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Excited State Dynamics of a CsPbBr3 Nanocrystal Terminated with Binary Ligands: Sparse Density of States with Giant Spin-Orbit Coupling Suppresses Carrier Cooling

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dc.contributor.author Forde, Aaron
dc.contributor.author Inerbaev, Talgat
dc.contributor.author Hobbie, Erik
dc.contributor.author Kilin, Dmitri
dc.date.accessioned 2024-09-12T04:38:48Z
dc.date.available 2024-09-12T04:38:48Z
dc.date.issued 2019-03
dc.identifier.issn 00027863
dc.identifier.other DOI 10.1021/jacs.8b13385
dc.identifier.uri http://rep.enu.kz/handle/enu/16223
dc.description.abstract Fully inorganic lead halide perovskite nanocrystals (NCs) are of interest for photovoltaic and light-emitting devices due to optoelectronic properties that can be tuned/optimized via halide composition, surface passivation, doping, and confinement. Compared to bulk materials, certain excited-state properties in NCs can be adjusted by electronic confinement effects such as suppressed hot carrier cooling and enhanced radiative recombination. Here we use spinor Kohn-Sham orbitals (SKSOs) with spin-orbit coupling (SOC) interaction as a basis to compute excited-state dissipative dynamics simulations on a fully passivated CsPbBr3 NC atomistic model. Redfield theory in the density matrix formalism is used to describe electron-phonon interactions which drive hot carrier cooling and nonradiative recombination (knonrad). Radiative recombination (krad) is calculated through oscillator strengths using SKSO basis. From krad and krad + knonrad, we compute a theoretical photoluminescence quantum yield (PLQY) of 53%. Computed rates of hot carrier cooling (kcooling ≈ 10-1 1/ps) compare favorably with what has been reported in the literature. Interestingly, we observe that hot electron cooling slows down near the band edge, which we attribute to large SOC in the conduction band combined with strong confinement, which creates subgaps above the band edge. This slow carrier cooling could potentially impact hot carrier extraction before complete thermalization in photovoltaics (PVs). Implications of this work suggest that strong/intermediate confined APbX3 NCs are better suited to applications in PVs due to slower carrier cooling near the conduction band edge, while intermediate/weak confined NCs are more appropriate for light-emitting applications, such as LEDs. © Copyright 2019 American Chemical Society. ru
dc.language.iso en ru
dc.publisher Journal of the American Chemical Society ru
dc.relation.ispartofseries Том 141,;Выпуск 10, Страницы 4388 - 4397
dc.title Excited State Dynamics of a CsPbBr3 Nanocrystal Terminated with Binary Ligands: Sparse Density of States with Giant Spin-Orbit Coupling Suppresses Carrier Cooling ru
dc.type Article ru


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