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Origin of the Size-Dependent Stokes Shift in CsPbBr3 Perovskite Nanocrystals

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    Origin of the Size-Dependent Stokes Shift in CsPbBr3 Perovskite Nanocrystals
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    † Department of Chemistry and Biochemistry, University of Notre Dame, 251 Nieuwland Science Hall, Notre Dame, Indiana 46556, United States
    ‡ Notre Dame Integrated Imaging Facility, University of Notre Dame, Notre Dame, Indiana 46556, United States
    *[email protected]
    *[email protected]
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    Cite this: J. Am. Chem. Soc. 2017, 139, 35, 12201–12208
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    https://doi.org/10.1021/jacs.7b05683
    Published August 3, 2017
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    Abstract

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    The origin of the size-dependent Stokes shift in CsPbBr3 nanocrystals (NCs) is explained for the first time. Stokes shifts range from 82 to 20 meV for NCs with effective edge lengths varying from ∼4 to 13 nm. We show that the Stokes shift is intrinsic to the NC electronic structure and does not arise from extrinsic effects such as residual ensemble size distributions, impurities, or solvent-related effects. The origin of the Stokes shift is elucidated via first-principles calculations. Corresponding theoretical modeling of the CsPbBr3 NC density of states and band structure reveals the existence of an intrinsic confined hole state 260 to 70 meV above the valence band edge state for NCs with edge lengths from ∼2 to 5 nm. A size-dependent Stokes shift is therefore predicted and is in quantitative agreement with the experimental data. Comparison between bulk and NC calculations shows that the confined hole state is exclusive to NCs. At a broader level, the distinction between absorbing and emitting states in CsPbBr3 is likely a general feature of other halide perovskite NCs and can be tuned via NC size to enhance applications involving these materials.

    Copyright © 2017 American Chemical Society

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.7b05683.

    • NC sizing histogram, absorption- and emission-derived NC sizing curves, NC PXRD data, excitation intensity-dependent emission data and discussion, table of PL quantum yields, table of relevant experimental absorption and emission data, linear absorption fits, TCSPC-TRES data, solvatochromism data, band-edge excitation emission and absorption spectra, convolution analysis of other ensemble NC sizes, discussion of bulk electronic structure calculations, discussion of geometries and band structure calculations, table of calculated bulk band gaps/lattice parameters, MOs for VBES/CHS of different NC sizes, MOs for CHS of NC models with various crystal phases, projected DOS for l = 2.64 nm NC model, discussion of SOC calculations, absorption strength calculations discussion, table of NC model data, discussion of exciton binding energies (PDF)

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