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Title: Emergent Electronic and Dielectric Properties of Interacting Nanoparticles at Finite Temperature

Abstract

Lead chalcogenide nanoparticle solids have been successfully integrated into certified solar cells and represent promising platforms for the design of novel photoabsorbers for photoelectrochemical cells. While much attention has been drawn to improving efficiency and device performance through altering the character of the individual nanoparticles, the role of interactions between nanoparticles is not yet well-understood. Using first-principles molecular dynamics and electronic structure calculations, we investigated the combined effect of temperature and interaction on functionalized lead chalcogenide nanoparticles (NPs). Here, we show that at finite temperature, interacting NPs are dynamical dipolar systems, with the average values of dipole moments and polarizabilities substantially increased with respect to those of the isolated building blocks. In addition, we show that the interacting NPs exhibit slightly smaller fundamental gaps that decrease as a function of temperature and that the radiative lifetimes of both the isolated NPs and the solids are greatly reduced at finite temperature compared to T = 0. Lastly, we present a critical discussion of various results reported in the literature for the values of dipole moments of nanoparticles.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [3]
  1. The Univ. of Chicago, Chicago, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. The Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Midwest Integrated Center for Computational Materials (MICCoM); Argonne National Laboratory; USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF); Centers for Chemical Innovation (CCI)
OSTI Identifier:
1421969
Grant/Contract Number:
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 1; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; chalcogenide quantum dots; density functional theory; molecular dynamics; photovoltaic devices

Citation Formats

Greenwood, Arin R., Voros, Marton, Giberti, Federico, and Galli, Giulia. Emergent Electronic and Dielectric Properties of Interacting Nanoparticles at Finite Temperature. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.7b04047.
Greenwood, Arin R., Voros, Marton, Giberti, Federico, & Galli, Giulia. Emergent Electronic and Dielectric Properties of Interacting Nanoparticles at Finite Temperature. United States. doi:10.1021/acs.nanolett.7b04047.
Greenwood, Arin R., Voros, Marton, Giberti, Federico, and Galli, Giulia. Mon . "Emergent Electronic and Dielectric Properties of Interacting Nanoparticles at Finite Temperature". United States. doi:10.1021/acs.nanolett.7b04047.
@article{osti_1421969,
title = {Emergent Electronic and Dielectric Properties of Interacting Nanoparticles at Finite Temperature},
author = {Greenwood, Arin R. and Voros, Marton and Giberti, Federico and Galli, Giulia},
abstractNote = {Lead chalcogenide nanoparticle solids have been successfully integrated into certified solar cells and represent promising platforms for the design of novel photoabsorbers for photoelectrochemical cells. While much attention has been drawn to improving efficiency and device performance through altering the character of the individual nanoparticles, the role of interactions between nanoparticles is not yet well-understood. Using first-principles molecular dynamics and electronic structure calculations, we investigated the combined effect of temperature and interaction on functionalized lead chalcogenide nanoparticles (NPs). Here, we show that at finite temperature, interacting NPs are dynamical dipolar systems, with the average values of dipole moments and polarizabilities substantially increased with respect to those of the isolated building blocks. In addition, we show that the interacting NPs exhibit slightly smaller fundamental gaps that decrease as a function of temperature and that the radiative lifetimes of both the isolated NPs and the solids are greatly reduced at finite temperature compared to T = 0. Lastly, we present a critical discussion of various results reported in the literature for the values of dipole moments of nanoparticles.},
doi = {10.1021/acs.nanolett.7b04047},
journal = {Nano Letters},
number = 1,
volume = 18,
place = {United States},
year = {Mon Dec 11 00:00:00 EST 2017},
month = {Mon Dec 11 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
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