Photoabsorbance of supported metal clusters: ab initio density matrix and model studies of large Ag clusters on Si surfaces

Abstract

Metal clusters with 10 to 100 atoms supported by a solid surface show electronic structure typical of molecules and require ab initio treatments starting from their atomic structure, and they...

Energy-Conserving and Thermally Corrected Neglect of Back-Reaction Approximation Method for Nonadiabatic Molecular Dynamics

“…Nonadiabatic molecular dynamics (NA-MD) is a widely adopted family of computational methods to model quantum dynamics of excited states in various systems. − The NA-MD simulations have found their use in describing various kinds of processes in many molecular and condensed-matter systems: modeling nonradiative electron–hole recombination and “hot” carrier relaxation in quantum dots and molecular clusters, − nanotubes, , plasmonic systems, or exotic states of matter; modeling photoinduced isomerization and reactive processes in various molecular systems; − and modeling charge transfer and charge carrier trapping processes in 2D materials, − interfaces, ,− ,, organic solids, , and pristine and defect-containing bulk semiconductors. − …”

“…N onadiabatic molecular dynamics (NA-MD) is a widely adopted family of computational methods to model quantum dynamics of excited states in various systems. 1−5 The NA-MD simulations have found their use in describing various kinds of processes in many molecular and condensed-matter systems: modeling nonradiative electron−hole recombination and "hot" carrier relaxation in quantum dots and molecular clusters, 6−13 nanotubes, 14,15 plasmonic systems, 16 or exotic states of matter; 17 modeling photoinduced isomerization and reactive processes in various molecular systems; 18−22 and modeling charge transfer and charge carrier trapping processes in 2D materials, 23−31 interfaces, 25,[32][33][34][35][36]36,37 organic solids, 38,39 and pristine and defect-containing bulk semiconductors. 40−46 Computing the nonadiabatic dynamics in atomistic and solidstate systems has been made possible by adopting quantumclassical trajectory surface hopping (TSH) techniques, 4,47−51 among which Tully's fewest switches surface hopping (FSSH) 52 has been one of the most popular choices due to its simplicity to implement and clear physical picture.…”