BROWSE

Related Researcher

Author

Granick, Steve
CSLM(Center for Soft and Living Matter) Lab
Research Interests
  • Chemistry, physics, biology, engineering

ITEM VIEW & DOWNLOAD

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

Cited 0 times inthomson ciCited 0 times inthomson ci
Title
Preorganized Chromophores Facilitate Triplet Energy Migration, Annihilation and Upconverted Singlet Energy Collection
Author
Mahato, PrasenjitYanai, NobuhiroSindoro, MelindaGranick, SteveKimizuka, Noburo
Keywords
Excitation intensity; Fluorescence efficiency; Fluorescence quantum yield; Metalorganic frameworks (MOFs); Molecular diffusion; Photocatalytic efficiency; Photon up conversions; Triplet-triplet annihilation
Issue Date
201605
Publisher
AMER CHEMICAL SOC
Citation
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.138, no.20, pp.6541 - 6549
Abstract
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.
URI
Go to Link
DOI
http://dx.doi.org/10.1021/jacs.6b01652
ISSN
0002-7863
Appears in Collections:
SNS_Journal Papers

find_unist can give you direct access to the published full text of this article. (UNISTARs only)

Show full item record

qr_code

  • mendeley

    citeulike

Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.

MENU