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Title: Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals

Abstract

Intrinsic constraints on efficient photoluminescence (PL) from smaller alkene-capped silicon nanocrystals (SiNCs) put limits on potential applications, but the root cause of such effects remains elusive. Here, plasma-synthesized colloidal SiNCs separated into monodisperse fractions reveal an abrupt size-dependent partitioning of multilevel PL relaxation, which we study as a function of temperature. Guided by theory and simulation, we explore the potential role of resonant phonon interactions with “minigaps” that emerge in the electronic density of states (DOS) under strong quantum confinement. Such higher-order structures can be very sensitive to SiNC surface chemistry, which we suggest might explain the common implication of surface effects in both the emergence of multimodal PL relaxation and the loss of quantum yield with decreasing nanocrystal size. Our results have potentially profound implications for optimizing the radiative recombination kinetics and quantum yield of smaller ligand-passivated SiNCs.

Authors:
 [1];  [1]; ORCiD logo [2];  [2];  [1]; ORCiD logo [1]
  1. North Dakota State University, Fargo, North Dakota 58108, United States
  2. University of Minnesota, Minneapolis, Minnesota 55455, United States
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1487446
DOE Contract Number:  
FG36-08GO88160; AC02-05CH11231
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Nano; Journal Volume: 11; Journal Issue: 2
Country of Publication:
United States
Language:
English

Citation Formats

Brown, Samuel L., Miller, Joseph B., Anthony, Rebecca J., Kortshagen, Uwe R., Kryjevski, Andrei, and Hobbie, Erik K. Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals. United States: N. p., 2017. Web. doi:10.1021/acsnano.6b07285.
Brown, Samuel L., Miller, Joseph B., Anthony, Rebecca J., Kortshagen, Uwe R., Kryjevski, Andrei, & Hobbie, Erik K. Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals. United States. doi:10.1021/acsnano.6b07285.
Brown, Samuel L., Miller, Joseph B., Anthony, Rebecca J., Kortshagen, Uwe R., Kryjevski, Andrei, and Hobbie, Erik K. Wed . "Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals". United States. doi:10.1021/acsnano.6b07285.
@article{osti_1487446,
title = {Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals},
author = {Brown, Samuel L. and Miller, Joseph B. and Anthony, Rebecca J. and Kortshagen, Uwe R. and Kryjevski, Andrei and Hobbie, Erik K.},
abstractNote = {Intrinsic constraints on efficient photoluminescence (PL) from smaller alkene-capped silicon nanocrystals (SiNCs) put limits on potential applications, but the root cause of such effects remains elusive. Here, plasma-synthesized colloidal SiNCs separated into monodisperse fractions reveal an abrupt size-dependent partitioning of multilevel PL relaxation, which we study as a function of temperature. Guided by theory and simulation, we explore the potential role of resonant phonon interactions with “minigaps” that emerge in the electronic density of states (DOS) under strong quantum confinement. Such higher-order structures can be very sensitive to SiNC surface chemistry, which we suggest might explain the common implication of surface effects in both the emergence of multimodal PL relaxation and the loss of quantum yield with decreasing nanocrystal size. Our results have potentially profound implications for optimizing the radiative recombination kinetics and quantum yield of smaller ligand-passivated SiNCs.},
doi = {10.1021/acsnano.6b07285},
journal = {ACS Nano},
number = 2,
volume = 11,
place = {United States},
year = {Wed Feb 01 00:00:00 EST 2017},
month = {Wed Feb 01 00:00:00 EST 2017}
}