Abstract
We present first-principles calculations of electron-electron scattering rates of low-energy electrons in Au. Our full band-structure calculations indicate that a major contribution from occupied $d$ states participating in the screening of electron-electron interactions yields lifetimes of electrons in Au with energies of $1.0--3.0 \mathrm{eV}$ above the Fermi level that are larger than those of electrons in a free-electron gas by a factor of $\ensuremath{\sim}4.5.$ This prediction is in agreement with a recent experimental study of ultrafast electron dynamics in Au(111) films [J. Cao et al., Phys. Rev. B 58, 10 948 (1998)], where electron transport has been shown to play a minor role in the measured lifetimes of hot electrons in this material.
Highlights
We present first-principles calculations of electron-electron scattering rates of low-energy electrons in Au
When these so-called hot electrons are generated by absorption of an optical pulse, as occurs in the case of time-resolved two-photon photoemissionTR-2PPEtechniques,[3,4] electron transport provides an additional decay component to the photoexcited electron population
Since inelastic lifetimes of hot electrons become infinitely long as they approach the Fermi level, e-p scattering and the scattering by defects both play a key role in the relaxation process of electrons very near the Fermi level
Summary
Recent TR-2PPE experiments in Au111͒ films with thicknesses ranging from 150 to 3000 Å have shown the relaxation from electron transport to be negligible and the hot-electron lifetime to be solely determined, at energies larger than ϳ0.5Ϫ1.0 eV above the Fermi level, by e-e inelastic scattering processes.[15] these measurements provide an excellent benchmark against which to investigate the importance of band-structure and many-body effects on electron dynamics in solids. We report first-principles calculations of the energy-dependent inelastic lifetime of hot electrons in Au. We follow the many-body scheme first developed by Quinn and Ferrell[17] and by Ritchie,[18] but we include the full band structure of the solid. The imaginary part of ⑀G,G(q,) represents a measure of the number of states available for the creation of an electron-hole pair involving a given momen-
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