Quantum memory effects on the dynamics of electrons in small gold clusters

Abstract

Electron dynamics in metallic clusters are examined using a time-dependent density functional theory that includes a 'memory term', i.e. attempts to describe temporal non-local correlations. Using the Iwamoto, Gross and Kohn exchange-correlation (XC) kernel we construct a translationally invariant memory action from which an XC potential is derived that is translationally covariant and exerts zero net force on the electrons. An efficient and stable numerical method to solve the resulting Kohn-Sham equations is presented. Using this framework, we study memory effects on electron dynamics in spherical Jellium 'gold clusters'. We find memory significantly broadens the surface plasmon absorption line, yet considerably less than measured in real gold clusters, attributed to the inadequacy of the Jellium model. Two-dimensional pump-probe spectroscopy is used to study the temporal decay profile of the plasmon, finding a fast decay followed by slower tail. Finally, we examine memory effects on high harmonic generation, finding memory narrows emission lines.

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Cited by in corpus (11)

• A well-tempered density functional theory of electrons in molecules
• Charge-Transfer in Time-Dependent Density Functional Theory
• A brief compendium of time-dependent density-functional theory
• Non-Adiabatic Approximations in Time-Dependent Density Functional Theory: Progress and Prospects
• Exploring non-adiabatic approximations to the exchange-correlation functional of TDDFT
• Adapting approximate memory potentials for time-dependent density functional theory
• Exchange-Correlation Asymptotics and High Harmonic Spectra
• Effects of inner electrons on atomic strong-field ionization dynamics
• Friction of the surface plasmon by high-energy particle-hole pairs: Are memory effects important?
• Pole placement design for quantum systems via coherent observers
• Nonadiabatic time-dependent density-functional theory at the cost of adiabatic local density approximation