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Title: Low irradiance multiphoton imaging with alloyed lanthanide nanocrystals

Multiphoton imaging techniques that convert low-energy excitation to higher energy emission are widely used to improve signal over background, reduce scatter, and limit photodamage. Lanthanide-doped upconverting nanoparticles (UCNPs) are among the most efficient multiphoton probes, but even UCNPs with optimized lanthanide dopant levels require laser intensities that may be problematic. Here, we develop protein-sized, alloyed UCNPs (aUCNPs) that can be imaged individually at laser intensities >300-fold lower than needed for comparably sized doped UCNPs. Using single UCNP characterization and kinetic modeling, we find that addition of inert shells changes optimal lanthanide content from Yb 3+, Er 3+-doped NaYF 4 nanocrystals to fully alloyed compositions. At high levels, emitter Er 3+ ions can adopt a second role to enhance aUCNP absorption cross-section by desaturating sensitizer Yb 3+ or by absorbing photons directly. Core/shell aUCNPs 12 nm in total diameter can be imaged through deep tissue in live mice using a laser intensity of 0.1 W cm -2.
Authors:
 [1] ;  [1] ;  [2] ;  [3] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [1] ;  [4] ;  [1] ;  [5] ; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
  2. Univ. of California, Berkeley, CA (United States). Dept. of Electrical Engineering and Computer Sciences
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry; Univ. of California, San Francisco, CA (United States). Dept. of Radiation Oncology
  4. Univ. of California, San Francisco, CA (United States). Dept. of Radiation Oncology
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry; Columbia Univ., New York, NY (United States). Dept. of Mechanical Engineering
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Chinese Scholarship Council (CSC); Weizmann Inst. of Science (Israel)
Country of Publication:
United States
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; materials for optics; nanoparticles; nonlinear optics
OSTI Identifier:
1462284
Alternate Identifier(s):
OSTI ID: 1477411

Tian, Bining, Fernandez-Bravo, Angel, Najafiaghdam, Hossein, Torquato, Nicole A., Altoe, M. Virginia P., Teitelboim, Ayelet, Tajon, Cheryl A., Tian, Yue, Borys, Nicholas J., Barnard, Edward S., Anwar, Mekhail, Chan, Emory M., Schuck, P. James, and Cohen, Bruce E.. Low irradiance multiphoton imaging with alloyed lanthanide nanocrystals. United States: N. p., Web. doi:10.1038/s41467-018-05577-8.
Tian, Bining, Fernandez-Bravo, Angel, Najafiaghdam, Hossein, Torquato, Nicole A., Altoe, M. Virginia P., Teitelboim, Ayelet, Tajon, Cheryl A., Tian, Yue, Borys, Nicholas J., Barnard, Edward S., Anwar, Mekhail, Chan, Emory M., Schuck, P. James, & Cohen, Bruce E.. Low irradiance multiphoton imaging with alloyed lanthanide nanocrystals. United States. doi:10.1038/s41467-018-05577-8.
Tian, Bining, Fernandez-Bravo, Angel, Najafiaghdam, Hossein, Torquato, Nicole A., Altoe, M. Virginia P., Teitelboim, Ayelet, Tajon, Cheryl A., Tian, Yue, Borys, Nicholas J., Barnard, Edward S., Anwar, Mekhail, Chan, Emory M., Schuck, P. James, and Cohen, Bruce E.. 2018. "Low irradiance multiphoton imaging with alloyed lanthanide nanocrystals". United States. doi:10.1038/s41467-018-05577-8.
@article{osti_1462284,
title = {Low irradiance multiphoton imaging with alloyed lanthanide nanocrystals},
author = {Tian, Bining and Fernandez-Bravo, Angel and Najafiaghdam, Hossein and Torquato, Nicole A. and Altoe, M. Virginia P. and Teitelboim, Ayelet and Tajon, Cheryl A. and Tian, Yue and Borys, Nicholas J. and Barnard, Edward S. and Anwar, Mekhail and Chan, Emory M. and Schuck, P. James and Cohen, Bruce E.},
abstractNote = {Multiphoton imaging techniques that convert low-energy excitation to higher energy emission are widely used to improve signal over background, reduce scatter, and limit photodamage. Lanthanide-doped upconverting nanoparticles (UCNPs) are among the most efficient multiphoton probes, but even UCNPs with optimized lanthanide dopant levels require laser intensities that may be problematic. Here, we develop protein-sized, alloyed UCNPs (aUCNPs) that can be imaged individually at laser intensities >300-fold lower than needed for comparably sized doped UCNPs. Using single UCNP characterization and kinetic modeling, we find that addition of inert shells changes optimal lanthanide content from Yb3+, Er3+-doped NaYF4 nanocrystals to fully alloyed compositions. At high levels, emitter Er3+ ions can adopt a second role to enhance aUCNP absorption cross-section by desaturating sensitizer Yb3+ or by absorbing photons directly. Core/shell aUCNPs 12 nm in total diameter can be imaged through deep tissue in live mice using a laser intensity of 0.1 W cm-2.},
doi = {10.1038/s41467-018-05577-8},
journal = {Nature Communications},
number = ,
volume = 9,
place = {United States},
year = {2018},
month = {8}
}

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