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Ab initio phonon‐coupled nonadiabatic relaxation dynamics of [Au 25 (SH) 18 ] − clusters
Author(s) -
Chen Xue,
Prezhdo Oleg V.,
Ma Zeyao,
Hou Tingjun,
Guo Zhenyu,
Li Youyong
Publication year - 2016
Publication title -
physica status solidi (b)
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.51
H-Index - 109
eISSN - 1521-3951
pISSN - 0370-1972
DOI - 10.1002/pssb.201552405
Subject(s) - nanoclusters , excited state , phonon , relaxation (psychology) , ab initio , homo/lumo , density functional theory , chemical physics , molecular physics , gold cluster , atomic physics , materials science , chemistry , physics , condensed matter physics , computational chemistry , nanotechnology , molecule , psychology , social psychology , organic chemistry
Nanoscale gold clusters exhibit unique electronic and optical properties. Here, we study the excited state dynamics and electron–phonon coupling of [Au 25 (SH) 18 ] – nanoclusters by using quantum‐classical molecular dynamics combined with time‐dependent density‐functional theory. Our result reproduces the experimental measurements and provides further insights into the relaxation dynamics of ligand protected gold clusters. We examine the ultrafast electronic dynamics induced by specific phonon modes. The roles of the Au 13 core and Au 12 ring in the optical process are investigated. We find that the LUMO–HOMO transition is dominated by AuAu stretching of the Au 13 core, whereas the LUMO + 1 − HOMO transition is induced by breathing vibrations of the Au core as well as AuS stretching. We clarify the interplay between electron–phonon couplings and specific energy‐transfer processes in [Au 25 (SH) 18 ] – nanoclusters.