4.8 Article

Octahedral Distortions Generate a Thermally Activated Phonon-Assisted Radiative Recombination Pathway in Cubic CsPbBr3 Perovskite Quantum Dots

Journal

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 14, Issue 39, Pages 8717-8725

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.3c02568

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Exciton-phonon interactions are found to cause broadening of photoluminescence line width and slower electron-hole recombination in cubic CsPbBr3 perovskite quantum dots (PQDs) due to structural distortions at room temperature. At low temperature, phonon-assisted recombination is reduced, resulting in minimized line width broadening.
Exciton-phonon interactions elucidate structure-function relationships that aid in the control of color purity and carrier diffusion, which is necessary for the performance-driven design of solid-state optical emitters. Temperature-dependent steady-state photoluminescence (PL) and time-resolved PL (TRPL) reveal that thermally activated exciton-phonon interactions originate from structural distortions related to vibrations in cubic CsPbBr3 perovskite quantum dots (PQDs) at room temperature. Exciton-phonon interactions cause performance-degrading PL line width broadening and slower electron-hole recombination. Structural distortions in cubic PQDs at room temperature exist as the bending and stretching of the PbBr6 octahedra subunit. The PbBr6 octahedral distortions cause symmetry breaking, resulting in thermally activated longitudinal optical (LO) phonon coupling to the photoexcited electron-hole pair that manifests as inhomogeneous PL line width broadening. At cryogenic temperatures, the line width broadening is minimized due to a decrease in phonon-assisted recombination through shallow traps. A fundamental understanding of these intrinsic exciton-phonon interactions gives insight into the polymorphic nature of the cubic phase and the origins of performance degradation in PQD optical emitters.

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