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Title: Sharp Transition from Nonmetallic Au 246 to Metallic Au 279 with Nascent Surface Plasmon Resonance

Abstract

Here, the optical properties of metal nanoparticles have attracted wide interest. Recent progress in controlling nanoparticles with atomic precision (often called nanoclusters) provide new opportunities for investigating many fundamental questions, such as the transition from excitonic to plasmonic state, which is a central question in metal nanoparticle research because it provides insights into the origin of surface plasmon resonance (SPR) as well as the formation of metallic bond. However, this question still remains elusive because of the extreme difficulty in preparing atomically precise nanoparticles larger than 2 nm. Here we report the synthesis and optical properties of an atomically precise Au 279(SR) 84 nanocluster. Femtosecond transient absorption spectroscopic analysis reveals that the Au 279 nanocluster shows a laser power dependence in its excited state lifetime, indicating metallic state of the particle, in contrast with the nonmetallic electronic structure of the Au 246(SR) 80 nanocluster. Steady-state absorption spectra reveal that the nascent plasmon band of Au 279 at 506 nm shows no peak shift even down to 60 K, consistent with plasmon behavior. The sharp transition from nonmetallic Au 246 to metallic Au 279 is surprising and will stimulate future theoretical work on the transition and many other relevant issues.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [2]; ORCiD logo [3]; ORCiD logo [1]
  1. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  2. Univ. of Toledo, Toledo, OH (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1460828
Report Number(s):
BNL-207860-2018-JAAM
Journal ID: ISSN 0002-7863
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 17; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Higaki, Tatsuya, Zhou, Meng, Lambright, Kelly J., Kirschbaum, Kristin, Sfeir, Matthew Y., and Jin, Rongchao. Sharp Transition from Nonmetallic Au246 to Metallic Au279 with Nascent Surface Plasmon Resonance. United States: N. p., 2018. Web. doi:10.1021/jacs.8b02487.
Higaki, Tatsuya, Zhou, Meng, Lambright, Kelly J., Kirschbaum, Kristin, Sfeir, Matthew Y., & Jin, Rongchao. Sharp Transition from Nonmetallic Au246 to Metallic Au279 with Nascent Surface Plasmon Resonance. United States. doi:10.1021/jacs.8b02487.
Higaki, Tatsuya, Zhou, Meng, Lambright, Kelly J., Kirschbaum, Kristin, Sfeir, Matthew Y., and Jin, Rongchao. Mon . "Sharp Transition from Nonmetallic Au246 to Metallic Au279 with Nascent Surface Plasmon Resonance". United States. doi:10.1021/jacs.8b02487. https://www.osti.gov/servlets/purl/1460828.
@article{osti_1460828,
title = {Sharp Transition from Nonmetallic Au246 to Metallic Au279 with Nascent Surface Plasmon Resonance},
author = {Higaki, Tatsuya and Zhou, Meng and Lambright, Kelly J. and Kirschbaum, Kristin and Sfeir, Matthew Y. and Jin, Rongchao},
abstractNote = {Here, the optical properties of metal nanoparticles have attracted wide interest. Recent progress in controlling nanoparticles with atomic precision (often called nanoclusters) provide new opportunities for investigating many fundamental questions, such as the transition from excitonic to plasmonic state, which is a central question in metal nanoparticle research because it provides insights into the origin of surface plasmon resonance (SPR) as well as the formation of metallic bond. However, this question still remains elusive because of the extreme difficulty in preparing atomically precise nanoparticles larger than 2 nm. Here we report the synthesis and optical properties of an atomically precise Au279(SR)84 nanocluster. Femtosecond transient absorption spectroscopic analysis reveals that the Au279 nanocluster shows a laser power dependence in its excited state lifetime, indicating metallic state of the particle, in contrast with the nonmetallic electronic structure of the Au246(SR)80 nanocluster. Steady-state absorption spectra reveal that the nascent plasmon band of Au279 at 506 nm shows no peak shift even down to 60 K, consistent with plasmon behavior. The sharp transition from nonmetallic Au246 to metallic Au279 is surprising and will stimulate future theoretical work on the transition and many other relevant issues.},
doi = {10.1021/jacs.8b02487},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 17,
volume = 140,
place = {United States},
year = {2018},
month = {4}
}

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Cited by: 15 works
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Works referencing / citing this record:

CSD 1838933: Experimental Crystal Structure Determination: Non-CSD Structure
dataset, April 2018