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Title: Enhanced Size Selection in Two-Photon Excitation for CsPbBr 3 Perovskite Nanocrystals

Abstract

Here, cesium lead bromide (CsPbBr 3) perovskite nanocrystals (NCs), with large two-photon absorption (TPA) cross-section and bright photoluminescence (PL), have been demonstrated as stable two-photon-pumped lasing medium. With two-photon excitation, red-shifted PL spectrum and increased PL lifetime is observed compared with one-photon excitation. We have investigated the origin of such difference using time-resolved laser spectroscopies. We ascribe the difference to the enhanced size selection of NCs by two-photon excitation. Because of inherent nonlinearity, the size dependence of absorption cross-section under TPA is stronger. Consequently, larger size NCs are preferably excited, leading to longer excited-state lifetime and red-shifted PL emission. In a broad view, the enhanced size selection in two-photon excitation of CsPbBr 3 NCs is likely a general feature of the perovskite NCs and can be tuned via NC size distribution to influence their performance within NC-based nonlinear optical materials and devices.

Authors:
ORCiD logo [1];  [2];  [2];  [2]; ORCiD logo [3];  [4];  [5];  [2]
  1. Lund Univ., Lund (Sweden); Chinese Academy of Sciences, Dalian (China)
  2. Lund Univ., Lund (Sweden)
  3. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
  4. ELI-HU Non-Profit, Ltd., Szeged (Hungary); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  5. Lund Univ., Lund (Sweden); Qatar Univ., Doha (Qatar)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Swedish Research Council (SRC); Knut and Alice Wallenberg Foundation; European Regional Development Fund (ERDF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1459646
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal Issue: 20; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Chen, Junsheng, Chabera, Pavel, Pascher, Torbjorn, Messing, Maria E., Schaller, Richard, Canton, Sophie, Zheng, Kaibo, and Pullerits, Tonu. Enhanced Size Selection in Two-Photon Excitation for CsPbBr3 Perovskite Nanocrystals. United States: N. p., 2017. Web. doi:10.1021/acs.jpclett.7b02178.
Chen, Junsheng, Chabera, Pavel, Pascher, Torbjorn, Messing, Maria E., Schaller, Richard, Canton, Sophie, Zheng, Kaibo, & Pullerits, Tonu. Enhanced Size Selection in Two-Photon Excitation for CsPbBr3 Perovskite Nanocrystals. United States. doi:10.1021/acs.jpclett.7b02178.
Chen, Junsheng, Chabera, Pavel, Pascher, Torbjorn, Messing, Maria E., Schaller, Richard, Canton, Sophie, Zheng, Kaibo, and Pullerits, Tonu. Wed . "Enhanced Size Selection in Two-Photon Excitation for CsPbBr3 Perovskite Nanocrystals". United States. doi:10.1021/acs.jpclett.7b02178. https://www.osti.gov/servlets/purl/1459646.
@article{osti_1459646,
title = {Enhanced Size Selection in Two-Photon Excitation for CsPbBr3 Perovskite Nanocrystals},
author = {Chen, Junsheng and Chabera, Pavel and Pascher, Torbjorn and Messing, Maria E. and Schaller, Richard and Canton, Sophie and Zheng, Kaibo and Pullerits, Tonu},
abstractNote = {Here, cesium lead bromide (CsPbBr3) perovskite nanocrystals (NCs), with large two-photon absorption (TPA) cross-section and bright photoluminescence (PL), have been demonstrated as stable two-photon-pumped lasing medium. With two-photon excitation, red-shifted PL spectrum and increased PL lifetime is observed compared with one-photon excitation. We have investigated the origin of such difference using time-resolved laser spectroscopies. We ascribe the difference to the enhanced size selection of NCs by two-photon excitation. Because of inherent nonlinearity, the size dependence of absorption cross-section under TPA is stronger. Consequently, larger size NCs are preferably excited, leading to longer excited-state lifetime and red-shifted PL emission. In a broad view, the enhanced size selection in two-photon excitation of CsPbBr3 NCs is likely a general feature of the perovskite NCs and can be tuned via NC size distribution to influence their performance within NC-based nonlinear optical materials and devices.},
doi = {10.1021/acs.jpclett.7b02178},
journal = {Journal of Physical Chemistry Letters},
issn = {1948-7185},
number = 20,
volume = 8,
place = {United States},
year = {2017},
month = {10}
}

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Works referencing / citing this record:

Two-Photon-Absorption Properties of Pyrene-Based Dipolar D-π-A Fluorophores
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Two-Photon-Absorption Properties of Pyrene-Based Dipolar D-π-A Fluorophores
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