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Title: Apparent self-heating of individual upconverting nanoparticle thermometers

Abstract

Individual luminescent nanoparticles enable thermometry with sub-diffraction limited spatial resolution, but potential self-heating effects from high single-particle excitation intensities remain largely uninvestigated because thermal models predict negligible self-heating. Here, we report that the common "ratiometric" thermometry signal of individual NaYF 4:Yb 3+,Er 3+ nanoparticles unexpectedly increases with excitation intensity, implying a temperature rise over 50 K if interpreted as thermal. Luminescence lifetime thermometry, which we demonstrate for the first time using individual NaYF 4:Yb 3+,Er 3+ nanoparticles, indicates a similar temperature rise. To resolve this apparent contradiction between model and experiment, we systematically vary the nanoparticle's thermal environment: the substrate thermal conductivity, nanoparticle-substrate contact resistance, and nanoparticle size. The apparent self-heating remains unchanged, demonstrating that this effect is an artifact, not a real temperature rise. Using rate equation modeling, we show that this artifact results from increased radiative and non-radiative relaxation from higher-lying Er 3+ energy levels. This study has important implications for single-particle thermometry.

Authors:
 [1];  [2];  [2];  [2];  [3];  [4]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Mechanical Engineering
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Columbia Univ., New York, NY (United States). Dept. of Mechanical Engineering
  4. Univ. of California, Berkeley, CA (United States). Dept. of Mechanical Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Materials Sciences & Engineering Division (SC-22.2); National Science Foundation (NSF)
OSTI Identifier:
1493268
Grant/Contract Number:  
AC02-05CH11231; 1512796; DGE 1752814
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Pickel, Andrea D., Teitelboim, Ayelet, Chan, Emory M., Borys, Nicholas J., Schuck, P. James, and Dames, Chris. Apparent self-heating of individual upconverting nanoparticle thermometers. United States: N. p., 2018. Web. doi:10.1038/s41467-018-07361-0.
Pickel, Andrea D., Teitelboim, Ayelet, Chan, Emory M., Borys, Nicholas J., Schuck, P. James, & Dames, Chris. Apparent self-heating of individual upconverting nanoparticle thermometers. United States. doi:10.1038/s41467-018-07361-0.
Pickel, Andrea D., Teitelboim, Ayelet, Chan, Emory M., Borys, Nicholas J., Schuck, P. James, and Dames, Chris. Wed . "Apparent self-heating of individual upconverting nanoparticle thermometers". United States. doi:10.1038/s41467-018-07361-0. https://www.osti.gov/servlets/purl/1493268.
@article{osti_1493268,
title = {Apparent self-heating of individual upconverting nanoparticle thermometers},
author = {Pickel, Andrea D. and Teitelboim, Ayelet and Chan, Emory M. and Borys, Nicholas J. and Schuck, P. James and Dames, Chris},
abstractNote = {Individual luminescent nanoparticles enable thermometry with sub-diffraction limited spatial resolution, but potential self-heating effects from high single-particle excitation intensities remain largely uninvestigated because thermal models predict negligible self-heating. Here, we report that the common "ratiometric" thermometry signal of individual NaYF4:Yb3+,Er3+ nanoparticles unexpectedly increases with excitation intensity, implying a temperature rise over 50 K if interpreted as thermal. Luminescence lifetime thermometry, which we demonstrate for the first time using individual NaYF4:Yb3+,Er3+ nanoparticles, indicates a similar temperature rise. To resolve this apparent contradiction between model and experiment, we systematically vary the nanoparticle's thermal environment: the substrate thermal conductivity, nanoparticle-substrate contact resistance, and nanoparticle size. The apparent self-heating remains unchanged, demonstrating that this effect is an artifact, not a real temperature rise. Using rate equation modeling, we show that this artifact results from increased radiative and non-radiative relaxation from higher-lying Er3+ energy levels. This study has important implications for single-particle thermometry.},
doi = {10.1038/s41467-018-07361-0},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Wed Nov 21 00:00:00 EST 2018},
month = {Wed Nov 21 00:00:00 EST 2018}
}

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Works referenced in this record:

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