Prof. Dr. Ulrich HöferPrincipal Investigator Universität RegensburgRegensburg Center for Ultrafast Nanoscopy (RUN)
K. Stallberg, A. Namgalies, S. Chatterjee, U. Höfer
In: J. Phys. Chem. C, vol. 126, pp. 12728–12734, 2022.
The functionality of organic electronic devices is governed by the dynamics of charge carriers and excited states in organic semiconductors. In particular, the relaxation of excitons and the transfer of charge carriers at metal electrodes crucially determine the performance of organic optoelectronic devices. In a combined experimental study we apply time-resolved photoluminescence and two-photon photoemission to reveal the ultrafast exciton dynamics and charge transfer at prototype organic/metal contacts comprising thin molecular films on single-crystalline noble-metal surfaces. On the basis of experiments with systematically varied film thicknesses, we relate the strong quenching of Frenkel excitons and charge-transfer excitons to the wave function overlap with the metal, indicating charge transfer as the dominant relaxation pathway. Moreover, the presence of an electronic interface state is found to facilitate the transfer of excited carriers across the organic/metal interface.
R. Wallauer, M. Raths, K. Stallberg, L. Münster, D. Brandstetter, X. Yang, J. Güdde, P. Puschnig, S. Soubatch, C. Kumpf, F. C. Bocquet, F. S. Tautz, U. Höfer
Tracing orbital images on ultrafast time scales Journal Article
In: Science, vol. 371, pp. 1056-1059, 2021.
Frontier orbitals determine fundamental molecular properties such as chemical reactivities. Although electron distributions of occupied orbitals can be imaged in momentum space by photoemission tomography, it has so far been impossible to follow the momentum-space dynamics of a molecular orbital in time, for example, through an excitation or a chemical reaction. Here, we combined time-resolved photoemission using high laser harmonics and a momentum microscope to establish a tomographic, femtosecond pump-probe experiment of unoccupied molecular orbitals. We measured the full momentum-space distribution of transiently excited electrons, connecting their excited-state dynamics to real-space excitation pathways. Because in molecules this distribution is closely linked to orbital shapes, our experiment may, in the future, offer the possibility of observing ultrafast electron motion in time and space.
R. Wallauer, R. Perea-Causin, L. Münster, S. Zajusch, S. Brem, J. Güdde, K. Tanimura, K. -Q. Lin, R. Huber, E. Malic, U. Höfer
In: Nano Lett., vol. 21, pp. 5867–5873, 2021.
The dynamics of momentum-dark exciton formation in transition metal dichalcogenides is difficult to measure experimentally, as many momentum-indirect exciton states are not accessible to optical interband spectroscopy. Here, we combine a tunable pump, high-harmonic probe laser source with a 3D momentum imaging technique to map photoemitted electrons from monolayer WS2. This provides momentum-, energy- and time-resolved access to excited states on an ultrafast time scale. The high temporal resolution of the setup allows us to trace the early-stage exciton dynamics on its intrinsic time scale and observe the formation of a momentum-forbidden dark KΣ exciton a few tens of femtoseconds after optical excitation. By tuning the excitation energy, we manipulate the temporal evolution of the coherent excitonic polarization and observe its influence on the dark exciton formation. The experimental results are in excellent agreement with a fully microscopic theory, resolving the temporal and spectral dynamics of bright and dark excitons in WS2.
J. Reimann, S. Schlauderer, C. P. Schmid, F. Langer, S. Baierl, K. A. Kokh, O. E. Tereshchenko, A. Kimura, C. Lange, J. Güdde, U. Höfer, R. Huber
In: Nature, vol. 562, pp. 396–400, 2018.
Harnessing the carrier wave of light as an alternating-current bias may enable electronics at optical clock rates1. Lightwave-driven currents have been assumed to be essential for high-harmonic generation in solids2–6, charge transport in nanostructures7,8, attosecond-streaking experiments9–16 and atomic-resolution ultrafast microscopy17,18. However, in conventional semiconductors and dielectrics, the finite effective mass and ultrafast scattering of electrons limit their ballistic excursion and velocity. The Dirac-like, quasi-relativistic band structure of topological insulators19–29 may allow these constraints to be lifted and may thus open a new era of lightwave electronics. To understand the associated, complex motion of electrons, comprehensive experimental access to carrier-wave-driven currents is crucial. Here we report angle-resolved photoemission spectroscopy with subcycle time resolution that enables us to observe directly how the carrier wave of a terahertz light pulse accelerates Dirac fermions in the band structure of the topological surface state of Bi2Te3. While terahertz streaking of photoemitted electrons traces the electromagnetic field at the surface, the acceleration of Dirac states leads to a strong redistribution of electrons in momentum space. The inertia-free surface currents are protected by spin–momentum locking and reach peak densities as large as two amps per centimetre, with ballistic mean free paths of several hundreds of nanometres, opening up a realistic parameter space for all-coherent lightwave-driven electronic devices. Furthermore, our subcycle-resolution analysis of the band structure may greatly improve our understanding of electron dynamics and strong-field interaction in solids.
N. Armbrust, F. Schiller, J. Güdde, U. Höfer
In: Sci. Rep., vol. 7, pp. 46561, 2017.
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.