Enhanced Luminescent Stability through Particle Interactions in Silicon Nanocrystal Aggregates

Miller, Joseph B.; Dandu, Naveen; Velizhanin, Kirill A.; Anthony, Rebecca J.; Kortshagen, Uwe R.; Kroll, Daniel M.; Kilina, Svetlana; Hobbie, Erik K.

doi:10.1021/acsnano.5b02676

Enhanced Luminescent Stability through Particle Interactions in Silicon Nanocrystal Aggregates

Journal Article · Tue Sep 08 00:00:00 EDT 2015 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5b02676· OSTI ID:1370941

Miller, Joseph B. ^[1]; Dandu, Naveen ^[1]; Velizhanin, Kirill A. ^[2]; Anthony, Rebecca J. ^[3]; Kortshagen, Uwe R. ^[3]; Kroll, Daniel M. ^[1]; Kilina, Svetlana ^[1]; Hobbie, Erik K. ^[1]

North Dakota State Univ., Fargo, ND (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of Minnesota, Minneapolis, MN (United States)

Close-packed assemblies of ligand-passivated colloidal nanocrystals can exhibit enhanced photoluminescent stability, but the origin of this effect is unclear. Here, we use experiment, simulation, and ab initio computation to examine the influence of interparticle interactions on the photoluminescent stability of silicon nanocrystal aggregates. The time-dependent photoluminescence emitted by structures ranging in size from a single quantum dot to agglomerates of more than a thousand is compared with Monte Carlo simulations of noninteracting ensembles using measured single-particle blinking data as input. In contrast to the behavior typically exhibited by the metal chalcogenides, the measured photoluminescent stability shows an enhancement with respect to the noninteracting scenario with increasing aggregate size. We model this behavior using time-dependent density functional theory calculations of energy transfer between neighboring nanocrystals as a function of nanocrystal size, separation, and the presence of charge and/or surface-passivation defects. In conclusion, our results suggest that rapid exciton transfer from “bright” nanocrystals to surface trap states in nearest-neighbors can efficiently fill such traps and enhance the stability of emission by promoting the radiative recombination of slowly diffusing excited electrons.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC04-94AL85000; AC52-06NA25396; FG36-08GO88160

OSTI ID:: 1370941

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 10 Vol. 9; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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