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Title: Precise Tuning of Surface Quenching for Luminescence Enhancement in Core–Shell Lanthanide-Doped Nanocrystals

Abstract

Lanthanide-doped nanocrystals are of particular interest for the research community not only due to their ability to shape light by downshifting, quantum cutting, and upconversion but also because novel optical properties can be found by the precise engineering of core-shell nanocrystals. Because of the large surface area-to-volume ratio of nanocrystals, the luminescence is typically suppressed by surface quenching. Here, we demonstrate a mechanism that exploits surface quenching processes to improve the luminescence of our core-shell lanthanide-doped nanocrystals. By carefully tuning the shell thickness of inert β-NaLuF4 around β-NaYF4 nanocrystals doped with Yb3+ and Er3+, we unravel the relationship between quantum yield and shell thickness, and quantify surface quenching rates for the relevant Er3+ and Yb3+ energy levels. This enhanced understanding of the system's dynamics allowed us to design nanocrystals with a surface quenching-assisted mechanism for bright NIR to NIR downshifting with a distinctive efficiency peak for an optimized shell thickness.

Authors:
 [1];  [1];  [1];  [2];  [3]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Inst., Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Light-Material Interactions in Energy Conversion (LMI)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1532207
Grant/Contract Number:  
AC02-05CH11231; SC0001293
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 16; Journal Issue: 11; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Fischer, Stefan, Bronstein, Noah D., Swabeck, Joseph K., Chan, Emory M., and Alivisatos, A. Paul. Precise Tuning of Surface Quenching for Luminescence Enhancement in Core–Shell Lanthanide-Doped Nanocrystals. United States: N. p., 2016. Web. doi:10.1021/acs.nanolett.6b03683.
Fischer, Stefan, Bronstein, Noah D., Swabeck, Joseph K., Chan, Emory M., & Alivisatos, A. Paul. Precise Tuning of Surface Quenching for Luminescence Enhancement in Core–Shell Lanthanide-Doped Nanocrystals. United States. https://doi.org/10.1021/acs.nanolett.6b03683
Fischer, Stefan, Bronstein, Noah D., Swabeck, Joseph K., Chan, Emory M., and Alivisatos, A. Paul. Tue . "Precise Tuning of Surface Quenching for Luminescence Enhancement in Core–Shell Lanthanide-Doped Nanocrystals". United States. https://doi.org/10.1021/acs.nanolett.6b03683. https://www.osti.gov/servlets/purl/1532207.
@article{osti_1532207,
title = {Precise Tuning of Surface Quenching for Luminescence Enhancement in Core–Shell Lanthanide-Doped Nanocrystals},
author = {Fischer, Stefan and Bronstein, Noah D. and Swabeck, Joseph K. and Chan, Emory M. and Alivisatos, A. Paul},
abstractNote = {Lanthanide-doped nanocrystals are of particular interest for the research community not only due to their ability to shape light by downshifting, quantum cutting, and upconversion but also because novel optical properties can be found by the precise engineering of core-shell nanocrystals. Because of the large surface area-to-volume ratio of nanocrystals, the luminescence is typically suppressed by surface quenching. Here, we demonstrate a mechanism that exploits surface quenching processes to improve the luminescence of our core-shell lanthanide-doped nanocrystals. By carefully tuning the shell thickness of inert β-NaLuF4 around β-NaYF4 nanocrystals doped with Yb3+ and Er3+, we unravel the relationship between quantum yield and shell thickness, and quantify surface quenching rates for the relevant Er3+ and Yb3+ energy levels. This enhanced understanding of the system's dynamics allowed us to design nanocrystals with a surface quenching-assisted mechanism for bright NIR to NIR downshifting with a distinctive efficiency peak for an optimized shell thickness.},
doi = {10.1021/acs.nanolett.6b03683},
journal = {Nano Letters},
number = 11,
volume = 16,
place = {United States},
year = {Tue Oct 11 00:00:00 EDT 2016},
month = {Tue Oct 11 00:00:00 EDT 2016}
}

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