Preorganized Chromophores Facilitate Triplet Energy Migration, Annihilation and Upconverted Singlet Energy Collection.

Citation data:

Journal of the American Chemical Society, ISSN: 1520-5126, Vol: 138, Issue: 20, Page: 6541-9

Publication Year:
2016
Usage 14
Abstract Views 13
Link-outs 1
Captures 50
Readers 50
Mentions 1
Blog Mentions 1
Social Media 11
Shares, Likes & Comments 11
Citations 19
Citation Indexes 19
Repository URL:
http://scholarworks.unist.ac.kr/handle/201301/19679
PMID:
27163784
DOI:
10.1021/jacs.6b01652
Author(s):
Mahato, Prasenjit, Yanai, Nobuhiro, Sindoro, Melinda, Granick, Steve, Kimizuka, Noburo
Publisher(s):
American Chemical Society (ACS), AMER CHEMICAL SOC
Tags:
Chemical Engineering, Chemistry, Biochemistry, Genetics and Molecular Biology, Excitation intensity, Fluorescence efficiency, Fluorescence quantum yield, Metalorganic frameworks (MOFs), Molecular diffusion, Photocatalytic efficiency, Photon up conversions, Triplet-triplet annihilation
Most Recent Blog Mention
retraction description
Photon upconversion (UC) based on triplet-triplet annihilation (TTA) has the potential to enhance significantly photovoltaic and photocatalytic efficiencies by harnessing sub-bandgap photons, but the progress of this field is held back by the chemistry problem of how to preorganize multiple chromophores for efficient UC under weak solar irradiance. Recently, the first maximization of UC quantum yield at solar irradiance was achieved using fast triplet energy migration (TEM) in metal-organic frameworks (MOFs) with ordered acceptor arrays, but at the same time, a trade-off between fast TEM and high fluorescence efficiency was also found. Here, we provide a solution for this trade-off issue by developing a new strategy, triplet energy migration, annihilation and upconverted singlet energy collection (TEM-UPCON). The porous structure of acceptor-based MOF crystals allows triplet donor molecules to be accommodated without aggregation. The surface of donor-doped MOF nanocrystals is modified with highly fluorescent energy collectors through coordination bond formation. Thanks to the higher fluorescence quantum yield of surface-bound collectors than parent MOFs, the implementation of the energy collector greatly improves the total UC quantum yield. The UC quantum yield maximization behavior at ultralow excitation intensity was retained because the TTA events take place only in the MOF acceptors. The TEM-UPCON concept may be generalized to collectors with various functions and would lead to quantitative harvesting of upconverted energy, which is difficult to achieve in common molecular diffusion-based systems.

This retraction has 0 Wikipedia reference.