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Title: Selective Facet Reactivity During Cation Exchange in Cadmium Sulfide Nanorods

Abstract

The partial transformation of ionic nanocrystals through cation exchange has been used to synthesize nanocrystal heterostructures. We demonstrate that the selectivity for cation exchange to take place at different facets of the nanocrystal plays an important role in determining the resulting morphology of the binary heterostructure. In the case of copper I (Cu+) cation exchange in cadmium sulfide (CdS) nanorods, the reaction starts preferentially at the ends of the nanorods such that copper sulfide (Cu2S) grows inwards from either end. The resulting morphology is very different from the striped pattern obtained in our previous studies of silver I (Ag+) exchange in CdS nanorods where non-selective nucleation of silver sulfide (Ag2S) occurs. From interface formation energies calculated for several models of epitaxialconnections between CdS and Cu2S or Ag2S, we infer the relative stability of each interface during the nucleation and growth of Cu2S or Ag2S within the CdS nanorods. The epitaxial connections of Cu2S to the end facets of CdS nanorods minimize the formation energy, making these interfaces stable throughout the exchange reaction. However, as the two end facets of wurtzite CdS nanorods are crystallographically nonequivalent, asymmetric heterostructures can be produced.

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
Computational Research Division; Materials Sciences Division
OSTI Identifier:
962717
Report Number(s):
LBNL-1385E
Journal ID: ISSN 0002-7863; JACSAT; TRN: US200916%%350
DOE Contract Number:  
DE-AC02-05CH11231
Resource Type:
Journal Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 131; Journal Issue: 14; Journal ID: ISSN 0002-7863
Country of Publication:
United States
Language:
English
Subject:
77; CADMIUM SULFIDES; CATIONS; COPPER; COPPER SULFIDES; MORPHOLOGY; NUCLEATION; SILVER; SILVER SULFIDES; STABILITY; TRANSFORMATIONS; nanocrystals, cation exchange

Citation Formats

Sadtler, Bryce, Demchenko, Denis, Zheng, Haimei, Hughes, Steven, Merkle, Maxwell, Dahmen, Ulrich, Wang, Lin-Wang, and Alivisatos, A Paul. Selective Facet Reactivity During Cation Exchange in Cadmium Sulfide Nanorods. United States: N. p., 2008. Web.
Sadtler, Bryce, Demchenko, Denis, Zheng, Haimei, Hughes, Steven, Merkle, Maxwell, Dahmen, Ulrich, Wang, Lin-Wang, & Alivisatos, A Paul. Selective Facet Reactivity During Cation Exchange in Cadmium Sulfide Nanorods. United States.
Sadtler, Bryce, Demchenko, Denis, Zheng, Haimei, Hughes, Steven, Merkle, Maxwell, Dahmen, Ulrich, Wang, Lin-Wang, and Alivisatos, A Paul. 2008. "Selective Facet Reactivity During Cation Exchange in Cadmium Sulfide Nanorods". United States. https://www.osti.gov/servlets/purl/962717.
@article{osti_962717,
title = {Selective Facet Reactivity During Cation Exchange in Cadmium Sulfide Nanorods},
author = {Sadtler, Bryce and Demchenko, Denis and Zheng, Haimei and Hughes, Steven and Merkle, Maxwell and Dahmen, Ulrich and Wang, Lin-Wang and Alivisatos, A Paul},
abstractNote = {The partial transformation of ionic nanocrystals through cation exchange has been used to synthesize nanocrystal heterostructures. We demonstrate that the selectivity for cation exchange to take place at different facets of the nanocrystal plays an important role in determining the resulting morphology of the binary heterostructure. In the case of copper I (Cu+) cation exchange in cadmium sulfide (CdS) nanorods, the reaction starts preferentially at the ends of the nanorods such that copper sulfide (Cu2S) grows inwards from either end. The resulting morphology is very different from the striped pattern obtained in our previous studies of silver I (Ag+) exchange in CdS nanorods where non-selective nucleation of silver sulfide (Ag2S) occurs. From interface formation energies calculated for several models of epitaxialconnections between CdS and Cu2S or Ag2S, we infer the relative stability of each interface during the nucleation and growth of Cu2S or Ag2S within the CdS nanorods. The epitaxial connections of Cu2S to the end facets of CdS nanorods minimize the formation energy, making these interfaces stable throughout the exchange reaction. However, as the two end facets of wurtzite CdS nanorods are crystallographically nonequivalent, asymmetric heterostructures can be produced.},
doi = {},
url = {https://www.osti.gov/biblio/962717}, journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 14,
volume = 131,
place = {United States},
year = {2008},
month = {12}
}