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Title: A Mechanistic Understanding of Nonclassical Crystal Growth in Hydrothermally Synthesized Sodium Yttrium Fluoride Nanowires

Abstract

Sodium yttrium fluoride (NaYF4) is an important upconverting material with many potential uses in chemistry, materials science, and biology, which can be synthesized hydrothermally in both cubic (a) and hexagonal (ß) crystallographic polymorphs. Understanding the mechanisms underlying the phase conversion between the cubic and hexagonal polymorphs is of great interest to help inform future efforts to synthesize atomically-precise quantum materials with well-defined sizes and morphologies. In this work, we use a combination of analytical transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM), powder X-ray diffraction (XRD), in situ liquid cell TEM, atom probe tomography (APT), and extended x-ray absorption fine structure (EXAFS) measurements to show that the hexagonal NaYF4 nanowires form through a non-classical crystal growth mechanism involving the formation and subsequent oriented attachment of mesocrystals consisting of cubic (a) phase units. EXAFS spectroscopy also suggests that substitutional Yb3+ point defects within NaYF4 are distributed evenly throughout the crystal lattice without clustering, and also that they may exhibit selective substitution into one of the two possible trivalent yttrium sites in the unit cell in hydrothermally synthesized ß-NaYF4.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [2]; ORCiD logo [1];  [3];  [1];  [1];  [4]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [2]; ORCiD logo [7]
  1. Univ. of Washington, Seattle, WA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)
  3. Korea Inst. of Science and Technology, Jeonbuk (Republic of Korea)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  6. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  7. Univ. of Washington, Seattle, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF)
OSTI Identifier:
1602835
Alternate Identifier(s):
OSTI ID: 1638492
Report Number(s):
PNNL-SA-147967
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
AC05-76RL01830; AC02-05CH11231; ECC-1542101
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 32; Journal Issue: 7; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Crystallization; Nanowires; Nanoparticles; Crystal structure; Transmission electron microscopy

Citation Formats

Bard, Alexander B., Zhou, Xuezhe, Xia, Xiaojing, Zhu, Guomin, Lim, Matthew B., Kim, Seung Min, Johnson, Matthew C., Kollman, Justin M., Marcus, Matthew A., Spurgeon, Steven R., Perea, Daniel E., Devaraj, Arun, Chun, Jaehun, De Yoreo, James J., and Pauzauskie, Peter J.. A Mechanistic Understanding of Nonclassical Crystal Growth in Hydrothermally Synthesized Sodium Yttrium Fluoride Nanowires. United States: N. p., 2020. Web. https://doi.org/10.1021/acs.chemmater.9b04076.
Bard, Alexander B., Zhou, Xuezhe, Xia, Xiaojing, Zhu, Guomin, Lim, Matthew B., Kim, Seung Min, Johnson, Matthew C., Kollman, Justin M., Marcus, Matthew A., Spurgeon, Steven R., Perea, Daniel E., Devaraj, Arun, Chun, Jaehun, De Yoreo, James J., & Pauzauskie, Peter J.. A Mechanistic Understanding of Nonclassical Crystal Growth in Hydrothermally Synthesized Sodium Yttrium Fluoride Nanowires. United States. https://doi.org/10.1021/acs.chemmater.9b04076
Bard, Alexander B., Zhou, Xuezhe, Xia, Xiaojing, Zhu, Guomin, Lim, Matthew B., Kim, Seung Min, Johnson, Matthew C., Kollman, Justin M., Marcus, Matthew A., Spurgeon, Steven R., Perea, Daniel E., Devaraj, Arun, Chun, Jaehun, De Yoreo, James J., and Pauzauskie, Peter J.. Wed . "A Mechanistic Understanding of Nonclassical Crystal Growth in Hydrothermally Synthesized Sodium Yttrium Fluoride Nanowires". United States. https://doi.org/10.1021/acs.chemmater.9b04076. https://www.osti.gov/servlets/purl/1602835.
@article{osti_1602835,
title = {A Mechanistic Understanding of Nonclassical Crystal Growth in Hydrothermally Synthesized Sodium Yttrium Fluoride Nanowires},
author = {Bard, Alexander B. and Zhou, Xuezhe and Xia, Xiaojing and Zhu, Guomin and Lim, Matthew B. and Kim, Seung Min and Johnson, Matthew C. and Kollman, Justin M. and Marcus, Matthew A. and Spurgeon, Steven R. and Perea, Daniel E. and Devaraj, Arun and Chun, Jaehun and De Yoreo, James J. and Pauzauskie, Peter J.},
abstractNote = {Sodium yttrium fluoride (NaYF4) is an important upconverting material with many potential uses in chemistry, materials science, and biology, which can be synthesized hydrothermally in both cubic (a) and hexagonal (ß) crystallographic polymorphs. Understanding the mechanisms underlying the phase conversion between the cubic and hexagonal polymorphs is of great interest to help inform future efforts to synthesize atomically-precise quantum materials with well-defined sizes and morphologies. In this work, we use a combination of analytical transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM), powder X-ray diffraction (XRD), in situ liquid cell TEM, atom probe tomography (APT), and extended x-ray absorption fine structure (EXAFS) measurements to show that the hexagonal NaYF4 nanowires form through a non-classical crystal growth mechanism involving the formation and subsequent oriented attachment of mesocrystals consisting of cubic (a) phase units. EXAFS spectroscopy also suggests that substitutional Yb3+ point defects within NaYF4 are distributed evenly throughout the crystal lattice without clustering, and also that they may exhibit selective substitution into one of the two possible trivalent yttrium sites in the unit cell in hydrothermally synthesized ß-NaYF4.},
doi = {10.1021/acs.chemmater.9b04076},
journal = {Chemistry of Materials},
number = 7,
volume = 32,
place = {United States},
year = {2020},
month = {2}
}

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