Jens Güdde

Time-Resolved Investigation of Coherently Controlled Electric Currents at a Metal Surface

Studies of current dynamics in solids have been hindered by insufficiently brief trigger signals and electronic detection speeds. By combining a coherent control scheme with photoelectron spectroscopy, we generated and detected lateral electron currents at a metal surface on a femtosecond time scale with a contact-free experimental setup. We used coherent optical excitation at the light frequencies ωa and ωa/2 to induce the current, whose direction was controlled by the relative phase between the phase-locked laser excitation pulses. Time- and angle-resolved photoelectron spectroscopy afforded a direct image of the momentum distribution of the excited electrons as a function of time. For the first (n = 1) image-potential state of Cu(100), we found a decay time of 10 femtoseconds, attributable to electron scattering with steps and surface defects.

Generation of Transient Photocurrents in the Topological Surface State of Sb_{2}Te_{3} by Direct Optical Excitation with Midinfrared Pulses.

We combine tunable midinfrared (mid-IR) pump pulses with time- and angle-resolved two-photon photoemission to study ultrafast photoexcitation of the topological surface state (TSS) of Sb_{2}Te_{3}. It is revealed that mid-IR pulses permit a direct excitation from the occupied to the unoccupied part of the TSS across the Dirac point. The novel optical coupling induces asymmetric transient populations of the TSS at ±k_{∥}, which reflects a macroscopic photoexcited electric surface current. By observing the decay of the asymmetric population, we directly investigate the dynamics of the long-lived photocurrent in the time domain. Our discovery promises important advantages of photoexcitation by mid-IR pulses for spintronic applications.

Intervalley scattering in MoS2 imaged by two-photon photoemission with a high-harmonic probe

We report on the direct mapping of electron transfer in the momentum space of bulk MoS2 by means of time- and angle-resolved two-photon photoemission with a high-harmonic probe. For this purpose, we have combined a high-repetition rate high-harmonic source with tunable femtosecond pump pulses and a 3D ( kx,ky,E) electron spectrometer. We show that optical excitation slightly above the A exciton resonance results in an immediate occupation of the conduction band at K¯ followed by an ultrafast transfer ( <50 fs) to the conduction band minimum at Σ¯. Both signals, at K¯ and Σ¯, do not vanish over the observed period of 400 fs. The technique described here enables direct access to the charge transfer dynamics in k-space and allows the study of decay times and decay channels in various systems with dependence on the excess energy or helicity of the excitation.

Model potential for the description of metal/organic interface states

We present an analytical one-dimensional model potential for the description of electronic interface states that form at the interface between a metal surface and flat-lying adlayers of π-conjugated organic molecules. The model utilizes graphene as a universal representation of these organic adlayers. It predicts the energy position of the interface state as well as the overlap of its wave function with the bulk metal without free fitting parameters. We show that the energy of the interface state depends systematically on the bond distance between the carbon backbone of the adayers and the metal. The general applicability and robustness of the model is demonstrated by a comparison of the calculated energies with numerous experimental results for a number of flat-lying organic molecules on different closed-packed metal surfaces that cover a large range of bond distances.

Spectroscopy and Dynamics of a Two-Dimensional Electron Gas on Ultrathin Helium Films on Cu(111).

Electrons in image-potential states on the surface of bulk helium represent a unique model system of a two-dimensional electron gas. Here, we investigate their properties in the extreme case of reduced film thickness: a monolayer of helium physisorbed on a single-crystalline (111)-oriented Cu surface. For this purpose we have utilized a customized setup for time-resolved two-photon photoemission at very low temperatures under ultrahigh vacuum conditions. We demonstrate that the highly polarizable metal substrate increases the binding energy of the first (n=1) image-potential state by more than 2 orders of magnitude as compared to the surface of liquid helium. An electron in this state is still strongly decoupled from the metal surface due to the large negative electron affinity of helium and we find that even 1 monolayer of helium increases its lifetime by 1 order of magnitude compared to the bare Cu(111) surface.

Ultrafast coherent control of electric currents at metal surfaces

We report the development of an experimental technique to measure the dynamics of electrical currents on the femtosecond timescale. The technique combines methods of coherent control with time- and angle-resolved photoelectron spectroscopy. Direct snapshots of the momentum distribution of the excited electrons as function of time are then determined by photoelectron spectroscopy. In this way we gain information on the generation and decay of ultrashort current pulses in unprecedented detail. In particular, this technique allows the observation of elastic electron scattering in terms of an incoherent population dynamics in momentum space. We have applied this optical current generation and detection scheme to electrons in so-called image-potential states which represent a prototype of two-dimensional electronic surface states. Electrons in these states are bound perpendicular to the metal surface by the Coulombic image potential whereas they can move almost freely parallel to the surface. For the (n=1) image-potential state of Cu(100) we find a decay time of 10 fs due to electron scattering with steps and surface defects.

Generation and Time-Resolved Detection of Coherently Controlled Electric Currents at Surfaces

We demonstrate an experimental technique for the generation and detection of electron currents at surfaces on a femtosecond time scale with a contact-free experimental setup based on a combination of coherent control and photoemission spectroscopy.