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Title: Isolation of a 300 kDa, Au -1400 Gold Compound, the Standard 3.6 nm Capstone to a Series of Plasmonic Nanocrystals Protected by Aliphatic-like Thiolates

Abstract

Disclosed herein is a method to obtain the ~300 kDa gold–hexanethiolate compound, extracted from the Faradaurate series of smaller (3) and larger (1) homologues, thereby permitting the first measurement of its distinctive properties by methods including mass spectrometry, optical spectroscopy, electron microscopy, X-ray scattering, and diffraction. The results suggest a monocrystalline metallic core (free of twinning planes) of ~3.1 nm minimum dimension, which supports a clear plasmonic optical response, along with a diffuse exterior shell. An idealized model to account for this (and smaller) members of the series is proposed based on the completion of a convex core of regular truncated-octahedral (TO) morphology, that is, the TO (5,5) crystallite comprising 1289 sites. The diffuse layer may comprise the 240 S sites (thiolate sulfur headgroups) and 96 Au-adatom sites, giving a total composition (1385,240) and a molar mass of ~301.0 kDa (90.7% Au). The ~300 and ~400 kDa gold compounds contain Au ~1400 and Au ~2000 atoms, respectively.

Authors:
 [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Mississippi, Oxford, MS (United States)
  2. Univ. of Texas, San Antonio, TX (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Welch Foundation; National Science Foundation (NSF)
OSTI Identifier:
1490576
Alternate Identifier(s):
OSTI ID: 1504766
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 23; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kumara, Chanaka, Hoque, M. Mozammel, Zuo, Xiaobing, Cullen, David A., Whetten, Robert L., and Dass, Amala. Isolation of a 300 kDa, Au-1400 Gold Compound, the Standard 3.6 nm Capstone to a Series of Plasmonic Nanocrystals Protected by Aliphatic-like Thiolates. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b02993.
Kumara, Chanaka, Hoque, M. Mozammel, Zuo, Xiaobing, Cullen, David A., Whetten, Robert L., & Dass, Amala. Isolation of a 300 kDa, Au-1400 Gold Compound, the Standard 3.6 nm Capstone to a Series of Plasmonic Nanocrystals Protected by Aliphatic-like Thiolates. United States. doi:10.1021/acs.jpclett.8b02993.
Kumara, Chanaka, Hoque, M. Mozammel, Zuo, Xiaobing, Cullen, David A., Whetten, Robert L., and Dass, Amala. Tue . "Isolation of a 300 kDa, Au-1400 Gold Compound, the Standard 3.6 nm Capstone to a Series of Plasmonic Nanocrystals Protected by Aliphatic-like Thiolates". United States. doi:10.1021/acs.jpclett.8b02993.
@article{osti_1490576,
title = {Isolation of a 300 kDa, Au-1400 Gold Compound, the Standard 3.6 nm Capstone to a Series of Plasmonic Nanocrystals Protected by Aliphatic-like Thiolates},
author = {Kumara, Chanaka and Hoque, M. Mozammel and Zuo, Xiaobing and Cullen, David A. and Whetten, Robert L. and Dass, Amala},
abstractNote = {Disclosed herein is a method to obtain the ~300 kDa gold–hexanethiolate compound, extracted from the Faradaurate series of smaller (3) and larger (1) homologues, thereby permitting the first measurement of its distinctive properties by methods including mass spectrometry, optical spectroscopy, electron microscopy, X-ray scattering, and diffraction. The results suggest a monocrystalline metallic core (free of twinning planes) of ~3.1 nm minimum dimension, which supports a clear plasmonic optical response, along with a diffuse exterior shell. An idealized model to account for this (and smaller) members of the series is proposed based on the completion of a convex core of regular truncated-octahedral (TO) morphology, that is, the TO (5,5) crystallite comprising 1289 sites. The diffuse layer may comprise the 240 S sites (thiolate sulfur headgroups) and 96 Au-adatom sites, giving a total composition (1385,240) and a molar mass of ~301.0 kDa (90.7% Au). The ~300 and ~400 kDa gold compounds contain Au~1400 and Au~2000 atoms, respectively.},
doi = {10.1021/acs.jpclett.8b02993},
journal = {Journal of Physical Chemistry Letters},
issn = {1948-7185},
number = 23,
volume = 9,
place = {United States},
year = {2018},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on November 6, 2019
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