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Title: Long-Range Exciton Diffusion in Two-Dimensional Assemblies of Cesium Lead Bromide Perovskite Nanocrystals

Abstract

Förster resonant energy transfer (FRET)-mediated exciton diffusion through artificial nanoscale building block assemblies could be used as an optoelectronic design element to transport energy. However, so far, nanocrystal (NC) systems supported only diffusion lengths of 30 nm, which are too small to be useful in devices. In this work, we demonstrate a FRET-mediated exciton diffusion length of 200 nm with 0.5 cm 2/s diffusivity through an ordered, two-dimensional assembly of cesium lead bromide perovskite nanocrystals (CsPbBr 3 PNCs). Exciton diffusion was directly measured via steady-state and time-resolved photoluminescence (PL) microscopy, with physical modeling providing deeper insight into the transport process. This exceptionally efficient exciton transport is facilitated by PNCs' high PL quantum yield, large absorption cross section, and high polarizability, together with minimal energetic and geometric disorder of the assembly. This FRET-mediated exciton diffusion length matches perovskites' optical absorption depth, thus enabling the design of device architectures with improved performances and providing insight into the high conversion efficiencies of PNC-based optoelectronic devices.

Authors:
 [1];  [2];  [1];  [1];  [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [2];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. École Polytechnique Fédérale de Lausanne (Switzerland)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1642691
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 14; Journal Issue: 6; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
perovskite nanocrystals; exciton diffusion; optoelectronics; Forster resonant energy transfer; excitonic transport

Citation Formats

Penzo, Erika, Loiudice, Anna, Barnard, Edward S., Borys, Nicholas J., Jurow, Matthew J., Lorenzon, Monica, Rajzbaum, Igor, Wong, Edward K., Liu, Yi, Schwartzberg, Adam M., Cabrini, Stefano, Whitelam, Stephen, Buonsanti, Raffaella, and Weber-Bargioni, Alexander. Long-Range Exciton Diffusion in Two-Dimensional Assemblies of Cesium Lead Bromide Perovskite Nanocrystals. United States: N. p., 2020. Web. doi:10.1021/acsnano.0c01536.
Penzo, Erika, Loiudice, Anna, Barnard, Edward S., Borys, Nicholas J., Jurow, Matthew J., Lorenzon, Monica, Rajzbaum, Igor, Wong, Edward K., Liu, Yi, Schwartzberg, Adam M., Cabrini, Stefano, Whitelam, Stephen, Buonsanti, Raffaella, & Weber-Bargioni, Alexander. Long-Range Exciton Diffusion in Two-Dimensional Assemblies of Cesium Lead Bromide Perovskite Nanocrystals. United States. doi:10.1021/acsnano.0c01536.
Penzo, Erika, Loiudice, Anna, Barnard, Edward S., Borys, Nicholas J., Jurow, Matthew J., Lorenzon, Monica, Rajzbaum, Igor, Wong, Edward K., Liu, Yi, Schwartzberg, Adam M., Cabrini, Stefano, Whitelam, Stephen, Buonsanti, Raffaella, and Weber-Bargioni, Alexander. Wed . "Long-Range Exciton Diffusion in Two-Dimensional Assemblies of Cesium Lead Bromide Perovskite Nanocrystals". United States. doi:10.1021/acsnano.0c01536.
@article{osti_1642691,
title = {Long-Range Exciton Diffusion in Two-Dimensional Assemblies of Cesium Lead Bromide Perovskite Nanocrystals},
author = {Penzo, Erika and Loiudice, Anna and Barnard, Edward S. and Borys, Nicholas J. and Jurow, Matthew J. and Lorenzon, Monica and Rajzbaum, Igor and Wong, Edward K. and Liu, Yi and Schwartzberg, Adam M. and Cabrini, Stefano and Whitelam, Stephen and Buonsanti, Raffaella and Weber-Bargioni, Alexander},
abstractNote = {Förster resonant energy transfer (FRET)-mediated exciton diffusion through artificial nanoscale building block assemblies could be used as an optoelectronic design element to transport energy. However, so far, nanocrystal (NC) systems supported only diffusion lengths of 30 nm, which are too small to be useful in devices. In this work, we demonstrate a FRET-mediated exciton diffusion length of 200 nm with 0.5 cm2/s diffusivity through an ordered, two-dimensional assembly of cesium lead bromide perovskite nanocrystals (CsPbBr3 PNCs). Exciton diffusion was directly measured via steady-state and time-resolved photoluminescence (PL) microscopy, with physical modeling providing deeper insight into the transport process. This exceptionally efficient exciton transport is facilitated by PNCs' high PL quantum yield, large absorption cross section, and high polarizability, together with minimal energetic and geometric disorder of the assembly. This FRET-mediated exciton diffusion length matches perovskites' optical absorption depth, thus enabling the design of device architectures with improved performances and providing insight into the high conversion efficiencies of PNC-based optoelectronic devices.},
doi = {10.1021/acsnano.0c01536},
journal = {ACS Nano},
issn = {1936-0851},
number = 6,
volume = 14,
place = {United States},
year = {2020},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on May 27, 2021
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