Two-Photon Up-Conversion Photoluminescence Realized through Spatially Extended Gap States in Quasi-2D Perovskite Films

Xixiang Zhu; Hengxing Xu; Yongtao Liu; Jia Zhang; Miaosheng Wang; Ilia N. Ivanov; Olga S. Ovchinnikova; Bin Hu

doi:10.1002/adma.201901240

Two-Photon Up-Conversion Photoluminescence Realized through Spatially Extended Gap States in Quasi-2D Perovskite Films

Xixiang Zhu, Hengxing Xu, Yongtao Liu, Jia Zhang, Miaosheng Wang, Ilia N. Ivanov, Olga S. Ovchinnikova, Bin Hu

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

26 Scopus citations

Abstract

A new approach to generate a two-photon up-conversion photoluminescence (PL) by directly exciting the gap states with continuous-wave (CW) infrared photoexcitation in solution-processing quasi-2D perovskite films [(PEA)₂(MA)₄Pb₅Br₁₆ with n = 5] is reported. Specifically, a visible PL peaked at 520 nm is observed with the quadratic power dependence by exciting the gap states with CW 980 nm laser excitation, indicating a two-photon up-conversion PL occurring in quasi-2D perovskite films. Decreasing the gap states by reducing the n value leads to a dramatic decrease in the two-photon up-conversion PL signal. This confirms that the gap states are indeed responsible for generating the two-photon up-conversion PL in quasi-2D perovskites. Furthermore, mechanical scratching indicates that the different-n-value nanoplates are essentially uniformly formed in the quasi-2D perovskite films toward generating multi-photon up-conversion light emission. More importantly, the two-photon up-conversion PL is found to be sensitive to an external magnetic field, indicating that the gap states are essentially formed as spatially extended states ready for multi-photon excitation. Polarization-dependent up-conversion PL studies reveal that the gap states experience the orbit–orbit interaction through Coulomb polarization to form spatially extended states toward developing multi-photon up-conversion light emission in quasi-2D perovskites.

Original language	English
Article number	1901240
Journal	Advanced Materials
Volume	31
Issue number	49
DOIs	https://doi.org/10.1002/adma.201901240
State	Published - Dec 1 2019

Funding

This research was supported by Air Force Office of Scientific Research (AFOSR) (FA9550-15-1-0064, FA2386-15-1-410) and National Science Foundation (NSF-1911659). This research was partially conducted at the Center for Nanophase Materials Sciences based on user projects (CNMS2012-106, CNMS2012-107, CNMS-2012-108, CNMS-2019-057), which is sponsored by Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. Department of Energy. X.Z. acknowledges support from Beijing Jiaotong University.

Keywords

gap states
quasi-2D perovskites
spatially extended states
two-photon absorption
up-conversion photoluminescence

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10.1002/adma.201901240

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title = "Two-Photon Up-Conversion Photoluminescence Realized through Spatially Extended Gap States in Quasi-2D Perovskite Films",

abstract = "A new approach to generate a two-photon up-conversion photoluminescence (PL) by directly exciting the gap states with continuous-wave (CW) infrared photoexcitation in solution-processing quasi-2D perovskite films [(PEA)2(MA)4Pb5Br16 with n = 5] is reported. Specifically, a visible PL peaked at 520 nm is observed with the quadratic power dependence by exciting the gap states with CW 980 nm laser excitation, indicating a two-photon up-conversion PL occurring in quasi-2D perovskite films. Decreasing the gap states by reducing the n value leads to a dramatic decrease in the two-photon up-conversion PL signal. This confirms that the gap states are indeed responsible for generating the two-photon up-conversion PL in quasi-2D perovskites. Furthermore, mechanical scratching indicates that the different-n-value nanoplates are essentially uniformly formed in the quasi-2D perovskite films toward generating multi-photon up-conversion light emission. More importantly, the two-photon up-conversion PL is found to be sensitive to an external magnetic field, indicating that the gap states are essentially formed as spatially extended states ready for multi-photon excitation. Polarization-dependent up-conversion PL studies reveal that the gap states experience the orbit–orbit interaction through Coulomb polarization to form spatially extended states toward developing multi-photon up-conversion light emission in quasi-2D perovskites.",

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author = "Xixiang Zhu and Hengxing Xu and Yongtao Liu and Jia Zhang and Miaosheng Wang and Ivanov, {Ilia N.} and Ovchinnikova, {Olga S.} and Bin Hu",

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Two-Photon Up-Conversion Photoluminescence Realized through Spatially Extended Gap States in Quasi-2D Perovskite Films

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