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Title: Enhanced Ultraviolet Photon Capture in Ligand-Sensitized Nanocrystals

The small absorption cross sections (ϵ < 10 M -1 cm -1 ) characteristic of Laporte-forbidden transitions in the f-elements have limited the practical implementation of lanthanide nanoparticles in solar capture devices. And while various strategies designed to circumvent the problems of low f-f oscillator strengths have been investigated, comparatively little work has explored the utility of organic ligands with high absorption coefficients (ϵ ≈ 10 3 -10 5 M -1 cm -1 ) in sensitizing excited states in lanthanide nanocrystals. Here, we detail the photophysics of NaGd 1-x Eu x F 4 nanoparticles featuring surface display of the ligand 3,4,3-LI(1,2-HOPO), an aromatic antenna functioning as the terminal light absorber in this system. The result is a ligand-nanocrystal hybrid that converts UV (250-360 nm) light into red Eu(III) luminescence with an external quantum yield of 3.3%. Here, we analyze this sensitization process, responsible for a 10 4 -fold increase in luminescence relative to metal-centered excitation, through a quantitative treatment of energy transfer between ligand and metal states.
Authors:
 [1] ;  [1] ;  [1] ;  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
ACS Photonics
Additional Journal Information:
Journal Volume: 3; Journal Issue: 4; Journal ID: ISSN 2330-4022
Publisher:
American Chemical Society (ACS)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; energy transfer; lanthanide; ligand antenna; nanocrystal; sensitization
OSTI Identifier:
1416910

Agbo, Peter, Xu, Tao, Sturzbecher-Hoehne, Manuel, and Abergel, Rebecca J. Enhanced Ultraviolet Photon Capture in Ligand-Sensitized Nanocrystals. United States: N. p., Web. doi:10.1021/acsphotonics.6b00118.
Agbo, Peter, Xu, Tao, Sturzbecher-Hoehne, Manuel, & Abergel, Rebecca J. Enhanced Ultraviolet Photon Capture in Ligand-Sensitized Nanocrystals. United States. doi:10.1021/acsphotonics.6b00118.
Agbo, Peter, Xu, Tao, Sturzbecher-Hoehne, Manuel, and Abergel, Rebecca J. 2016. "Enhanced Ultraviolet Photon Capture in Ligand-Sensitized Nanocrystals". United States. doi:10.1021/acsphotonics.6b00118. https://www.osti.gov/servlets/purl/1416910.
@article{osti_1416910,
title = {Enhanced Ultraviolet Photon Capture in Ligand-Sensitized Nanocrystals},
author = {Agbo, Peter and Xu, Tao and Sturzbecher-Hoehne, Manuel and Abergel, Rebecca J.},
abstractNote = {The small absorption cross sections (ϵ < 10 M -1 cm -1 ) characteristic of Laporte-forbidden transitions in the f-elements have limited the practical implementation of lanthanide nanoparticles in solar capture devices. And while various strategies designed to circumvent the problems of low f-f oscillator strengths have been investigated, comparatively little work has explored the utility of organic ligands with high absorption coefficients (ϵ ≈ 10 3 -10 5 M -1 cm -1 ) in sensitizing excited states in lanthanide nanocrystals. Here, we detail the photophysics of NaGd 1-x Eu x F 4 nanoparticles featuring surface display of the ligand 3,4,3-LI(1,2-HOPO), an aromatic antenna functioning as the terminal light absorber in this system. The result is a ligand-nanocrystal hybrid that converts UV (250-360 nm) light into red Eu(III) luminescence with an external quantum yield of 3.3%. Here, we analyze this sensitization process, responsible for a 10 4 -fold increase in luminescence relative to metal-centered excitation, through a quantitative treatment of energy transfer between ligand and metal states.},
doi = {10.1021/acsphotonics.6b00118},
journal = {ACS Photonics},
number = 4,
volume = 3,
place = {United States},
year = {2016},
month = {4}
}