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Enhanced Size Selection in Two-Photon Excitation for CsPbBr3 Perovskite Nanocrystals
Author(s) -
Junsheng Chen,
Pavel Chábera,
Torbjörn Pascher,
Maria E. Messing,
Richard D. Schaller,
Sophie E. Canton,
Kaibo Zheng,
Tönu Pullerits
Publication year - 2017
Publication title -
the journal of physical chemistry letters
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.563
H-Index - 203
ISSN - 1948-7185
DOI - 10.1021/acs.jpclett.7b02178
Subject(s) - photoluminescence , excitation , excited state , materials science , lasing threshold , absorption (acoustics) , perovskite (structure) , absorption cross section , laser , nanocrystal , photon , atomic physics , molecular physics , optoelectronics , chemistry , optics , cross section (physics) , physics , nanotechnology , wavelength , crystallography , quantum mechanics , composite material
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.

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