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Title: Single-Crystal Thin Films of Cesium Lead Bromide Perovskite Epitaxially Grown on Metal Oxide Perovskite (SrTiO 3)

Abstract

High-quality metal halide perovskite single crystals have low defect densities and excellent photophysical properties, yet thin films are the most sought after material geometry for optoelectronic devices. Perovskite single-crystal thin films (SCTFs) would be highly desirable for high-performance devices, but their growth remains challenging, particularly for inorganic metal halide perovskites. Herein, we report the facile vapor-phase epitaxial growth of cesium lead bromide perovskite (CsPbBr 3) continuous SCTFs with controllable micrometer thickness, as well as nanoplate arrays, on traditional oxide perovskite SrTiO 3(100) substrates. Heteroepitaxial single-crystal growth is enabled by the serendipitous incommensurate lattice match between these two perovskites, and overcoming the limitation of island-forming Volmer–Weber crystal growth is critical for growing large-area continuous thin films. Time-resolved photoluminescence, transient reflection spectroscopy, and electrical transport measurements show that the CsPbBr 3 epitaxial thin film has a slow charge carrier recombination rate, low surface recombination velocity (10 4 cm s –1), and low defect density of 10 12 cm –3, which are comparable to those of CsPbBr 3 single crystals. This work suggests a general approach using oxide perovskites as substrates for heteroepitaxial growth of halide perovskites. Furthermore, the high-quality halide perovskite SCTFs epitaxially integrated with multifunctional oxide perovskites could open up opportunitiesmore » for a variety of high-performance optoelectronics devices.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2];  [3];  [2];  [2]; ORCiD logo [2];  [2];  [3];  [2];  [2];  [4]; ORCiD logo [4]; ORCiD logo [3];  [2]; ORCiD logo [2]
  1. Univ. of Wisconsin-Madison, Madison, WI (United States); Xi'an Jiaotong Univ., Shaanxi (People's Republic of China)
  2. Univ. of Wisconsin-Madison, Madison, WI (United States)
  3. Hunan Univ., Changsha (People's Republic of China)
  4. Xi'an Jiaotong Univ., Shaanxi (People's Republic of China)
Publication Date:
Research Org.:
Univ. of Wisconsin-Madison, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1390338
Grant/Contract Number:
FG02-09ER46664; SC0002162
Resource Type:
Journal Article: Published Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 38; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Chen, Jie, Morrow, Darien J., Fu, Yongping, Zheng, Weihao, Zhao, Yuzhou, Dang, Lianna, Stolt, Matthew J., Kohler, Daniel D., Wang, Xiaoxia, Czech, Kyle J., Hautzinger, Matthew P., Shen, Shaohua, Guo, Liejin, Pan, Anlian, Wright, John C., and Jin, Song. Single-Crystal Thin Films of Cesium Lead Bromide Perovskite Epitaxially Grown on Metal Oxide Perovskite (SrTiO3). United States: N. p., 2017. Web. doi:10.1021/jacs.7b07506.
Chen, Jie, Morrow, Darien J., Fu, Yongping, Zheng, Weihao, Zhao, Yuzhou, Dang, Lianna, Stolt, Matthew J., Kohler, Daniel D., Wang, Xiaoxia, Czech, Kyle J., Hautzinger, Matthew P., Shen, Shaohua, Guo, Liejin, Pan, Anlian, Wright, John C., & Jin, Song. Single-Crystal Thin Films of Cesium Lead Bromide Perovskite Epitaxially Grown on Metal Oxide Perovskite (SrTiO3). United States. doi:10.1021/jacs.7b07506.
Chen, Jie, Morrow, Darien J., Fu, Yongping, Zheng, Weihao, Zhao, Yuzhou, Dang, Lianna, Stolt, Matthew J., Kohler, Daniel D., Wang, Xiaoxia, Czech, Kyle J., Hautzinger, Matthew P., Shen, Shaohua, Guo, Liejin, Pan, Anlian, Wright, John C., and Jin, Song. 2017. "Single-Crystal Thin Films of Cesium Lead Bromide Perovskite Epitaxially Grown on Metal Oxide Perovskite (SrTiO3)". United States. doi:10.1021/jacs.7b07506.
@article{osti_1390338,
title = {Single-Crystal Thin Films of Cesium Lead Bromide Perovskite Epitaxially Grown on Metal Oxide Perovskite (SrTiO3)},
author = {Chen, Jie and Morrow, Darien J. and Fu, Yongping and Zheng, Weihao and Zhao, Yuzhou and Dang, Lianna and Stolt, Matthew J. and Kohler, Daniel D. and Wang, Xiaoxia and Czech, Kyle J. and Hautzinger, Matthew P. and Shen, Shaohua and Guo, Liejin and Pan, Anlian and Wright, John C. and Jin, Song},
abstractNote = {High-quality metal halide perovskite single crystals have low defect densities and excellent photophysical properties, yet thin films are the most sought after material geometry for optoelectronic devices. Perovskite single-crystal thin films (SCTFs) would be highly desirable for high-performance devices, but their growth remains challenging, particularly for inorganic metal halide perovskites. Herein, we report the facile vapor-phase epitaxial growth of cesium lead bromide perovskite (CsPbBr3) continuous SCTFs with controllable micrometer thickness, as well as nanoplate arrays, on traditional oxide perovskite SrTiO3(100) substrates. Heteroepitaxial single-crystal growth is enabled by the serendipitous incommensurate lattice match between these two perovskites, and overcoming the limitation of island-forming Volmer–Weber crystal growth is critical for growing large-area continuous thin films. Time-resolved photoluminescence, transient reflection spectroscopy, and electrical transport measurements show that the CsPbBr3 epitaxial thin film has a slow charge carrier recombination rate, low surface recombination velocity (104 cm s–1), and low defect density of 1012 cm–3, which are comparable to those of CsPbBr3 single crystals. This work suggests a general approach using oxide perovskites as substrates for heteroepitaxial growth of halide perovskites. Furthermore, the high-quality halide perovskite SCTFs epitaxially integrated with multifunctional oxide perovskites could open up opportunities for a variety of high-performance optoelectronics devices.},
doi = {10.1021/jacs.7b07506},
journal = {Journal of the American Chemical Society},
number = 38,
volume = 139,
place = {United States},
year = 2017,
month = 9
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/jacs.7b07506

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Cited by: 2works
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  • High-quality metal halide perovskite single crystals have low defect densities and excellent photophysical properties, yet thin films are the most sought after material geometry for optoelectronic devices. Perovskite single-crystal thin films (SCTFs) would be highly desirable for high-performance devices, but their growth remains challenging, particularly for inorganic metal halide perovskites. Herein, we report the facile vapor-phase epitaxial growth of cesium lead bromide perovskite (CsPbBr 3) continuous SCTFs with controllable micrometer thickness, as well as nanoplate arrays, on traditional oxide perovskite SrTiO 3(100) substrates. Heteroepitaxial single-crystal growth is enabled by the serendipitous incommensurate lattice match between these two perovskites, and overcomingmore » the limitation of island-forming Volmer–Weber crystal growth is critical for growing large-area continuous thin films. Time-resolved photoluminescence, transient reflection spectroscopy, and electrical transport measurements show that the CsPbBr 3 epitaxial thin film has a slow charge carrier recombination rate, low surface recombination velocity (10 4 cm s –1), and low defect density of 10 12 cm –3, which are comparable to those of CsPbBr 3 single crystals. This work suggests a general approach using oxide perovskites as substrates for heteroepitaxial growth of halide perovskites. Furthermore, the high-quality halide perovskite SCTFs epitaxially integrated with multifunctional oxide perovskites could open up opportunities for a variety of high-performance optoelectronics devices.« less
  • Normal-metal/insulator/superconductor (NIS) junctions were fabricated using thin films of YBa/sub 2/Cu/sub 3/O/sub 7-//sub x/ (YBCO) or ErBa/sub 2/Cu/sub 3/O/sub 7-//sub x/. These were epitaxially grown on single-crystal SrTiO/sub 3/ by the activated reactive evaporation method. For some NIS junctions prepared on SrTiO/sub 3/ (110) substrates, we observed multipeaks in the differential conductance versus voltage curve. NIS junctions using single-crystal YBCO films on SrTiO/sub 3/ (100) showed a set of peaks, from which we obtained a gap parameter of 11.5 +- 1.5 meV at 4.4 K and a coupling constant of 3.2 +- 0.4.
  • L1{sub 0}–FePt(001) single-crystal films were grown epitaxially on SrTiO{sub 3}(001), MgAl{sub 2}O{sub 4}(001), and MgO(001) substrates. Their uniaxial magnetic anisotropy K{sub u} and the order structure were examined for the film thickness t range of 2–14 nm. All series of films show large K{sub u} of 4 × 10{sup 7} erg/cm{sup 3} in the thickness range higher than 10 nm, with order parameter S of 0.8 and saturation magnetization M{sub s} of 1120 emu/cm{sup 3}. K{sub u} decreased gradually as t decreased. The K{sub u} reduction was considerable when t decreased from 4 nm to 2 nm. No marked difference in the thickness dependence of K{sub u} wasmore » found in any series of films, although the lattice mismatch between FePt and the substrates was markedly different. K{sub u} reduction showed good agreement with the reduction of S for the films on MgAl{sub 2}O{sub 4} and MgO. The K{sub u} ∼ S{sup 2} plot showed an almost linear relation, which is in good agreement with theoretical predictions. Transmission electron microscopy images for a FePt film on MgO substrate revealed that the lattice mismatch between FePt(001) and MgO(001) was relaxed in the initial 1 or 2 layers of FePt(001) lattices, which is likely to be true also for two other series of films.« less
  • Ni(1120) epitaxial thin films with hcp structure were prepared on Au(100) single-crystal underlayers at 100 deg. C by ultra high vacuum molecular beam epitaxy. The detailed film structure is studied by in situ reflection high energy electron diffraction, x-ray diffraction, and transmission electron microscopy. The hcp-Ni film consists of two types of variants whose c-axes are rotated around the film normal by 90 deg. each other. An atomically sharp boundary is recognized between the film and the underlayer, where misfit dislocations are introduced. Presence of such dislocations seems to relieve the strain caused by the lattice mismatch between the filmmore » and the underlayer.« less