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

Chanaka Kumara; M. Mozammel Hoque; Xiaobing Zuo; David A. Cullen; Robert L. Whetten; Amala Dass

doi:10.1021/acs.jpclett.8b02993

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

Chanaka Kumara, M. Mozammel Hoque, Xiaobing Zuo, David A. Cullen, Robert L. Whetten, Amala Dass

Materials MicroAnalysis

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

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.

Original language	English
Pages (from-to)	6825-6832
Number of pages	8
Journal	Journal of Physical Chemistry Letters
Volume	9
Issue number	23
DOIs	https://doi.org/10.1021/acs.jpclett.8b02993
State	Published - Dec 6 2018

Funding

C.K. and A.D. gratefully acknowledge support from NSF CHE-1255519 and NSF 1808138. We thank Karena Chapman for collecting PDF data at APS. Small-angle X-ray scattering data were collected at Beamline 12-ID-B of APS at Argonne National Laboratory. Work performed at Argonne and the use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract No. DEAC02-06CH11357. Electron microscopy research was supported through a user project supported by ORNL’s Center for Nanophase Materials Sciences (CNMS), which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. R.L.W. acknowledges support from the Welch Foundation AX-1857.

Funders	Funder number
CNMS
ORNL’s Center for Nanophase Materials Sciences
Office of Basic Energy Sciences
Scientific User Facilities Division
U.S. DOE
National Science Foundation	1808138, CHE-1255519
U.S. Department of Energy
Welch Foundation	AX-1857
Office of Science
Argonne National Laboratory

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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.",

author = "Chanaka Kumara and Hoque, {M. Mozammel} and Xiaobing Zuo and Cullen, {David A.} and Whetten, {Robert L.} and Amala Dass",

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AU - Cullen, David A.

AU - Whetten, Robert L.

AU - Dass, Amala

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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

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