Ultrafast Relaxation Dynamics of [Au-25(SR)(18)](q) Nanoclusters: Effects of Charge State

作者:Qian Huifeng; Sfeir Matthew Y*; Jin Rongchao
来源:Journal of Physical Chemistry C, 2010, 114(47): 19935-19940.
DOI:10.1021/jp107915x

摘要

The ultrafast electron relaxation dynamics of anionic and neutral Au-25(SR)(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-25(SR)(18)](-) 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.

  • 出版日期2010-12-2