Förster Energy Transport in Metal–Organic Frameworks Is Beyond Step-by-Step Hoppingстатья из журнала
Аннотация: 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.
Год издания: 2016
Авторы: Qiongqiong Zhang, Cankun Zhang, Lingyun Cao, Zi Wang, Bing An, Zekai Lin, Ruiyun Huang, Zhiming Zhang, Cheng Wang, Wenbin Lin
Издательство: American Chemical Society
Источник: Journal of the American Chemical Society
Ключевые слова: Metal-Organic Frameworks: Synthesis and Applications, Electrochemical Analysis and Applications, Machine Learning and ELM
Другие ссылки: Journal of the American Chemical Society (HTML)
OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (HTML)
OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (HTML)
PubMed (HTML)
OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (HTML)
OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (HTML)
PubMed (HTML)
Открытый доступ: hybrid
Том: 138
Выпуск: 16
Страницы: 5308–5315