期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 16, 页码 5308-5315出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b01345
关键词
-
资金
- National Natural Science Foundation of PR China [21471126]
- National Thousand Talents Program of the PR of China
- 985 Program of Chemistry and Chemical Engineering disciplines of Xiamen University
- National Science Foundation [NSF/CHE-1346572]
- U.S. DOE [DE-AC02-06CH11357]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1346572] Funding Source: National Science Foundation
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 Forster 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 X 10(-2) cm(2)/s and 2.3 X 10(-2) cm(2)/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.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据