SurfaceScience21 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 67: Poster Session V: Ultrafast electron dynamics at surface and interfaces I

O 67.5: Poster

Mittwoch, 3. März 2021, 10:30–12:30, P

Pump-probe second harmonic spectroscopy of molecule/metal interfaces — Jinghao Chen, Ping Zhou, Uwe Bovensiepen, and •Andrea Eschenlohr — Faculty of Physics, University Duisburg-Essen, Lotharstr. 1, 47057 Duisburg, Germany

Achieving a microscopic understanding of charge transfer dynamics and the relaxation of optically excited electrons and holes at molecule/metal interfaces requires an interface-sensitive analysis on the respective femtosecond timescales. Second harmonic spectroscopy (SHS) [1] is such an interface-sensitive probe in centrosymmetric materials. We employ a non-collinear optical parametric amplifier in the visible wavelength range (1.9-2.5 eV) for pump-probe SHS with <20 fs pulse duration. A prototypical molecule/metal interface is prepared by adsorption of iron octaethylporphyrin (FeOEP) molecules on Cu(001) [2] and analyzed in situ in ultrahigh vacuum. We find a molecule-induced resonance at about 2.2 eV fundamental photon energy in the second harmonic spectrum of one monolayer of FeOEP/Cu(001). At this resonance, we observe a markedly slower relaxation time of the pump-induced changes in SHS compared to the bare Cu(001) surface, which indicates an increased lifetime of the electronic molecular state.

We thank H. Wende, J. Güdde and E. Riedle for valuable experimental advice, and the German Research Foundation for funding via SPP 1840 QUTIF and Sfb 1242.

[1] T. F. Heinz, C. K. Chen, D. Ricard, and Y. R. Shen, Phys. Rev. Lett. 48, 478 (1982); U. Höfer, Appl. Phys. A 63, 533 (1996).

[2] H. C. Herper et al., Phys. Rev. B 87, 174424 (2013).