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Title: Controlled Isotropic and Anisotropic Shell Growth in β-NaLnF4 Nanocrystals Induced by Precursor Injection Rate

Abstract

Precise morphology and composition control is vital for designing multifunctional lanthanide-doped core/shell nanocrystals. Herein, we report controlled isotropic and anisotropic shell growth techniques in hexagonal sodium rare-earth tetrafluoride (β-NaLnF4) nanocrystals by exploiting the kinetics of the shell growth. A drastic change of the shell morphology was observed by changing the injection rate of the shell precursors while keeping all other reaction conditions constant. We obtained isotropic shell growth for fast sequential injection and a preferred growth of the shell layers along the crystal's c-axis [001] for slow dropwise injection. Using this slow shell growth technique, we have grown rod-like shells around different almost spherical core nanocrystals. Bright and efficient upconversion was measured for both isotropic and rod-like shells around β-NaYF4 nanocrystals doped with Yb3+/Er3+ and Yb3+/Tm3+. Photoluminescence upconversion quantum yield and lifetime measurements reveal the high quality of the core/shell nanocrystal. Furthermore, multishell rod-like nanostructures have been prepared with optically active cores and tips separated by an inert intermediate shell layer. The controlled anisotropic shell growth allows the design of new core/multishell nanostructures and enables independent investigations of the chemistry and physics of different nanocrystal facets.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry and Dept. of Materials Science and Engineering; 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); German Research Foundation (DFG)
OSTI Identifier:
1532260
Grant/Contract Number:  
AC02-05CH11231; SC0001293
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 35; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Fischer, Stefan, Swabeck, Joseph K., and Alivisatos, A. Paul. Controlled Isotropic and Anisotropic Shell Growth in β-NaLnF4 Nanocrystals Induced by Precursor Injection Rate. United States: N. p., 2017. Web. doi:10.1021/jacs.7b07496.
Fischer, Stefan, Swabeck, Joseph K., & Alivisatos, A. Paul. Controlled Isotropic and Anisotropic Shell Growth in β-NaLnF4 Nanocrystals Induced by Precursor Injection Rate. United States. https://doi.org/10.1021/jacs.7b07496
Fischer, Stefan, Swabeck, Joseph K., and Alivisatos, A. Paul. Fri . "Controlled Isotropic and Anisotropic Shell Growth in β-NaLnF4 Nanocrystals Induced by Precursor Injection Rate". United States. https://doi.org/10.1021/jacs.7b07496. https://www.osti.gov/servlets/purl/1532260.
@article{osti_1532260,
title = {Controlled Isotropic and Anisotropic Shell Growth in β-NaLnF4 Nanocrystals Induced by Precursor Injection Rate},
author = {Fischer, Stefan and Swabeck, Joseph K. and Alivisatos, A. Paul},
abstractNote = {Precise morphology and composition control is vital for designing multifunctional lanthanide-doped core/shell nanocrystals. Herein, we report controlled isotropic and anisotropic shell growth techniques in hexagonal sodium rare-earth tetrafluoride (β-NaLnF4) nanocrystals by exploiting the kinetics of the shell growth. A drastic change of the shell morphology was observed by changing the injection rate of the shell precursors while keeping all other reaction conditions constant. We obtained isotropic shell growth for fast sequential injection and a preferred growth of the shell layers along the crystal's c-axis [001] for slow dropwise injection. Using this slow shell growth technique, we have grown rod-like shells around different almost spherical core nanocrystals. Bright and efficient upconversion was measured for both isotropic and rod-like shells around β-NaYF4 nanocrystals doped with Yb3+/Er3+ and Yb3+/Tm3+. Photoluminescence upconversion quantum yield and lifetime measurements reveal the high quality of the core/shell nanocrystal. Furthermore, multishell rod-like nanostructures have been prepared with optically active cores and tips separated by an inert intermediate shell layer. The controlled anisotropic shell growth allows the design of new core/multishell nanostructures and enables independent investigations of the chemistry and physics of different nanocrystal facets.},
doi = {10.1021/jacs.7b07496},
journal = {Journal of the American Chemical Society},
number = 35,
volume = 139,
place = {United States},
year = {Fri Aug 04 00:00:00 EDT 2017},
month = {Fri Aug 04 00:00:00 EDT 2017}
}

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