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Title: Förster Energy Transport in Metal–Organic Frameworks Is Beyond Step-by-Step Hopping

Abstract

Metal–organic frameworks (MOFs) with light-harvesting building blocks designed to mimic photosynthetic chromophore arrays in green plants provide an excellent platform to study exciton transport in networks with well-defined structures. A step-by-step exciton random hopping model made of the elementary steps of energy transfer between only the nearest neighbors is usually used to describe the transport dynamics. Although such a nearest neighbor approximation is valid in describing the energy transfer of triplet states via the Dexter mechanism, we found it inadequate in evaluating singlet exciton migration that occurs through the Förster mechanism, which involves one-step jumping over longer distance. We measured migration rates of singlet excitons on two MOFs constructed from truxene-derived ligands and zinc nodes, by monitoring energy transfer from the MOF skeleton to a coumarin probe in the MOF cavity. The diffusivities of the excitons on the frameworks were determined to be 1.8 × 10–2 cm2/s and 2.3 × 10–2 cm2/s, corresponding to migration distances of 43 and 48 nm within their lifetimes, respectively. “Through space” energy-jumping beyond nearest neighbor accounts for up to 67% of the energy transfer rates. This finding presents a new perspective in the design and understanding of highly efficient energy transport networks for singletmore » excited states.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [2];  [1];  [1];  [1];  [3]
  1. Xiamen Univ. (China)
  2. Univ. of Chicago, IL (United States)
  3. Xiamen Univ. (China); Univ. of Chicago, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1247615
Alternate Identifier(s):
OSTI ID: 1337702
Grant/Contract Number:  
21471126; NSF/CHE-1346572; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 16; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Dyes and pigments; Excitons; Energy transfer; Ligands; Metal organic frameworks

Citation Formats

Zhang, Qiongqiong, Zhang, Cankun, Cao, Lingyun, Wang, Zi, An, Bing, Lin, Zekai, Huang, Ruiyun, Zhang, Zhiming, Wang, Cheng, and Lin, Wenbin. Förster Energy Transport in Metal–Organic Frameworks Is Beyond Step-by-Step Hopping. United States: N. p., 2016. Web. doi:10.1021/jacs.6b01345.
Zhang, Qiongqiong, Zhang, Cankun, Cao, Lingyun, Wang, Zi, An, Bing, Lin, Zekai, Huang, Ruiyun, Zhang, Zhiming, Wang, Cheng, & Lin, Wenbin. Förster Energy Transport in Metal–Organic Frameworks Is Beyond Step-by-Step Hopping. United States. https://doi.org/10.1021/jacs.6b01345
Zhang, Qiongqiong, Zhang, Cankun, Cao, Lingyun, Wang, Zi, An, Bing, Lin, Zekai, Huang, Ruiyun, Zhang, Zhiming, Wang, Cheng, and Lin, Wenbin. Fri . "Förster Energy Transport in Metal–Organic Frameworks Is Beyond Step-by-Step Hopping". United States. https://doi.org/10.1021/jacs.6b01345.
@article{osti_1247615,
title = {Förster Energy Transport in Metal–Organic Frameworks Is Beyond Step-by-Step Hopping},
author = {Zhang, Qiongqiong and Zhang, Cankun and Cao, Lingyun and Wang, Zi and An, Bing and Lin, Zekai and Huang, Ruiyun and Zhang, Zhiming and Wang, Cheng and Lin, Wenbin},
abstractNote = {Metal–organic frameworks (MOFs) with light-harvesting building blocks designed to mimic photosynthetic chromophore arrays in green plants provide an excellent platform to study exciton transport in networks with well-defined structures. A step-by-step exciton random hopping model made of the elementary steps of energy transfer between only the nearest neighbors is usually used to describe the transport dynamics. Although such a nearest neighbor approximation is valid in describing the energy transfer of triplet states via the Dexter mechanism, we found it inadequate in evaluating singlet exciton migration that occurs through the Förster mechanism, which involves one-step jumping over longer distance. We measured migration rates of singlet excitons on two MOFs constructed from truxene-derived ligands and zinc nodes, by monitoring energy transfer from the MOF skeleton to a coumarin probe in the MOF cavity. The diffusivities of the excitons on the frameworks were determined to be 1.8 × 10–2 cm2/s and 2.3 × 10–2 cm2/s, corresponding to migration distances of 43 and 48 nm within their lifetimes, respectively. “Through space” energy-jumping beyond nearest neighbor accounts for up to 67% of the energy transfer rates. This finding presents a new perspective in the design and understanding of highly efficient energy transport networks for singlet excited states.},
doi = {10.1021/jacs.6b01345},
journal = {Journal of the American Chemical Society},
number = 16,
volume = 138,
place = {United States},
year = {2016},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/jacs.6b01345

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