Composition-dependent electronic energy relaxation dynamics of metal domains as revealed by bimetallic Au144−xAgx(SC8H9)60 monolayer-protected clusters

文献情報

出版日 2017-05-03

DOI 10.1039/C7CP00884H

インパクトファクター 3.676

著者

Hongjun Zheng, Marcus A. Tofanelli, Christopher J. Ackerson

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要旨

We examined the electronic relaxation dynamics for mono and bimetallic Au144−xAgx(SC8H9)60 monolayer-protected clusters (MPCs) using femtosecond time-resolved transient extinction spectroscopy. MPCs provide compositionally well-defined model systems for structure-specific determination of nanoscale electronic properties. Based on pulse-energy-dependent transient extinction data, we quantified electron–phonon coupling constants for three distinct Au144−xAgx(SC8H9)60 MPC samples, where x = 0, 0 < x < 30, and x ∼ 30, as Gx=0 = (1.61 ± 0.1) × 1016 W m−3 K−1, Gx<30 = (1.74 ± 0.1) × 1016 W m−3 K−1 and Gx∼30 = (2.07 ± 0.15) × 1016 W m−3 K−1, respectively. These results reflect a trend of greater electron–phonon coupling efficiency with increasing silver content. Based on these data, we conclude that gold-atom replacement by silver occurs at surface sites of the 114-atom metal core of the MPC. Definitive determinations of functional response to nanoscale “alloy” formation and dopant inclusion are critical to establishing predictive models for the development of materials that feature nanoparticles as active components.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

Composition-dependent electronic energy relaxation dynamics of metal domains as revealed by bimetallic Au144−xAgx(SC8H9)60 monolayer-protected clusters

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