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

被引:203
作者
Lisowski, M [1 ]
Loukakos, PA [1 ]
Bovensiepen, U [1 ]
Stähler, J [1 ]
Gahl, C [1 ]
Wolf, M [1 ]
机构
[1] Free Univ Berlin, Fachbereich Phys, D-14195 Berlin, Germany
来源
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING | 2004年 / 78卷 / 02期
关键词
D O I
10.1007/s00339-003-2301-7
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
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.
引用
收藏
页码:165 / 176
页数:12
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