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Title: Exciton size and quantum transport in nanoplatelets

Abstract

Two-dimensional nanoplatelets (NPLs) are an exciting class of materials with promising optical and energy transport properties. The possibility of efficient energy transport between nanoplatelets raises questions regarding the nature of energy transfer in these thin, laterally extended systems. A challenge in understanding exciton transport is the uncertainty regarding the size of the exciton. Depending on the material and defects in the nanoplatelet, an exciton could plausibly extend over an entire plate or localize to a small region. The variation in possible exciton sizes raises the question how exciton size impacts the efficiency of transport between nanoplatelet structures. Here, in this paper, we explore this issue using a quantum master equation approach. This method goes beyond the assumptions of Förster theory to allow for quantum mechanical effects that could increase energy transfer efficiency. The model is extremely flexible in describing different systems, allowing us to test the effect of varying the spatial extent of the exciton. We first discuss qualitative aspects of the relationship between exciton size and transport and then conduct simulations of exciton transport between NPLs for a range of exciton sizes and environmental conditions. Our results reveal that exciton size has a strong effect on energy transfer efficiencymore » and suggest that manipulation of exciton size may be useful in designing NPLs for energy transport.« less

Authors:
 [1];  [2];  [1];  [3]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM); Univ. of Chicago, IL (United States). Inst. for Molecular Engineering
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM); Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1391760
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 143; Journal Issue: 22; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; heterostructures

Citation Formats

Pelzer, Kenley M., Darling, Seth B., Gray, Stephen K., and Schaller, Richard D. Exciton size and quantum transport in nanoplatelets. United States: N. p., 2015. Web. doi:10.1063/1.4936407.
Pelzer, Kenley M., Darling, Seth B., Gray, Stephen K., & Schaller, Richard D. Exciton size and quantum transport in nanoplatelets. United States. https://doi.org/10.1063/1.4936407
Pelzer, Kenley M., Darling, Seth B., Gray, Stephen K., and Schaller, Richard D. Wed . "Exciton size and quantum transport in nanoplatelets". United States. https://doi.org/10.1063/1.4936407. https://www.osti.gov/servlets/purl/1391760.
@article{osti_1391760,
title = {Exciton size and quantum transport in nanoplatelets},
author = {Pelzer, Kenley M. and Darling, Seth B. and Gray, Stephen K. and Schaller, Richard D.},
abstractNote = {Two-dimensional nanoplatelets (NPLs) are an exciting class of materials with promising optical and energy transport properties. The possibility of efficient energy transport between nanoplatelets raises questions regarding the nature of energy transfer in these thin, laterally extended systems. A challenge in understanding exciton transport is the uncertainty regarding the size of the exciton. Depending on the material and defects in the nanoplatelet, an exciton could plausibly extend over an entire plate or localize to a small region. The variation in possible exciton sizes raises the question how exciton size impacts the efficiency of transport between nanoplatelet structures. Here, in this paper, we explore this issue using a quantum master equation approach. This method goes beyond the assumptions of Förster theory to allow for quantum mechanical effects that could increase energy transfer efficiency. The model is extremely flexible in describing different systems, allowing us to test the effect of varying the spatial extent of the exciton. We first discuss qualitative aspects of the relationship between exciton size and transport and then conduct simulations of exciton transport between NPLs for a range of exciton sizes and environmental conditions. Our results reveal that exciton size has a strong effect on energy transfer efficiency and suggest that manipulation of exciton size may be useful in designing NPLs for energy transport.},
doi = {10.1063/1.4936407},
journal = {Journal of Chemical Physics},
number = 22,
volume = 143,
place = {United States},
year = {Wed Dec 09 00:00:00 EST 2015},
month = {Wed Dec 09 00:00:00 EST 2015}
}

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