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Title: Ultrafast Relaxation Dynamics of [Au25(SR)18]q Nanoclusters: Effects of Charge State

Journal Article · · Journal of Physical Chemistry C
DOI:https://doi.org/10.1021/jp107915x· OSTI ID:1000916

The ultrafast electron relaxation dynamics of anionic and neutral Au{sub 25}(SR){sub 18} nanoclusters are investigated using broad-band time-resolved optical spectroscopy. From an analysis of the wavelength-dependent transient absorption kinetics, we have obtained valuable information on the spectral features that originate from excitation of 'core' and 'core-shell' states. In both clusters, photoexcitation occurs into two nondegenerate states near the HOMO-LUMO gap that are derived from the core orbitals. A large difference in the lifetime of the core excitations is observed, with [Au{sub 25}(SR){sub 18}]{sup -} exhibiting a decay rate more than 1000 times slower than the neutral cluster. Both clusters show strong coupling to two different coherent phonon modes, which are observed at 2.4 and 1.2 THz. The electron-phonon coupling is analyzed in terms of the spectral distribution and damping of the coherent modes.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Sponsoring Organization:
DOE - Office Of Science
DOE Contract Number:
DE-AC02-98CH10886
OSTI ID:
1000916
Report Number(s):
BNL-93921-2010-JA; ISSN 1932-7455; KC0202020; TRN: US1100241
Journal Information:
Journal of Physical Chemistry C, Vol. 114, Issue 47; ISSN 1932-7447
Country of Publication:
United States
Language:
English