Optical properties and electronic energy relaxation of metallic au 144(sr)60 nanoclusters

Chongyue Yi, Marcus A. Tofanelli, Christopher J. Ackerson, Kenneth L. Knappenberger

Research output: Contribution to journalArticle

63 Scopus citations

Abstract

Electronic energy relaxation of Au144(SR)60 q ligand-protected nanoclusters, where SR = SC6H 13 and q = -1, 0, +1, and +2, was examined using femtosecond time-resolved transient absorption spectroscopy. The observed differential transient spectra contained three distinct components: (1) transient bleaches at 525 and 600 nm, (2) broad visible excited-state absorption (ESA), and (3) stimulated emission (SE) at 670 nm. The bleach recovery kinetics depended upon the excitation pulse energy and were thus attributed to electron-phonon coupling typical of metallic nanostructures. The prominent bleach at 525 nm was assigned to a core-localized plasmon resonance (CLPR). ESA decay kinetics were oxidation-state dependent and could be described using a metal-sphere charging model. The dynamics, emission energy, and intensity of the SE peak exhibited dielectric-dependent responses indicative of Superatom charge transfer states. On the basis of these data, the Au144(SR)60 system is the smallest-known nanocluster to exhibit quantifiable electron dynamics and optical properties characteristic of metals.

Original languageEnglish (US)
Pages (from-to)18222-18228
Number of pages7
JournalJournal of the American Chemical Society
Volume135
Issue number48
DOIs
StatePublished - Dec 4 2013

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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