On the Origin of Room-Temperature Amplified Spontaneous Emission in CsPbBr3Single Crystals

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

doi:10.1021/acs.chemmater.1c00591

On the Origin of Room-Temperature Amplified Spontaneous Emission in CsPbBr₃Single Crystals

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

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

Abstract

CsPbBr₃is 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 CsPbBr₃nanostructures, 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 CsPbBr₃single crystals exhibit highly efficient ASE with a threshold of 46 MWcm^-2at 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 CsPbBr₃single crystal can be utilized for lasing applications when engineered into a submillimeter thickness for effective light-matter interaction.

Original language	English (US)
Pages (from-to)	7185-7193
Number of pages	9
Journal	Chemistry of Materials
Volume	33
Issue number	18
DOIs	https://doi.org/10.1021/acs.chemmater.1c00591
State	Published - Sep 28 2021

Funding

This work was supported by the Basic Science Research Programs (2019R1A2C3006189, 2017R1D1A1B03035539, 2020R1F1A1069646, and 2021R1A2C2013625) and the Priority Research Centers Program (2019R1A6A1A11053838) through the National Research Foundation of Korea (NRF), funded by the Korean government. Y.S.K. also thanks Technology Innovation Program (20009803), funded by the Ministry of Trade, Industry & Energy (MOITE, Korea). At the Northwestern University, this work was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, under grant no. SC0012541 (synthesis and structural characterization).

ASJC Scopus subject areas

General Chemistry
General Chemical Engineering
Materials Chemistry

Access to Document

10.1021/acs.chemmater.1c00591

Cite this

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title = "On the Origin of Room-Temperature Amplified Spontaneous Emission in CsPbBr3Single Crystals",

abstract = "CsPbBr3is 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 CsPbBr3nanostructures, 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 CsPbBr3single crystals exhibit highly efficient ASE with a threshold of 46 MWcm-2at 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 CsPbBr3single crystal can be utilized for lasing applications when engineered into a submillimeter thickness for effective light-matter interaction.",

author = "Donggyu Kim and Hongsun Ryu and Lim, {Soo Yeon} and McCall, {Kyle M.} and Jongwoo Park and Sungdo Kim and Kim, {Tae Jung} and Jeongyong Kim and Kim, {Yong Soo} and Kanatzidis, {Mercouri G.} and Hyeonsik Cheong and Jang, {Joon I.}",

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doi = "10.1021/acs.chemmater.1c00591",

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T1 - On the Origin of Room-Temperature Amplified Spontaneous Emission in CsPbBr3Single Crystals

AU - Kim, Donggyu

AU - Ryu, Hongsun

AU - Lim, Soo Yeon

AU - McCall, Kyle M.

AU - Park, Jongwoo

AU - Kim, Sungdo

AU - Kim, Tae Jung

AU - Kim, Jeongyong

AU - Kim, Yong Soo

AU - Kanatzidis, Mercouri G.

AU - Cheong, Hyeonsik

AU - Jang, Joon I.

PY - 2021/9/28

Y1 - 2021/9/28

N2 - CsPbBr3is 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 CsPbBr3nanostructures, 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 CsPbBr3single crystals exhibit highly efficient ASE with a threshold of 46 MWcm-2at 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 CsPbBr3single crystal can be utilized for lasing applications when engineered into a submillimeter thickness for effective light-matter interaction.

AB - CsPbBr3is 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 CsPbBr3nanostructures, 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 CsPbBr3single crystals exhibit highly efficient ASE with a threshold of 46 MWcm-2at 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 CsPbBr3single crystal can be utilized for lasing applications when engineered into a submillimeter thickness for effective light-matter interaction.

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