Nanomaterials (May 2022)

Influence of Electronic Non-Equilibrium on Energy Distribution and Dissipation in Aluminum Studied with an Extended Two-Temperature Model

  • Markus Uehlein,
  • Sebastian T. Weber,
  • Baerbel Rethfeld

DOI
https://doi.org/10.3390/nano12101655
Journal volume & issue
Vol. 12, no. 10
p. 1655

Abstract

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When an ultrashort laser pulse excites a metal surface, only a few of all the free electrons absorb a photon. The resulting non-equilibrium electron energy distribution thermalizes quickly to a hot Fermi distribution. The further energy dissipation is usually described in the framework of a two-temperature model, considering the phonons of the crystal lattice as a second subsystem. Here, we present an extension of the two-temperature model including the non-equilibrium electrons as a third subsystem. The model was proposed initially by E. Carpene and later improved by G.D. Tsibidis. We introduce further refinements, in particular, a temperature-dependent electron–electron thermalization time and an extended energy interval for the excitation function. We show results comparing the transient energy densities as well as the energy-transfer rates of the original equilibrium two-temperature description and the improved extended two-temperature model, respectively. Looking at the energy distribution of all electrons, we find good agreement in the non-equilibrium distribution of the extended two-temperature model with results from a kinetic description solving full Boltzmann collision integrals. The model provides a convenient tool to trace non-equilibrium electrons at small computational effort. As an example, we determine the dynamics of high-energy electrons observable in photo-electron spectroscopy. The comparison of the calculated spectral densities with experimental results demonstrates the necessity of considering electronic non-equilibrium distributions and electron–electron thermalization processes in time- and energy-resolved analyses.

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