On the Origin of Room-Temperature Amplified Spontaneous Emission in CsPbBr3 Single Crystals

Kim, Donggyu; Ryu, Hongsun; Lim, Soo Yeon; McCall, Kyle M.; Park, Jongwoo; Kim, Sungdo; Kim, Tae Jung; Kim, Jeongyong; Kim, Yong Soo; Kanatzidis, Mercouri G.; Cheong, Hyeonsik; Jang, Joon I.

doi:10.1021/acs.chemmater.1c00591

Title: On the Origin of Room-Temperature Amplified Spontaneous Emission in CsPbBr₃ Single Crystals

Journal Article · 17 September 2021 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.1c00591 · OSTI ID:1870317

^[1]; Ryu, Hongsun ^[2]; Lim, Soo Yeon ^[2]; McCall, Kyle M. ^[3]; Park, Jongwoo ^[4];

^[4]; Kim, Tae Jung ^[5];

^[6]; Kim, Yong Soo ^[4];

^[3];

^[2];

^[2]

Sogang Univ. Seoul (Korea, Republic of); Northwestern University
Sogang Univ. Seoul (Korea, Republic of)
Northwestern Univ., Evanston, IL (United States)
Univ. of Ulsan (Korea, Republic of)
Kyung Hee Univ., Seoul (Korea, Republic of)
Sungkyunkwan Univ., Suwon (Republic of Korea)

CsPbBr₃ is an all-inorganic halide perovskite with excellent photoluminescence (PL) properties for laser applications. Amplified spontaneous emission (ASE) is a prerequisite for lasing and typically observed from low-dimensional CsPbBr3 nanostructures, where quantum confinement enhances ASE. However, a gain medium for lasing should be prepared into a robust bulk form that works under intense light illumination. Here, we demonstrate that bulk CsPbBr₃ single crystals exhibit highly efficient ASE with a threshold of 46 MWcm^-2 at 520 nm, if PL reabsorption via the indirect Rashba gap is properly suppressed by thickness control. Based on a series of spectroscopic and microscopic measurements, we show that this below-the-gap absorption can significantly alter the PL feature and even the apparent color of the crystal depending on the crystal size. Our results show that a thin CsPbBr₃ single crystal can be utilized for lasing applications when engineered into a submillimeter thickness for effective light–matter interaction.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Univ. of California, Santa Barbara, CA (United States); Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Research Foundation of Korea (NRF); Ministry of Trade, Industry and Energy (MOITE)

Grant/Contract Number:: SC0012541

OSTI ID:: 1870317

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 18 Vol. 33; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (59)

Room‐Temperature Stimulated Emission and Lasing in Recrystallized Cesium Lead Bromide Perovskite Thin Films Pourdavoud, Neda; Haeger, Tobias; Mayer, Andre Advanced Materials, Vol. 31, Issue 39 https://doi.org/10.1002/adma.201903717	journal	August 2019
Room-Temperature Red-Green-Blue Whispering-Gallery Mode Lasing and White-Light Emission from Cesium Lead Halide Perovskite (CsPbX ₃ , X = Cl, Br, I) Microstructures Guo, Pengfei; Hossain, Mohammad Kamal; Shen, Xia Advanced Optical Materials, Vol. 6, Issue 3 https://doi.org/10.1002/adom.201700993	journal	December 2017
Role of Localized States in Photoluminescence Dynamics of High Optical Gain CsPbBr ₃ Nanocrystals Dey, Amrita; Rathod, Pravin; Kabra, Dinesh Advanced Optical Materials, Vol. 6, Issue 11 https://doi.org/10.1002/adom.201800109	journal	March 2018
Vertical Cavity Biexciton Lasing in 2D Dodecylammonium Lead Iodide Perovskites Booker, Edward P.; Price, Michael B.; Budden, Peter J. Advanced Optical Materials, Vol. 6, Issue 21 https://doi.org/10.1002/adom.201800616	journal	August 2018
Stable Whispering Gallery Mode Lasing from Solution‐Processed Formamidinium Lead Bromide Perovskite Microdisks Li, Xiaojun; Wang, Kaiyang; Chen, Mingming Advanced Optical Materials, Vol. 8, Issue 15 https://doi.org/10.1002/adom.202000030	journal	May 2020
Amplified Spontaneous Emission and Random Lasing in MAPbBr ₃ Halide Perovskite Single Crystals Murzin, Aleksei O.; Stroganov, Boris V.; Günnemann, Carsten Advanced Optical Materials, Vol. 8, Issue 17 https://doi.org/10.1002/adom.202000690	journal	June 2020
Unexpectedly Strong Auger Recombination in Halide Perovskites Shen, Jimmy-Xuan; Zhang, Xie; Das, Suvadip Advanced Energy Materials, Vol. 8, Issue 30 https://doi.org/10.1002/aenm.201801027	journal	September 2018
White CsPbBr ₃ : Characterizing the One‐Dimensional Cesium Lead Bromide Polymorph Aebli, Marcel; Benin, Bogdan M.; McCall, Kyle M. Helvetica Chimica Acta, Vol. 103, Issue 7 https://doi.org/10.1002/hlca.202000080	journal	June 2020
Electron–hole liquid formation by exciton and biexciton resonant excitation in CuCl Nagai, Masaya; Kuwata-Gonokami, Makoto Journal of Luminescence, Vol. 100, Issue 1-4 https://doi.org/10.1016/S0022-2313(02)00442-8	journal	December 2002
Red-Shifted Photoluminescence from Crystal Edges Due to Carrier Redistribution and Reabsorption in Lead Triiodide Perovskites Hong, Daocheng; Li, Jun; Wan, Sushu The Journal of Physical Chemistry C, Vol. 123, Issue 19 https://doi.org/10.1021/acs.jpcc.9b03647	journal	April 2019
Light–Matter Interactions in Cesium Lead Halide Perovskite Nanowire Lasers Park, Kidong; Lee, Jong Woon; Kim, Jun Dong The Journal of Physical Chemistry Letters, Vol. 7, Issue 18 https://doi.org/10.1021/acs.jpclett.6b01821	journal	September 2016
Photoresponse of CsPbBr ₃ and Cs ₄ PbBr ₆ Perovskite Single Crystals Cha, Ji-Hyun; Han, Jae Hoon; Yin, Wenping The Journal of Physical Chemistry Letters, Vol. 8, Issue 3 https://doi.org/10.1021/acs.jpclett.6b02763	journal	January 2017
Two-Photon Absorption and Two-Photon-Induced Gain in Perovskite Quantum Dots Nagamine, Gabriel; Rocha, Jaqueline O.; Bonato, Luiz G. The Journal of Physical Chemistry Letters, Vol. 9, Issue 12 https://doi.org/10.1021/acs.jpclett.8b01127	journal	June 2018
Optical Gain from Biexcitons in CsPbBr ₃ Nanocrystals Revealed by Two-dimensional Electronic Spectroscopy Zhao, Wei; Qin, Zhengyuan; Zhang, Chunfeng The Journal of Physical Chemistry Letters, Vol. 10, Issue 6 https://doi.org/10.1021/acs.jpclett.9b00524	journal	February 2019
Stable Two-Photon Pumped Amplified Spontaneous Emission from Millimeter-Sized CsPbBr ₃ Single Crystals Zhao, Chunyi; Tian, Wenming; Liu, Junxue The Journal of Physical Chemistry Letters, Vol. 10, Issue 10 https://doi.org/10.1021/acs.jpclett.9b00734	journal	April 2019
Single-Exciton Amplified Spontaneous Emission in Thin Films of CsPbX ₃ (X = Br, I) Perovskite Nanocrystals Navarro-Arenas, Juan; Suárez, Isaac; Chirvony, Vladimir S. The Journal of Physical Chemistry Letters, Vol. 10, Issue 20 https://doi.org/10.1021/acs.jpclett.9b02369	journal	September 2019
Role of the Exciton–Polariton in a Continuous-Wave Optically Pumped CsPbBr ₃ Perovskite Laser Shang, Qiuyu; Li, Meili; Zhao, Liyun Nano Letters, Vol. 20, Issue 9 https://doi.org/10.1021/acs.nanolett.0c02462	journal	August 2020
Nonlinear Absorption and Low-Threshold Multiphoton Pumped Stimulated Emission from All-Inorganic Perovskite Nanocrystals Wang, Yue; Li, Xiaoming; Zhao, Xin Nano Letters, Vol. 16, Issue 1 https://doi.org/10.1021/acs.nanolett.5b04110	journal	December 2015
Room-Temperature Polariton Lasing in All-Inorganic Perovskite Nanoplatelets Su, Rui; Diederichs, Carole; Wang, Jun Nano Letters, Vol. 17, Issue 6 https://doi.org/10.1021/acs.nanolett.7b01956	journal	May 2017
Benzyl Alcohol-Treated CH ₃ NH ₃ PbBr ₃ Nanocrystals Exhibiting High Luminescence, Stability, and Ultralow Amplified Spontaneous Emission Thresholds Veldhuis, Sjoerd A.; Tay, Yong Kang Eugene; Bruno, Annalisa Nano Letters, Vol. 17, Issue 12 https://doi.org/10.1021/acs.nanolett.7b03272	journal	November 2017
Stable, Ultralow Threshold Amplified Spontaneous Emission from CsPbBr ₃ Nanoparticles Exhibiting Trion Gain Wang, Yi; Zhi, Min; Chang, Yu-Qiang Nano Letters, Vol. 18, Issue 8 https://doi.org/10.1021/acs.nanolett.8b01817	journal	July 2018
Simple Approach to Improving the Amplified Spontaneous Emission Properties of Perovskite Films Li, Jing; Si, Junjie; Gan, Lu ACS Applied Materials & Interfaces, Vol. 8, Issue 48 https://doi.org/10.1021/acsami.6b13289	journal	November 2016
A Photonic Crystal Laser from Solution Based Organo-Lead Iodide Perovskite Thin Films Chen, Songtao; Roh, Kwangdong; Lee, Joonhee ACS Nano, Vol. 10, Issue 4 https://doi.org/10.1021/acsnano.5b08153	journal	March 2016
Broad Wavelength Tunable Robust Lasing from Single-Crystal Nanowires of Cesium Lead Halide Perovskites (CsPbX ₃ , X = Cl, Br, I) Fu, Yongping; Zhu, Haiming; Stoumpos, Constantinos C. ACS Nano, Vol. 10, Issue 8 https://doi.org/10.1021/acsnano.6b03916	journal	July 2016
Organic–Inorganic Hybrid Perovskite Nanowire Laser Arrays Liu, Peng; He, Xianxiong; Ren, Jiahuan ACS Nano, Vol. 11, Issue 6 https://doi.org/10.1021/acsnano.7b01351	journal	May 2017
CsPbBr ₃ Perovskite Quantum Dot Vertical Cavity Lasers with Low Threshold and High Stability Huang, Chun-Ying; Zou, Chen; Mao, Chenyi ACS Photonics, Vol. 4, Issue 9 https://doi.org/10.1021/acsphotonics.7b00520	journal	August 2017
Efficient Optical Amplification in the Nanosecond Regime from Formamidinium Lead Iodide Nanocrystals Papagiorgis, Paris; Manoli, Andreas; Protesescu, Loredana ACS Photonics, Vol. 5, Issue 3 https://doi.org/10.1021/acsphotonics.7b01159	journal	December 2017
Crystal Growth of the Perovskite Semiconductor CsPbBr ₃ : A New Material for High-Energy Radiation Detection Stoumpos, Constantinos C.; Malliakas, Christos D.; Peters, John A. Crystal Growth & Design, Vol. 13, Issue 7 https://doi.org/10.1021/cg400645t	journal	June 2013
Static Rashba Effect by Surface Reconstruction and Photon Recycling in the Dynamic Indirect Gap of APbBr ₃ (A = Cs, CH ₃ NH ₃ ) Single Crystals Ryu, Hongsun; Park, Dae Young; McCall, Kyle M. Journal of the American Chemical Society, Vol. 142, Issue 50 https://doi.org/10.1021/jacs.0c09132	journal	November 2020
Role of the A-Site Cation in Low-Temperature Optical Behaviors of APbBr ₃ (A = Cs, CH ₃ NH ₃ ) Ryu, Hongsun; Byun, Hye Ryung; McCall, Kyle M. Journal of the American Chemical Society, Vol. 143, Issue 5 https://doi.org/10.1021/jacs.0c11980	journal	January 2021
High Photoluminescence Efficiency and Optically Pumped Lasing in Solution-Processed Mixed Halide Perovskite Semiconductors Deschler, Felix; Price, Michael; Pathak, Sandeep The Journal of Physical Chemistry Letters, Vol. 5, Issue 8 https://doi.org/10.1021/jz5005285	journal	March 2014
Room-Temperature Near-Infrared High-Q Perovskite Whispering-Gallery Planar Nanolasers Zhang, Qing; Ha, Son Tung; Liu, Xinfeng Nano Letters, Vol. 14, Issue 10 https://doi.org/10.1021/nl503057g	journal	September 2014
Nanocrystals of Cesium Lead Halide Perovskites (CsPbX ₃ , X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut Protesescu, Loredana; Yakunin, Sergii; Bodnarchuk, Maryna I. Nano Letters, Vol. 15, Issue 6 https://doi.org/10.1021/nl5048779	journal	February 2015
Sequential deposition as a route to high-performance perovskite-sensitized solar cells Burschka, Julian; Pellet, Norman; Moon, Soo-Jin Nature, Vol. 499, Issue 7458, p. 316-319 https://doi.org/10.1038/nature12340	journal	July 2013
Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites Yakunin, Sergii; Protesescu, Loredana; Krieg, Franziska Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9056	journal	August 2015
Hot-carrier cooling and photoinduced refractive index changes in organic–inorganic lead halide perovskites Price, Michael B.; Butkus, Justinas; Jellicoe, Tom C. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9420	journal	September 2015
Bright light-emitting diodes based on organometal halide perovskite Tan, Zhi-Kuang; Moghaddam, Reza Saberi; Lai, May Ling Nature Nanotechnology, Vol. 9, Issue 9 https://doi.org/10.1038/nnano.2014.149	journal	August 2014
Perovskite light-emitting diodes based on solution-processed self-organized multiple quantum wells Wang, Nana; Cheng, Lu; Ge, Rui Nature Photonics, Vol. 10, Issue 11 https://doi.org/10.1038/nphoton.2016.185	journal	September 2016
Consolidation of the optoelectronic properties of CH3NH3PbBr3 perovskite single crystals Wenger, Bernard; Nayak, Pabitra K.; Wen, Xiaoming Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-017-00567-8	journal	September 2017
How lasing happens in CsPbBr3 perovskite nanowires Schlaus, Andrew P.; Spencer, Michael S.; Miyata, Kiyoshi Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-018-07972-7	journal	January 2019
Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites Wu, Bo; Yuan, Haifeng; Xu, Qiang Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-08326-7	journal	January 2019
Perovskite light-emitting diodes with external quantum efficiency exceeding 20 per cent Lin, Kebin; Xing, Jun; Quan, Li Na Nature, Vol. 562, Issue 7726 https://doi.org/10.1038/s41586-018-0575-3	journal	October 2018
Efficient, stable and scalable perovskite solar cells using poly(3-hexylthiophene) Jung, Eui Hyuk; Jeon, Nam Joong; Park, Eun Young Nature, Vol. 567, Issue 7749 https://doi.org/10.1038/s41586-019-1036-3	journal	March 2019
Green Perovskite Distributed Feedback Lasers Harwell, J. R.; Whitworth, G. L.; Turnbull, G. A. Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-11569-3	journal	September 2017
Whispering gallery mode lasing in lead halide perovskite crystals grown in microcapillary Kurahashi, Naho; Nguyen, Van-Cao; Sasaki, Fumio Applied Physics Letters, Vol. 113, Issue 1 https://doi.org/10.1063/1.5037243	journal	July 2018
Lasing in robust cesium lead halide perovskite nanowires Eaton, Samuel W.; Lai, Minliang; Gibson, Natalie A. Proceedings of the National Academy of Sciences, Vol. 113, Issue 8 https://doi.org/10.1073/pnas.1600789113	journal	February 2016
Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity Bao, Wei; Liu, Xiaoze; Xue, Fei Proceedings of the National Academy of Sciences, Vol. 116, Issue 41 https://doi.org/10.1073/pnas.1909948116	journal	September 2019
Mechanisms of Spontaneous and Amplified Spontaneous Emission in CH 3 NH 3 Pb I 3 Perovskite Thin Films Integrated in an Optical Waveguide Suárez, I.; Juárez-Pérez, E. J.; Chirvony, V. S. Physical Review Applied, Vol. 13, Issue 6 https://doi.org/10.1103/PhysRevApplied.13.064071	journal	June 2020
Auger recombination and biexcitons in Cu 2 O : A case for dark excitonic matter Jang, J. I.; Wolfe, J. P. Physical Review B, Vol. 74, Issue 4 https://doi.org/10.1103/PhysRevB.74.045211	journal	July 2006
Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH₃NH₃PbI₃ Xing, G.; Mathews, N.; Sun, S. Science, Vol. 342, Issue 6156, p. 344-347 https://doi.org/10.1126/science.1243167	journal	October 2013
Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber Stranks, S. D.; Eperon, G. E.; Grancini, G. Science, Vol. 342, Issue 6156, p. 341-344 https://doi.org/10.1126/science.1243982	journal	October 2013
Water photolysis at 12.3% efficiency via perovskite photovoltaics and Earth-abundant catalysts Luo, J.; Im, J. -H.; Mayer, M. T. Science, Vol. 345, Issue 6204 https://doi.org/10.1126/science.1258307	journal	September 2014
Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals Shi, D.; Adinolfi, V.; Comin, R. Science, Vol. 347, Issue 6221 https://doi.org/10.1126/science.aaa2725	journal	January 2015
Electron-hole diffusion lengths > 175 μm in solution-grown CH ₃ NH ₃ PbI ₃ single crystals Dong, Qingfeng; Fang, Yanjun; Shao, Yuchuan Science, Vol. 347, Issue 6225 https://doi.org/10.1126/science.aaa5760	journal	January 2015
High-performance photovoltaic perovskite layers fabricated through intramolecular exchange Yang, W. S.; Noh, J. H.; Jeon, N. J. Science, Vol. 348, Issue 6240 https://doi.org/10.1126/science.aaa9272	journal	May 2015
Quantum dot-induced phase stabilization of -CsPbI3 perovskite for high-efficiency photovoltaics Swarnkar, A.; Marshall, A. R.; Sanehira, E. M. Science, Vol. 354, Issue 6308 https://doi.org/10.1126/science.aag2700	journal	October 2016
Nanoimprinted distributed feedback lasers of solution processed hybrid perovskites Whitworth, Guy L.; Harwell, Jonathan R.; Miller, David N. Optics Express, Vol. 24, Issue 21 https://doi.org/10.1364/OE.24.023677	journal	January 2016
Exciton and bi-exciton mechanisms in amplified spontaneous emission from CsPbBr ₃ perovskite thin films Liu, Yang; Wang, Ju; Zhang, Lin Optics Express, Vol. 27, Issue 20 https://doi.org/10.1364/OE.27.029124	journal	January 2019
Theoretical Study of Auger Recombination of Excitons in Monolayer Transition-metal Dichalcogenides Lee, Hyun Cheol Journal of the Korean Physical Society, Vol. 73, Issue 11 https://doi.org/10.3938/jkps.73.1735	journal	December 2018

Similar Records

Near Room Temperature Solvothermal Growth of Ferroelectric CsPbBr₃ Nanoplatelets with Ultralow Dark Current

Journal Article · 2024 · Advanced Materials · OSTI ID:2429526

Anilkumar, Gokul M.; Bhakar, Monika; Taneja, Chetna; +4 more

Amplified spontaneous emission (ASE) in laser oscillators and amplifiers

Journal Article · 1983 · IEEE J. Quant. Electron.; (United States) · OSTI ID:5509257

Haag, G; Marowsky, G; Munz, M

Electrochemical Lithium Doping Induced Property Changes In Halide Perovskite CsPbBr₃ Crystal

Journal Article · 2017 · ACS Energy Letters · OSTI ID:1466317

Jiang, Qinglong; Zeng, Xiaoqiao; Wang, Ning; +3 more

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Perovskites
Photoluminescence
crystal structure
nanomaterials

Title: On the Origin of Room-Temperature Amplified Spontaneous Emission in CsPbBr3 Single Crystals

Citation Formats

References (59)

Similar Records

Related Subjects

Title: On the Origin of Room-Temperature Amplified Spontaneous Emission in CsPbBr₃ Single Crystals