Enhanced Luminescent Stability through Particle Interactions in Silicon Nanocrystal Aggregates

ACS Nano
Joseph B MillerErik K Hobbie

Abstract

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. 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 o...Continue Reading

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Citations

Dec 17, 2015·The Journal of Chemical Physics·Kenley M PelzerRichard D Schaller
Mar 5, 2016·The Journal of Physical Chemistry Letters·Dmitry A KislitsynGeorge V Nazin
Oct 19, 2016·Accounts of Chemical Research·Svetlana V KilinaDmitri S Kilin
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Jan 3, 2019·Chemistry : a European Journal·Matthias JakobUlrich Heiz
Jun 6, 2017·Nanoscale·A ShavelR A Alvarez-Puebla
Jun 13, 2017·Small·Lucía Labrador-PáezDaniel Jaque
Jul 14, 2018·The Journal of Physical Chemistry Letters·Yulun HanDmitri S Kilin
Aug 31, 2017·ACS Applied Materials & Interfaces·Aleksandrs MarininsIlya Sychugov
Aug 12, 2017·The Journal of Physical Chemistry Letters·A A ChistyakovO V Prezhdo

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