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Title: In situ Characterization of Kinetics and Mass Transport of PbSe Nanowire Growth via LS and VLS Mechanisms

Abstract

As a versatile approach, the vapor-liquid-solid (VLS) mechanism is widely used to grow nanowires. However, the details of the mass transit and mechanism of compound nanowire growth have been limited because of the complex growth process. In this study, we grew binary PbSe nanowires using an in situ gas-heating cell and elucidated two different growth mechanisms and mass transit pathways of different growth species, as well as their controlling factors, using in situ high-resolution transmission electron microscopy and composition analysis. Initial high supersaturation led to poly-nucleation and fast PbSe crystal growth through bulk diffusion of Pb and Se growth species from liquid to solid—a liquid-solid (LS) mechanism. In situ composition analysis showed that Pb dissolved in liquid catalyst at miscible atomic percentages as a precursor during growth. Se precursor was depleted after initial growth and was supplied from the vapor phase, leading to subsequently relatively slow VLS controlled mono-nuclear growth. We revealed the correlation between the nucleation mechanisms and the growth kinetics using a generalized Avrami model. Our study highlighted the key correlations among supersaturation, nucleation, mass transit, and growth kinetics, thereby enabling morphological and compositional control of nanowires.

Authors:
 [1];  [1];  [2];  [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. BATTELLE (PACIFIC NW LAB)
  2. UNIVERSITY PROGRAMS
  3. UNIVERSITY OF WASHINGTON
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1530601
Report Number(s):
PNNL-SA-135948
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 11; Journal Issue: 13
Country of Publication:
United States
Language:
English

Citation Formats

Song, Miao, Lee, Jaewon, Wang, Bin, Legg, Benjamin A., Hu, Shenyang, Chun, Jaehun, and Li, Dongsheng. In situ Characterization of Kinetics and Mass Transport of PbSe Nanowire Growth via LS and VLS Mechanisms. United States: N. p., 2019. Web. doi:10.1039/C9NR01200A.
Song, Miao, Lee, Jaewon, Wang, Bin, Legg, Benjamin A., Hu, Shenyang, Chun, Jaehun, & Li, Dongsheng. In situ Characterization of Kinetics and Mass Transport of PbSe Nanowire Growth via LS and VLS Mechanisms. United States. doi:10.1039/C9NR01200A.
Song, Miao, Lee, Jaewon, Wang, Bin, Legg, Benjamin A., Hu, Shenyang, Chun, Jaehun, and Li, Dongsheng. Sun . "In situ Characterization of Kinetics and Mass Transport of PbSe Nanowire Growth via LS and VLS Mechanisms". United States. doi:10.1039/C9NR01200A.
@article{osti_1530601,
title = {In situ Characterization of Kinetics and Mass Transport of PbSe Nanowire Growth via LS and VLS Mechanisms},
author = {Song, Miao and Lee, Jaewon and Wang, Bin and Legg, Benjamin A. and Hu, Shenyang and Chun, Jaehun and Li, Dongsheng},
abstractNote = {As a versatile approach, the vapor-liquid-solid (VLS) mechanism is widely used to grow nanowires. However, the details of the mass transit and mechanism of compound nanowire growth have been limited because of the complex growth process. In this study, we grew binary PbSe nanowires using an in situ gas-heating cell and elucidated two different growth mechanisms and mass transit pathways of different growth species, as well as their controlling factors, using in situ high-resolution transmission electron microscopy and composition analysis. Initial high supersaturation led to poly-nucleation and fast PbSe crystal growth through bulk diffusion of Pb and Se growth species from liquid to solid—a liquid-solid (LS) mechanism. In situ composition analysis showed that Pb dissolved in liquid catalyst at miscible atomic percentages as a precursor during growth. Se precursor was depleted after initial growth and was supplied from the vapor phase, leading to subsequently relatively slow VLS controlled mono-nuclear growth. We revealed the correlation between the nucleation mechanisms and the growth kinetics using a generalized Avrami model. Our study highlighted the key correlations among supersaturation, nucleation, mass transit, and growth kinetics, thereby enabling morphological and compositional control of nanowires.},
doi = {10.1039/C9NR01200A},
journal = {Nanoscale},
number = 13,
volume = 11,
place = {United States},
year = {2019},
month = {4}
}