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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, mechanic-al 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. Finally, 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.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [2]
  1. Univ. of Tennessee, Knoxville, TN (United States); Beijing Jiaotong Univ. (China)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE; US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1607028
Alternate Identifier(s):
OSTI ID: 1571545
Grant/Contract Number:  
AC05-00OR22725; FA 9550-15-1-0064; FA2386-15-1-410; NSF-1911659; 61475051; 61634001
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 49; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; gap states; quasi-2D perovskites; spatially extended states; two-photon absorption; up-conversion photoluminescence

Citation Formats

Zhu, Xixiang, Xu, Hengxing, Liu, Yongtao, Zhang, Jia, Wang, Miaosheng, Ivanov, Ilia N., Ovchinnikova, Olga S., and Hu, Bin. Two-Photon Up-Conversion Photoluminescence Realized through Spatially Extended Gap States in Quasi-2D Perovskite Films. United States: N. p., 2019. Web. doi:10.1002/adma.201901240.
Zhu, Xixiang, Xu, Hengxing, Liu, Yongtao, Zhang, Jia, Wang, Miaosheng, Ivanov, Ilia N., Ovchinnikova, Olga S., & Hu, Bin. Two-Photon Up-Conversion Photoluminescence Realized through Spatially Extended Gap States in Quasi-2D Perovskite Films. United States. https://doi.org/10.1002/adma.201901240
Zhu, Xixiang, Xu, Hengxing, Liu, Yongtao, Zhang, Jia, Wang, Miaosheng, Ivanov, Ilia N., Ovchinnikova, Olga S., and Hu, Bin. Wed . "Two-Photon Up-Conversion Photoluminescence Realized through Spatially Extended Gap States in Quasi-2D Perovskite Films". United States. https://doi.org/10.1002/adma.201901240. https://www.osti.gov/servlets/purl/1607028.
@article{osti_1607028,
title = {Two-Photon Up-Conversion Photoluminescence Realized through Spatially Extended Gap States in Quasi-2D Perovskite Films},
author = {Zhu, Xixiang and Xu, Hengxing and Liu, Yongtao and Zhang, Jia and Wang, Miaosheng and Ivanov, Ilia N. and Ovchinnikova, Olga S. and Hu, Bin},
abstractNote = {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, mechanic-al 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. Finally, 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.},
doi = {10.1002/adma.201901240},
journal = {Advanced Materials},
number = 49,
volume = 31,
place = {United States},
year = {2019},
month = {10}
}

Journal Article:
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Cited by: 19 works
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Figures / Tables:

Figure 1 Figure 1: Absorption and down-conversion PL characteristics for 2D perovskite (PEA)2(MA)4Pb5Br16 films. (a) Absorption and PL spectra. (b) Up-conversion PL spectrum under CW 980 nm laser excitation (2500 mW/cm2). (c) Emission-excitation intensity dependence under up-conversion condition.

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