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Strong Influence of Ti Adhesion Layer on Electron-Phonon Relaxation in Thin Gold Films: Ab Initio Nonadiabatic Molecular Dynamics.
ACS Applied Materials & Interfaces 2017 December 14
Electron-phonon relaxation in thin metal films is an important consideration for many ultrasmall devices and ultrafast applications. Recent time-resolved experiments demonstrate a significant, more than a factor of five, increase in the electron-phonon coupling and acceleration in the electron-phonon relaxation rate when a narrow Ti adhesion layer is introduced between an Au film and a nonmetal substrate. Using nonadiabatic molecular dynamics combined with real-time time-dependent density functional theory, we identify the reasons that give rise to this strong effect. First, the Ti layer greatly enhances the density of states (DOS) in the energy region starting at 1 eV below the Fermi level and extending several electronvolts above it. Second, Ti atoms are four times lighter than Au atoms and therefore generate larger nonadiabatic (NA) electron-phonon coupling. Because the transition rates depend on coupling and DOS, both the factors accelerate the dynamics. Showing good agreement with the experiments, the time-domain atomistic simulations provide a detailed mechanistic understanding of the electron-phonon relaxation dynamics in thin gold films and related nanomaterials.
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