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Ultra-fast dynamics of electron thermalization, cooling and transport effects in Ru(001)

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Abstract

Time-resolved two-photon photoelectron spectroscopy is used to study the dynamics of non-equilibrium electron and hole distributions at bare and D2O-covered Ru(001) following optical excitation (55-fs, 800-nm pulses) with variable fluence (0.04–0.6 mJ cm-2). Within the first 0.5 ps we observe an ultra-fast transient of the excited-carrier population and energy density at the surface which is accompanied by pronounced deviations of the electron-energy distribution from a (thermalized) Fermi–Dirac distribution. Comparison of the transient energy density of the photoexcited electrons at the surface with predictions of the two-temperature model provides fair agreement up to 400 fs, but exhibits a systematically lower energy density at later times, where electrons and phonons are equilibrated. We propose that this reduced energy density at the surface originates from ultra-fast energy transport of non-thermal electrons into the bulk in competition to electron–phonon coupling at the surface. This is corroborated by extending the two-temperature model to account for non-thermal, photoexcited electrons, whereby quantitative agreement with experiment can only be achieved if ballistic transport and reduced electron–phonon coupling is incorporated for non-thermal electrons. Implications for surface femtochemistry are discussed.

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Authors and Affiliations

  1. Fachbereich Physik, Freie Universität Berlin, Arnimallee 14, 14195, Berlin, Germany

    M. Lisowski, P.A. Loukakos, U. Bovensiepen, J. Stähler, C. Gahl & M. Wolf

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  1. M. Lisowski
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  2. P.A. Loukakos
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  3. U. Bovensiepen
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  4. J. Stähler
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  5. C. Gahl
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  6. M. Wolf
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Correspondence to M. Lisowski.

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PACS

78.47.+p; 71.38.-k; 73.40.-c

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Lisowski, M., Loukakos, P., Bovensiepen, U. et al. Ultra-fast dynamics of electron thermalization, cooling and transport effects in Ru(001). Appl Phys A 78, 165–176 (2004). https://doi.org/10.1007/s00339-003-2301-7

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  • DOI: https://doi.org/10.1007/s00339-003-2301-7

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