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

We examined the electronic relaxation dynamics for mono and bimetallic Au 144− x Ag x (SC 8 H 9 ) 60 monolayer-protected clusters (MPCs) using femtosecond time-resolved transient extinction spectroscopy. MPCs provide compositionally well-defined model systems for structure-specific determination of...

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Veröffentlicht in:Physical chemistry chemical physics : PCCP 2017-06, Vol.19 (22), p.14471-14477
Hauptverfasser: Zheng, Hongjun, Tofanelli, Marcus A, Ackerson, Christopher J, Knappenberger, Kenneth L
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creator Zheng, Hongjun
Tofanelli, Marcus A
Ackerson, Christopher J
Knappenberger, Kenneth L
description We examined the electronic relaxation dynamics for mono and bimetallic Au 144− x Ag x (SC 8 H 9 ) 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 Au 144− x Ag x (SC 8 H 9 ) 60 MPC samples, where x = 0, 0 < x < 30, and x ∼ 30, as G x =0 = (1.61 ± 0.1) × 10 16 W m −3 K −1 , G x
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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 Au 144− x Ag x (SC 8 H 9 ) 60 MPC samples, where x = 0, 0 &lt; x &lt; 30, and x ∼ 30, as G x =0 = (1.61 ± 0.1) × 10 16 W m −3 K −1 , G x &lt;30 = (1.74 ± 0.1) × 10 16 W m −3 K −1 and G x ∼30 = (2.07 ± 0.15) × 10 16 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. 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The influence of nanoscale composition on electronic relaxation is determined using monolayer-protected clusters as structurally precise model systems.</abstract><doi>10.1039/c7cp00884h</doi><tpages>7</tpages></addata></record>
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subjects Bimetals
Clusters
Coupling
Dynamics
Electronics
Extinction
Nanostructure
Silver
title Composition-dependent electronic energy relaxation dynamics of metal domains as revealed by bimetallic Au144−xAgx(SC8H9)60 monolayer-protected clusters
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