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Title: Evolution from the plasmon to exciton state in ligand-protected atomically precise gold nanoparticles

Abstract

The evolution from the metallic (or plasmonic) to molecular state in metal nanoparticles constitutes a central question in nanoscience research because of its importance in revealing the origin of metallic bonding and offering fundamental insights into the birth of surface plasmon resonance. Previous research has not been able to probe the transition due to the unavailability of atomically precise nanoparticles in the 1–3 nm size regime. Herein, we investigate the transition by performing ultrafast spectroscopic studies on atomically precise thiolate-protected Au 25, Au 38, Au 144, Au 333, Au ~520 and Au ~940 nanoparticles. Our results clearly map out three distinct states: metallic (size larger than Au333, that is, larger than 2.3 nm), transition regime (between Au 333 and Au 144, that is, 2.3–1.7 nm) and non-metallic or excitonic state (smaller than Au 144, that is, smaller than 1.7 nm). As a result, the transition also impacts the catalytic properties as demonstrated in both carbon monoxide oxidation and electrocatalytic oxidation of alcohol.

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [1]
  1. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Anhui Univ., Anhui (China)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1347376
Report Number(s):
BNL-113660-2017-JA
Journal ID: ISSN 2041-1723; R&D Project: 16063/16058; KC0403020
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Center for Functional Nanomaterials; nanoparticles; ultrafast photonics

Citation Formats

Zhou, Meng, Zeng, Chenjie, Chen, Yuxiang, Zhao, Shuo, Sfeir, Matthew Y., Zhu, Manzhou, and Jin, Rongchao. Evolution from the plasmon to exciton state in ligand-protected atomically precise gold nanoparticles. United States: N. p., 2016. Web. doi:10.1038/ncomms13240.
Zhou, Meng, Zeng, Chenjie, Chen, Yuxiang, Zhao, Shuo, Sfeir, Matthew Y., Zhu, Manzhou, & Jin, Rongchao. Evolution from the plasmon to exciton state in ligand-protected atomically precise gold nanoparticles. United States. doi:10.1038/ncomms13240.
Zhou, Meng, Zeng, Chenjie, Chen, Yuxiang, Zhao, Shuo, Sfeir, Matthew Y., Zhu, Manzhou, and Jin, Rongchao. Mon . "Evolution from the plasmon to exciton state in ligand-protected atomically precise gold nanoparticles". United States. doi:10.1038/ncomms13240. https://www.osti.gov/servlets/purl/1347376.
@article{osti_1347376,
title = {Evolution from the plasmon to exciton state in ligand-protected atomically precise gold nanoparticles},
author = {Zhou, Meng and Zeng, Chenjie and Chen, Yuxiang and Zhao, Shuo and Sfeir, Matthew Y. and Zhu, Manzhou and Jin, Rongchao},
abstractNote = {The evolution from the metallic (or plasmonic) to molecular state in metal nanoparticles constitutes a central question in nanoscience research because of its importance in revealing the origin of metallic bonding and offering fundamental insights into the birth of surface plasmon resonance. Previous research has not been able to probe the transition due to the unavailability of atomically precise nanoparticles in the 1–3 nm size regime. Herein, we investigate the transition by performing ultrafast spectroscopic studies on atomically precise thiolate-protected Au25, Au38, Au144, Au333, Au~520 and Au~940 nanoparticles. Our results clearly map out three distinct states: metallic (size larger than Au333, that is, larger than 2.3 nm), transition regime (between Au333 and Au144, that is, 2.3–1.7 nm) and non-metallic or excitonic state (smaller than Au144, that is, smaller than 1.7 nm). As a result, the transition also impacts the catalytic properties as demonstrated in both carbon monoxide oxidation and electrocatalytic oxidation of alcohol.},
doi = {10.1038/ncomms13240},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {10}
}

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