Au 130− x Ag x Nanoclusters with Non‐Metallicity: A Drum of Silver‐Rich Sites Enclosed in a Marks‐Decahedral Cage of Gold‐Rich Sites

Higaki, Tatsuya; Liu, Chong; Morris, David J.; He, Guiying; Luo, Tian‐Yi; Sfeir, Matthew Y.; Zhang, Peng; Rosi, Nathaniel L.; Jin, Rongchao

doi:10.1002/anie.201908694

Au _{130− x} Ag _x Nanoclusters with Non‐Metallicity: A Drum of Silver‐Rich Sites Enclosed in a Marks‐Decahedral Cage of Gold‐Rich Sites

Journal Article · Thu Nov 07 23:00:00 EST 2019 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201908694· OSTI ID:1573510

Higaki, Tatsuya ^[1]; Liu, Chong ^[2]; Morris, David J. ^[3]; He, Guiying ^[4]; Luo, Tian‐Yi ^[2]; Sfeir, Matthew Y. ^[5]; Zhang, Peng ^[3]; Rosi, Nathaniel L. ^[2]; ^[1]

Department of Chemistry Carnegie Mellon University Pittsburgh PA 15213 USA
Department of Chemistry University of Pittsburgh Pittsburgh PA 15260 USA
Department of Chemistry Dalhousie University Halifax Nova Scotia B3H 4R2 Canada
Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA
Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA, Present address: Department of Physics Graduate Center City University of New York New York NY 10016 USA, Photonics Initiative Advanced Science Research Center City University of New York New York NY 10031 USA

Abstract

The synthesis and structure of atomically precise Au _{130− x} Ag _x (average x= 98) alloy nanoclusters protected by 55 ligands of 4‐ tert ‐butylbenzenethiolate are reported. This large alloy structure has a decahedral M ₅₄ (M=Au/Ag) core. The Au atoms are localized in the truncated Marks decahedron. In the core, a drum of Ag‐rich sites is found, which is enclosed by a Marks decahedral cage of Au‐rich sites. The surface is exclusively Ag−SR; X‐ray absorption fine structure analysis supports the absence of Au−S bonds. The optical absorption spectrum shows a strong peak at 523 nm, seemingly a plasmon peak, but fs spectroscopic analysis indicates its non‐plasmon nature. The non‐metallicity of the Au _{130− x} Ag _x nanocluster has set up a benchmark to study the transition to metallic state in the size evolution of bimetallic nanoclusters. The localized Au/Ag binary architecture in such a large alloy nanocluster provides atomic‐level insights into the Au−Ag bonds in bimetallic nanoclusters.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0012704

OSTI ID:: 1573510

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 52 Vol. 58; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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