arXiv subjects

Lukas Wittenbecher

Publications and source records attributed to Lukas Wittenbecher.

3 recordsLinked to original sources

arXiv2024

Sub-100-fs formation of dark excitons in monolayer WS2

Two-dimensional semiconducting transition metal dichalcogenides (TMDs) are promising for optoelectronic applications due to their strongly bound excitons. While bright excitons have been thoroughly scrutinized, dark excitons are much less investigated as they are not observable with far-field spectroscopy. However, with their non-zero momenta, dark excitons are significant for applications requiring long-range transport or coupling to external fields. We access such dark excitons in WS2 monolayer using transient photoemission electron microscopy with sub-diffraction limited spatial resolution (75 nm) and exceptionally high temporal resolution (13 fs). Image time series of TMD flakes are recorded at several different fluences. We directly observe the ultrafast formation of dark K-Q excitons in monolayer WS2 occurring within 14-50 fs and follow their subsequent picosecond decay. We distinguish exciton dynamics between the interior and edges of the monolayer TMD and conclude that the long-term evolution of dark excitations is defect-mediated while intervalley scattering is not affected.

cond-mat.mes-hall↗

arXiv2023

Time-resolved photoemission electron microscopy on a ZnO surface using an extreme ultraviolet attosecond pulse pair

Electrons photoemitted by extreme ultraviolet attosecond pulses derive spatially from the first few atomic surface layers and energetically from the valence band and highest atomic orbitals. As a result, it is possible to probe the emission dynamics from a narrow two-dimensional region in the presence of optical fields as well as obtain elemental specific information. However, combining this with spatially-resolved imaging is a long-standing challenge because of the large inherent spectral width of attosecond pulses as well as the difficulty of making them at high repetition rates. Here we demonstrate an attosecond interferometry experiment on a zinc oxide (ZnO) surface using spatially and energetically resolved photoelectrons. We combine photoemission electron microscopy with near-infrared pump - extreme ultraviolet probe laser spectroscopy and resolve the instantaneous phase of an infrared field with high spatial resolution. Our results show how the core level states with low binding energy of ZnO are well suited to perform spatially resolved attosecond interferometry experiments. We observe a distinct phase shift of the attosecond beat signal across the laser focus which we attribute to wavefront differences between the pump and the probe fields at the surface. Our work demonstrates a clear pathway for attosecond interferometry with high spatial resolution at atomic scale surface regions opening up for a detailed understanding of nanometric light-matter interaction.

physics.optics↗

arXiv2021

Understanding Radiative Transitions and Relaxation Pathways in Plexcitons

Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of cavity quantum electrodynamics. They are highly tunable, scalable, easy to synthesize and offer sub-wavelength confinement, all while giving access to the ultrastrong light-matter coupling regime at room temperature and promising a plethora of applications. However, the complexity of both the molecular aggregate and plasmonic nanoparticle introduces many more processes affecting the excitation and its relaxation, than are present in atom-cavity systems. Here, we follow the complex relaxation pathways of the photoexcitation of such hybrid systems and conclude that while the metal is responsible for destroying the coherence of the excitation, the molecular aggregate significantly participates in dissipating the energy. We rely on two-dimensional electronic spectroscopy in a combined theory-experiment approach, which allows us to ascribe the different timescales of relaxation to processes inside the molecules or the metal nanoparticle. We show that the dynamics beyond a few femtoseconds has to be cast in the language of hot electron distributions and excitons instead of the accepted lower and upper polariton branches, and furthermore set the framework for delving deeper into the photophysics of excitations that could be used in hot electron transfer, for example to drive photocatalytic reactions.

physics.chem-ph↗