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Caixia Huo

Publications and source records attributed to Caixia Huo.

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Impact of bright-dark exciton thermal population mixing on the brightness of CsPbBr$_3$ nanocrystals

Understanding the interplay between bright and dark exciton states is crucial for deciphering the luminescence properties of low-dimensional materials. The origin of the outstanding brightness of lead halide perovskites remains elusive. Here, we analyse temperature-dependent time-resolved photoluminescence to investigate the population mixing between bright and dark exciton sublevels in individual CsPbBr$_3$ nanocrystals in the intermediate confinement regime. We extract bright and dark exciton decay rates, and show quantitatively that the decay dynamics can only be reproduced with second-order phonon transitions. Furthermore, we find that any exciton sublevel ordering is compatible with the most likely population transfer mechanism. The remarkable brightness of lead halide perovskite nanocrystals rather stems from a reduced asymmetry between bright-to-dark and dark-to-bright conversion originating from the peculiar second-order phonon-assisted transitions that freeze bright-dark conversion at low temperature together with the very fast radiative recombination and favourable degeneracy of the bright exciton state.

cond-mat.mes-hall

Spectral fingerprint of quantum confinement in single CsPbBr$_3$ nanocrystals

Lead halide perovskite nanocrystals are promising materials for classical and quantum light emission. To understand these outstanding properties, a thorough analysis of the band-edge exciton emission is needed which is not reachable in ensemble and room temperature studies because of broadening effects. Here, we report on a cryogenic-temperature study of the photoluminescence of single CsPbBr$_3$ NCs in the intermediate quantum confinement regime. We reveal the size-dependence of the spectral features observed: the bright-triplet exciton energy splittings, the trion and biexciton binding energies as well as the optical phonon replica spectrum. In addition, we show that bright triplet energy splittings are consistent with a pure exchange model and that the variety of polarisation properties and spectra recorded can be rationalised simply by considering the orientation of the emitting dipoles and the populations of the emitting states.

cond-mat.mes-hall