J. Semicond. > 2022, Volume 43 > Issue 7 > 070202

RESEARCH HIGHLIGHTS

Perovskite films for X-ray detection

Pei Yuan1, Lixiu Zhang2, Menghua Zhu1, and Liming Ding2,

+ Author Affiliations

 Corresponding author: Menghua Zhu, mhzhu@nwpu.edu.cn; Liming Ding, ding@nanoctr.cn

DOI: 10.1088/1674-4926/43/7/070202

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X-ray detection is widely used in research[1-3], product inspection[4], nuclear station, and medical imaging. Si[5], α-Se[6], PbI2[7], and CdZnTe[8] are conventional semiconductors, and some problems limit their applications. For instance, Si and α-Se have low stopping power for X-ray[8], which hinders their application in high-energy range over 50 keV. Moreover, the complicated preparation, high operating voltage, and high fabrication cost of these materials are the negative issues.

Perovskite materials are promising candidates for X-ray detection due to facile synthesis[9-14] and large mobility-lifetime (μτ) products for highly sensitive detection. The μτ product of MAPbBr3 single crystal reaches 1.2 × 10–2 cm2 V–1[12], which is comparable to the μτ value of CdZnTe[3]. Perovskite-based X-ray detectors also exhibited a record X-ray sensitivity[15] of ~710 000 μC Gy–1 cm–2 and an ultralow detection limit[16] of 0.62 nGy s–1. Tang et al. developed a hot-pressing method to grow quasi-monocrystalline CsPbBr3 films, which exhibits a superior sensitivity of 55 684 μC Gy–1 cm–2 and a low detection limit of 215 nGy s–1[17]. To date, halide perovskites in various forms like polycrystalline films, single crystals, and nanocrystals have been used in X-ray detectors. Especially, polycrystalline films prepared by hot-pressing, coating or printing have attracted great interests due to their superior flexibility, lightweight and facile synthesis.

In comparison to brittle single-crystal films, polycrystalline films can be curved to fit non-flat substrates, thus showing potential for flexible X-ray detectors[18, 19]. Some high-quality flexible perovskite films were prepared, presenting high performance. Liu et al.[20] reported a flexible and printable X-ray detector based on colloidal CsPbBr3 QDs. To enhance the sensitivity, they effectively reduced the surface defects and tuned crystallinity via chemical engineering. This detector can sense a very low X-ray dose rate (~17.2 µGy s–1) with a high sensitivity of 1450 µC Gy–1 cm–2 at 0.1 V bias. Meanwhile, the vignetting issues can be effectively alleviated, leading to reduced misdiagnosis. 400 cm2 MAPb(I0.9Cl0.1)3-filled nylon membranes were used to make X-ray detectors[21]. The devices exhibited a high sensitivity of ~8696 μC Gy–1 cm–2 and could be bent at 2 mm radius without performance loss (Figs. 1(a)–1(d)).

Fig. 1.  (Color online) (a) Perovskite-filled membrane (PFM). (b) A 400 cm2 nylon membrane without (left) and with (right) perovskites. (c) Current density for the PFM device changes with the dose rate. (d) Dependence of the sensitivity and flexibility of PFM devices on device thicknesses. Inset: the bending of a PFM device. The error bars were obtained from three devices. Reproduced with permission[21], Copyright 2020, Springer Nature. (e) Illustration for an all-solution-processed X-ray detector. (f) Printed MPC on PI-MAPbI3. (g) Signal current and sensitivity change with bias voltage. Reproduced with permission[22], Copyright 2017, Springer Nature.

For polycrystalline films, besides flexibility, the facile preparation of large-area and thick films by solution processing is another advantage over single crystal films. Blade coating is one of the common methods. Kim et al.[22] made a thick polycrystalline MAPbI3 film by this method, and it had excellent optoelectronic properties, which are comparable to single crystal films. The device had a thickness of 830 μm and an active area of ~100 cm2 (Figs. 1(e)–1(g)). In order to minimize dark current drift, the polycrystalline films should have high crystallinity and large grain to reduce grain boundaries. He et al.[23] made a quasi-2D perovskite film with low defects and suppressed ion migration. The average grain size was 31.88 µm. Such large grain size resulted from colloidal particles aggregating in the slurry with PEA+, which can decrease nucleation sites. The resulted µτ value was 2.6 × 10–5 cm2 V–1 and the minimum current drift was 1.5 × 10–2 pA cm–1 s–1 V–1.

The perovskite films should give low dark current to ensure high X-ray sensitivity. The patients under a high level of radiation exposure may face cancer risk[24]. To capture clear X-ray images under a low dose of X-ray is desired[25]. The detection limit is the minimum signal which can be reliably identified by X-ray detectors and is defined as the equivalent dose rate of a signal 3 times greater than the noise. A low detection limit results from high current signal with low noise current dominated by dark current, which can reduce the imaging capability of detectors under weak X-ray. Most polycrystalline perovskite detectors[17, 26] have large dark current densities of 50–500 nA cm–2 under an electrical field of 0.05 V μm–1 due to the defective structures as compared to single crystals. To solve this problem, great efforts have been devoted to improve the quality of perovskite films. Zhou et al.[27] reported a heterojunction structure formed by laminating membranes filled with perovskites with different bandgaps. The membranes reduced dark current density of the devices by over 200 times without compromising their sensitivity. They captured clear X-ray images at a low dose rate of 32.2 nGy s–1 (Figs. 2(a)–2(c)). Tang et al.[23] also proposed a new strategy to suppress ion migration by inserting 2D Ruddlesden-Popper layer into 3D perovskite film. The quasi-2D perovskite X-ray detector offered a sensitivity of 10 860 µC Gy–1 cm–2 with a stable dark current.

Fig. 2.  (Color online) (a) The lamination technique. (b) Heterojunction perovskite film. (c) Response of single-composition and heterojunction perovskite detectors. Reproduced with permission[27], Copyright 2021, AAAS. (d) Wet film fabrication by spin-coating or blade-coating. (e) The ALS method. (f) The nucleation and growth process in (d). (g) Nucleation and growth process in ALS method. Reproduced with permission[30], Copyright 2021, Elsevier.

Generally, perovskite films should have a thickness of hundreds micrometers for sufficient X-ray absorption[28]. However, it is very difficult to make such films by spin-coating or blade-coating methods. First, it is difficult to deposit a very thick wet film due to the limitations of surface tension and viscosity[29]. Second, even though a thick wet film could be made, it is still difficult to obtain perovskite films with high crystallinity and low defect density (Figs. 2(d) and 2(f)). To solve this issue, Wei et al.[30] developed an aerosol–liquid–solid (ALS) method to make perovskite films on TFT substrates by spray coating. This method solved the problem of uncontrolled crystallization of perovskites (Figs. 2(e) and 2(g)). The detectors demonstrated a high sensitivity (~1.48 × 105 μC Gy–1 cm–2), a low detection limit (280 nGy s–1), and they could also realize high-resolution imaging.

In summary, high-quality perovskite films featuring large area, sufficient thickness, flexibility and high sensitivity are prerequisites for high-performance X-ray detectors. Perovskite X-ray detectors may find applications in security inspection, medical imaging, and nondestructive checking in the future.

M. Zhu thanks the National Natural Science Foundation of China (62104194) for financial support. L. Ding thanks the National Key Research and Development Program of China (2017YFA0206600), the National Natural Science Foundation of China (51922032 and 21961160720), and the open research fund of Songshan Lake Materials Laboratory (2021SLABFK02) for financial support.



[1]
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[2]
Wu H, Ge Y, Niu G, et al. Metal halide perovskites for X-ray detection and imaging. Matter, 2021, 4, 144 doi: 10.1016/j.matt.2020.11.015
[3]
Wei H, Huang J. Halide lead perovskites for ionizing radiation detection. Nat Commun, 2019, 10, 1066 doi: 10.1038/s41467-019-08981-w
[4]
Olivo A, Chana D, Speller R. A preliminary investigation of the potential of phase contrast X-ray imaging in the field of homeland security. J Phys D, 2008, 41, 225503 doi: 10.1088/0022-3727/41/22/225503
[5]
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[6]
Kasap S. X-ray sensitivity of photoconductors: application to stabilized α-Se. J Phys D, 2000, 33, 2853 doi: 10.1088/0022-3727/33/21/326
[7]
Street R, Ready S, Van Schuylenbergh K, et al. Comparison of PbI2 and HgI2 for direct detection active matrix X-ray image sensors. J Appl Phys, 2002, 91, 3345 doi: 10.1063/1.1436298
[8]
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[9]
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[10]
Yakunin S, Dirin D N, Shynkarenko Y, et al. Detection of gamma photons using solution-grown single crystals of hybrid lead halide perovskites. Nat Photonics, 2016, 10, 585 doi: 10.1038/nphoton.2016.139
[11]
Huang J, Yuan Y, Shao Y, et al. Understanding the physical properties of hybrid perovskites for photovoltaic applications. Nat Rev Mater, 2017, 2, 17042 doi: 10.1038/natrevmats.2017.42
[12]
Wei H, Fang Y, Mulligan P, et al. Sensitive X-ray detectors made of methylammonium lead tribromide perovskite single crystals. Nat Photonics, 2016, 10, 333 doi: 10.1038/nphoton.2016.41
[13]
Zhou F, Li Z, Lan W, et al. Halide perovskite, a potential scintillator for X-ray detection. Small Methods, 2020, 4, 2000506 doi: 10.1002/smtd.202000506
[14]
Li C, Ma Y, Xiao Y, et al. Advances in perovskite photodetectors. InfoMat, 2020, 2, 1247 doi: 10.1002/inf2.12141
[15]
Song Y, Li L, Bi W, et al. Atomistic surface passivation of CH3NH3PbI3 perovskite single crystals for highly sensitive coplanar-structure X-ray detectors. Research, 2020, 2020, 5958243 doi: 10.34133/2020/5958243
[16]
Zheng X, Zhao W, Wang P, et al. Ultrasensitive and stable X-ray detection using zero-dimensional lead-free perovskites. J Energy Chem, 2020, 49, 299 doi: 10.1016/j.jechem.2020.02.049
[17]
Pan W, Yang B, Niu G, et al. Hot-pressed CsPbBr3 quasi-monocrystalline film for sensitive direct X-ray detection. Adv Mater, 2019, 31, 1904405 doi: 10.1002/adma.201904405
[18]
Thirimanne H, Jayawardena K, Parnell A, et al. High sensitivity organic inorganic hybrid X-ray detectors with direct transduction and broadband response. Nat Commun, 2018, 9, 2926 doi: 10.1038/s41467-018-05301-6
[19]
Demchyshyn S, Verdi M, Basirico L, et al. Designing ultraflexible perovskite X-ray detectors through interface engineering. Adv Sci, 2020, 7, 2002586 doi: 10.1002/advs.202002586
[20]
Liu J, Shabbir B, Wang C, et al. Flexible, printable soft-X-ray detectors based on all-inorganic perovskite quantum dots. Adv Mater, 2019, 31, 1901644 doi: 10.1002/adma.201901644
[21]
Zhao J, Zhao L, Deng Y, et al. Perovskite-filled membranes for flexible and large-area direct-conversion X-ray detector arrays. Nat Photonics, 2020, 14, 612 doi: 10.1038/s41566-020-0678-x
[22]
Kim Y C, Kim K H, Son D Y, et al. Printable organometallic perovskite enables large-area, low-dose X-ray imaging. Nature, 2017, 550, 87 doi: 10.1038/nature24032
[23]
He X, Xia M, Wu H, et al. Quasi-2D perovskite thick film for X-ray detection with low detection limit. Adv Funct Mater, 2021, 32, 2109458 doi: 10.1002/adfm.202109458
[24]
Datta A, Zhong Z, Motakef S. A new generation of direct X-ray detectors for medical and synchrotron imaging applications. Sci Rep, 2020, 10, 20097 doi: 10.1038/s41598-020-76647-5
[25]
Brenner D J, Elliston C D, Hall E J, et al. Estimated risks of radiation-induced fatal cancer from pediatric CT. Am J Roentgenol, 2001, 176, 289 doi: 10.2214/ajr.176.2.1760289
[26]
Yang B, Pan W, Wu H, et al. Heteroepitaxial passivation of Cs2AgBiBr6 wafers with suppressed ionic migration for X-ray imaging. Nat Commun, 2019, 10, 1989 doi: 10.1038/s41467-018-07882-8
[27]
Zhou Y, Zhao L, Ni Z, et al. Heterojunction structures for reduced noise in large-area and sensitive perovskite X-ray detectors. Sci Adv, 2021, 7, eabg6716 doi: 10.1126/sciadv.abg6716
[28]
Gill H S, Elshahat B, Kokil A, et al. Flexible perovskite based X-ray detectors for dose monitoring in medical imaging applications. Phys Med, 2018, 5, 20 doi: 10.1016/j.phmed.2018.04.001
[29]
Chen S, Xiao X, Chen B, et al. Crystallization in one-step solution deposition of perovskite films: Upward or downward. Sci Adv, 2021, 7, eabb2412 doi: 10.1126/sciadv.abb2412
[30]
Qian W, Xu X, Wang J, et al. An aerosol-liquid-solid process for the general synthesis of halide perovskite thick films for direct-conversion X-ray detectors. Matter, 2021, 4, 942 doi: 10.1016/j.matt.2021.01.020
Fig. 1.  (Color online) (a) Perovskite-filled membrane (PFM). (b) A 400 cm2 nylon membrane without (left) and with (right) perovskites. (c) Current density for the PFM device changes with the dose rate. (d) Dependence of the sensitivity and flexibility of PFM devices on device thicknesses. Inset: the bending of a PFM device. The error bars were obtained from three devices. Reproduced with permission[21], Copyright 2020, Springer Nature. (e) Illustration for an all-solution-processed X-ray detector. (f) Printed MPC on PI-MAPbI3. (g) Signal current and sensitivity change with bias voltage. Reproduced with permission[22], Copyright 2017, Springer Nature.

Fig. 2.  (Color online) (a) The lamination technique. (b) Heterojunction perovskite film. (c) Response of single-composition and heterojunction perovskite detectors. Reproduced with permission[27], Copyright 2021, AAAS. (d) Wet film fabrication by spin-coating or blade-coating. (e) The ALS method. (f) The nucleation and growth process in (d). (g) Nucleation and growth process in ALS method. Reproduced with permission[30], Copyright 2021, Elsevier.

[1]
Zhou Y, Chen J, Bakr O M, et al. Metal halide perovskites for X-ray imaging scintillators and detectors. ACS Energy Lett, 2021, 6, 739 doi: 10.1021/acsenergylett.0c02430
[2]
Wu H, Ge Y, Niu G, et al. Metal halide perovskites for X-ray detection and imaging. Matter, 2021, 4, 144 doi: 10.1016/j.matt.2020.11.015
[3]
Wei H, Huang J. Halide lead perovskites for ionizing radiation detection. Nat Commun, 2019, 10, 1066 doi: 10.1038/s41467-019-08981-w
[4]
Olivo A, Chana D, Speller R. A preliminary investigation of the potential of phase contrast X-ray imaging in the field of homeland security. J Phys D, 2008, 41, 225503 doi: 10.1088/0022-3727/41/22/225503
[5]
Guerra M, Manso M, Longelin S, et al. Performance of three different Si X-ray detectors for portable XRF spectrometers in cultural heritage applications. J Instrum, 2012, 7, C10004 doi: 10.1088/1748-0221/7/10/C10004
[6]
Kasap S. X-ray sensitivity of photoconductors: application to stabilized α-Se. J Phys D, 2000, 33, 2853 doi: 10.1088/0022-3727/33/21/326
[7]
Street R, Ready S, Van Schuylenbergh K, et al. Comparison of PbI2 and HgI2 for direct detection active matrix X-ray image sensors. J Appl Phys, 2002, 91, 3345 doi: 10.1063/1.1436298
[8]
Del Sordo S, Abbene L, Caroli E, et al. Progress in the development of CdTe and CdZnTe semiconductor radiation detectors for astrophysical and medical applications. Sensors, 2009, 9, 3491 doi: 10.3390/s90503491
[9]
Su Y, Ma W, Yang Y M. Perovskite semiconductors for direct X-ray detection and imaging. J Semicond, 2020, 41, 051204 doi: 10.1088/1674-4926/41/5/051204
[10]
Yakunin S, Dirin D N, Shynkarenko Y, et al. Detection of gamma photons using solution-grown single crystals of hybrid lead halide perovskites. Nat Photonics, 2016, 10, 585 doi: 10.1038/nphoton.2016.139
[11]
Huang J, Yuan Y, Shao Y, et al. Understanding the physical properties of hybrid perovskites for photovoltaic applications. Nat Rev Mater, 2017, 2, 17042 doi: 10.1038/natrevmats.2017.42
[12]
Wei H, Fang Y, Mulligan P, et al. Sensitive X-ray detectors made of methylammonium lead tribromide perovskite single crystals. Nat Photonics, 2016, 10, 333 doi: 10.1038/nphoton.2016.41
[13]
Zhou F, Li Z, Lan W, et al. Halide perovskite, a potential scintillator for X-ray detection. Small Methods, 2020, 4, 2000506 doi: 10.1002/smtd.202000506
[14]
Li C, Ma Y, Xiao Y, et al. Advances in perovskite photodetectors. InfoMat, 2020, 2, 1247 doi: 10.1002/inf2.12141
[15]
Song Y, Li L, Bi W, et al. Atomistic surface passivation of CH3NH3PbI3 perovskite single crystals for highly sensitive coplanar-structure X-ray detectors. Research, 2020, 2020, 5958243 doi: 10.34133/2020/5958243
[16]
Zheng X, Zhao W, Wang P, et al. Ultrasensitive and stable X-ray detection using zero-dimensional lead-free perovskites. J Energy Chem, 2020, 49, 299 doi: 10.1016/j.jechem.2020.02.049
[17]
Pan W, Yang B, Niu G, et al. Hot-pressed CsPbBr3 quasi-monocrystalline film for sensitive direct X-ray detection. Adv Mater, 2019, 31, 1904405 doi: 10.1002/adma.201904405
[18]
Thirimanne H, Jayawardena K, Parnell A, et al. High sensitivity organic inorganic hybrid X-ray detectors with direct transduction and broadband response. Nat Commun, 2018, 9, 2926 doi: 10.1038/s41467-018-05301-6
[19]
Demchyshyn S, Verdi M, Basirico L, et al. Designing ultraflexible perovskite X-ray detectors through interface engineering. Adv Sci, 2020, 7, 2002586 doi: 10.1002/advs.202002586
[20]
Liu J, Shabbir B, Wang C, et al. Flexible, printable soft-X-ray detectors based on all-inorganic perovskite quantum dots. Adv Mater, 2019, 31, 1901644 doi: 10.1002/adma.201901644
[21]
Zhao J, Zhao L, Deng Y, et al. Perovskite-filled membranes for flexible and large-area direct-conversion X-ray detector arrays. Nat Photonics, 2020, 14, 612 doi: 10.1038/s41566-020-0678-x
[22]
Kim Y C, Kim K H, Son D Y, et al. Printable organometallic perovskite enables large-area, low-dose X-ray imaging. Nature, 2017, 550, 87 doi: 10.1038/nature24032
[23]
He X, Xia M, Wu H, et al. Quasi-2D perovskite thick film for X-ray detection with low detection limit. Adv Funct Mater, 2021, 32, 2109458 doi: 10.1002/adfm.202109458
[24]
Datta A, Zhong Z, Motakef S. A new generation of direct X-ray detectors for medical and synchrotron imaging applications. Sci Rep, 2020, 10, 20097 doi: 10.1038/s41598-020-76647-5
[25]
Brenner D J, Elliston C D, Hall E J, et al. Estimated risks of radiation-induced fatal cancer from pediatric CT. Am J Roentgenol, 2001, 176, 289 doi: 10.2214/ajr.176.2.1760289
[26]
Yang B, Pan W, Wu H, et al. Heteroepitaxial passivation of Cs2AgBiBr6 wafers with suppressed ionic migration for X-ray imaging. Nat Commun, 2019, 10, 1989 doi: 10.1038/s41467-018-07882-8
[27]
Zhou Y, Zhao L, Ni Z, et al. Heterojunction structures for reduced noise in large-area and sensitive perovskite X-ray detectors. Sci Adv, 2021, 7, eabg6716 doi: 10.1126/sciadv.abg6716
[28]
Gill H S, Elshahat B, Kokil A, et al. Flexible perovskite based X-ray detectors for dose monitoring in medical imaging applications. Phys Med, 2018, 5, 20 doi: 10.1016/j.phmed.2018.04.001
[29]
Chen S, Xiao X, Chen B, et al. Crystallization in one-step solution deposition of perovskite films: Upward or downward. Sci Adv, 2021, 7, eabb2412 doi: 10.1126/sciadv.abb2412
[30]
Qian W, Xu X, Wang J, et al. An aerosol-liquid-solid process for the general synthesis of halide perovskite thick films for direct-conversion X-ray detectors. Matter, 2021, 4, 942 doi: 10.1016/j.matt.2021.01.020
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    Pei Yuan, Lixiu Zhang, Menghua Zhu, Liming Ding. Perovskite films for X-ray detection[J]. Journal of Semiconductors, 2022, 43(7): 070202. doi: 10.1088/1674-4926/43/7/070202
    P Yuan, L X Zhang, M H Zhu, L M Ding. Perovskite films for X-ray detection[J]. J. Semicond, 2022, 43(7): 070202. doi: 10.1088/1674-4926/43/7/070202
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    Received: 25 April 2022 Revised: Online: Uncorrected proof: 26 April 2022Published: 01 July 2022

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      Pei Yuan, Lixiu Zhang, Menghua Zhu, Liming Ding. Perovskite films for X-ray detection[J]. Journal of Semiconductors, 2022, 43(7): 070202. doi: 10.1088/1674-4926/43/7/070202 ****P Yuan, L X Zhang, M H Zhu, L M Ding. Perovskite films for X-ray detection[J]. J. Semicond, 2022, 43(7): 070202. doi: 10.1088/1674-4926/43/7/070202
      Citation:
      Pei Yuan, Lixiu Zhang, Menghua Zhu, Liming Ding. Perovskite films for X-ray detection[J]. Journal of Semiconductors, 2022, 43(7): 070202. doi: 10.1088/1674-4926/43/7/070202 ****
      P Yuan, L X Zhang, M H Zhu, L M Ding. Perovskite films for X-ray detection[J]. J. Semicond, 2022, 43(7): 070202. doi: 10.1088/1674-4926/43/7/070202

      Perovskite films for X-ray detection

      DOI: 10.1088/1674-4926/43/7/070202
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      • Pei Yuan:got her BE from Shenyang Jianzhu University in 2021. Now she is a MS student at Northwestern Polytechnical University under the supervision of Prof. Menghua Zhu. Her research focuses on perovskite X-ray detectors
      • Lixiu Zhang:got her BS degree from Soochow University in 2019. Now she is a PhD student at University of Chinese Academy of Sciences under the supervision of Prof. Liming Ding. Her research focuses on innovative materials and devices
      • Menghua Zhu:received her PhD from Harbin Institute of Technology in 2017. She did two-year postdoctoral research at Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology under the supervision of Prof. Jiang Tang. Then she joined School of Materials Science and Engineering, Northwestern Polytechnical University as an associate professor. Her research focuses on new semiconductors for optoelectronic devices
      • Liming Ding:got his PhD from University of Science and Technology of China (was a joint student at Changchun Institute of Applied Chemistry, CAS). He started his research on OSCs and PLEDs in Olle Ingans Lab in 1998. Later on, he worked at National Center for Polymer Research, Wright-Patterson Air Force Base and Argonne National Lab (USA). He joined Konarka as a Senior Scientist in 2008. In 2010, he joined National Center for Nanoscience and Technology as a full professor. His research focuses on innovative materials and devices. He is RSC Fellow, the nominator for Xplorer Prize, and the Associate Editor for Journal of Semiconductors
      • Corresponding author: mhzhu@nwpu.edu.cnding@nanoctr.cn
      • Received Date: 2022-04-25
        Available Online: 2022-04-26

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