through hollow channels 2 can be formed in the first perovskite crystal 1. The first perovskite crystal 1 is taken out, immersed in a precursor solution at normal temperature and normal pressure, and the first perovskite crystal 1 is grown for the second time by a temperature-changing method or an inverse temperature method, as shown in fig. 2 (b). The first perovskite crystal 1 fills the hollow pore canal 2 of the first growth template to form a perovskite crystal column 3. Since the first perovskite crystal 1 is grown under normal pressure for the second time, the first perovskite crystal 1 has a lower growth rate but fewer defects. Therefore, the perovskite crystal column 3 has high carrier mobility and long carrier life. Finally, as shown in fig. 2 (c), an anisotropic photon absorber is formed by the first perovskite crystal 1 with low carrier mobility and the perovskite crystal column 3 with high carrier mobility, and the common electrode 4 and the pixel electrode 5 are deposited on the top surface and the bottom surface of the anisotropic photon absorber by an evaporation method, so that a perovskite crystal gamma ray imaging device is formed.
The second embodiment adopts a directional irradiation method to prepare anisotropic perovskite crystals. As shown in fig. 3 (a). First, a conventional reverse temperature or variable temperature method is adopted to prepare an ultra-thick second perovskite crystal 8, and the second perovskite crystal 8 is an isotropic crystal. Then, a mask 7 prepared by heavy metal is arranged at the top end of the second perovskite crystal 8, and the second perovskite crystal 8 is subjected to aftertreatment by using high-dose-rate radiation rays 6 (such as gamma rays) to penetrate through the mask 7. As shown in fig. 3 (b), the second perovskite crystal 8 may generate lattice distortion 9 under the effect of the high dose rate radiation line 6, and even defects such as dislocation, fracture, etc. may occur, thereby enhancing the anisotropy of the second perovskite crystal 8.
The third example uses a heteroepitaxial process to produce anisotropic perovskite crystals as shown in fig. 4. During the solution growth of the third perovskite crystal 10, a suitable amount of heteroepitaxial metal salt is added to the precursor solution to form a number of heteroepitaxial channels 11 in the crystal. We can use this method to form CdS channel in CdSe crystal and AlN channel in GaN crystal, MAPbBr 3 PbS channels and the like are formed in the crystal. Since the lattice type and lattice constant of the heteroepitaxial channels 11 are different from those of the third perovskite crystal 10, mobility and lifetime of carriers in these channels are changed, and thus anisotropy of the perovskite crystal can be enhanced by the heteroepitaxial channel method.
The structure of a conventional perovskite gamma ray imaging device is shown in fig. 5, which adopts an isotropic fourth perovskite crystal 13 as a gamma ray photon absorber, wherein a common electrode 4 is prepared on the top surface of the photon absorber by evaporation or sputtering and the like, and an array pixel electrode 5 is prepared on the bottom surface of the photon absorber by evaporation or sputtering and is connected with an array readout circuit formed by a thin film transistor or a field effect transistor. A line driving circuit 16 and an analog-to-digital converter 17 are provided around the display device, and a control signal is input through an input channel 18 to output gamma-ray image data through an output channel 19. Due to the structural features of the common electrode 4 and the pixel electrode 5, a fringe electric field 14 is formed in the detection unit. When the high energy gamma photon 12 is incident, a photo-generated carrier 15 (electron/hole pair) is generated in the perovskite crystal. The photo-generated carriers 15 generate lateral diffusion of carriers under the action of the fringe electric field 14, thereby causing a decrease in gamma ray imaging resolution.
Fig. 6 is a high resolution gamma ray imaging device according to the present invention employing an anisotropic fifth perovskite crystal 20 instead of an isotropic perovskite crystal as compared to the conventional imaging device of fig. 5. Although the fringe field 14 is still present, laterally diffused photogenerated carriers 15 (electron/hole pairs) are recombined before reaching the collection electrode, without generating cross-talk electrical signals, due to low carrier mobility with carrier lateral drift, short lifetime. Therefore, the invention reduces signal crosstalk between different pixels and improves imaging resolution.
It will be understood that the invention has been described in terms of several embodiments, and that various changes and equivalents may be made to these features and embodiments by those skilled in the art without departing from the spirit and scope of the invention. In addition, many modifications may be made to adapt a particular situation or material to the teachings of the invention without departing from the essential scope thereof. Therefore, it is intended that the invention not be limited to the particular embodiment disclosed, but that the invention will include all embodiments falling within the scope of the appended claims.
Claims (2)
1. A perovskite anisotropic enhanced high-resolution gamma ray imaging method is characterized in that,
the method comprises the following steps:
step one, adopting a process method to treat the perovskite crystal so that anisotropy of the structure and the electrical property of the perovskite crystal appears;
utilizing anisotropy of perovskite crystals to enable photo-generated carriers generated by gamma ray photons to be transmitted longitudinally and rapidly to form effective detection electric signals, enabling the photo-generated carriers to be low in transverse transmission speed and short in service life, enabling the photo-generated carriers which are diffused transversely to be compounded before reaching electrodes, reducing transverse charge crosstalk between adjacent electrodes and improving gamma ray imaging resolution;
the process method comprises a template method or a directional irradiation method;
the template method comprises the following steps:
step 1, growing perovskite crystals in a vacuum freeze-drying experimental device by adopting a variable temperature method or a reverse temperature method;
step 2, forming a penetrating hollow pore canal in the perovskite crystal by controlling the pressure of a growth system;
step 3, taking out the perovskite crystal in the step 2, immersing the perovskite crystal in a precursor liquid at normal temperature and normal pressure, growing the perovskite crystal for the second time through a temperature changing method or a reverse temperature method, filling the hollow pore canal of the first time growing template with the perovskite crystal grown for the second time, and forming an anisotropic perovskite crystal by the template grown for the first time and the perovskite crystal column grown for the second time;
the directional irradiation method comprises the following steps:
step 1, preparing an ultra-thick perovskite single crystal by adopting a conventional reverse temperature or variable temperature method, and arranging a mask plate prepared by heavy metals at the top end of the perovskite single crystal;
and 2, processing the perovskite crystal by using high-dose-rate radiation through the mask.
2. The perovskite anisotropic enhanced high resolution gamma ray imaging method as claimed in claim 1, wherein the perovskite crystal has a thickness of more than 1 cm and is used as an absorption and conversion layer of gamma photons, and the gamma ray detection sensitivity is improved by using an absorption coefficient of the perovskite crystal to gamma photons and a carrier transport property of the perovskite crystal.
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| CN111554813A (en) * | 2020-05-11 | 2020-08-18 | 吉林大学 | Controllable growth method of dodecahedral methylamine lead bromide perovskite monocrystal [110] crystal face and application of X-ray detector of dodecahedral methylamine lead bromide perovskite monocrystal |
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| CN111554813A (en) * | 2020-05-11 | 2020-08-18 | 吉林大学 | Controllable growth method of dodecahedral methylamine lead bromide perovskite monocrystal [110] crystal face and application of X-ray detector of dodecahedral methylamine lead bromide perovskite monocrystal |
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