arXiv subjects

Jens Güdde

Publications and source records attributed to Jens Güdde.

6 recordsLinked to original sources

arXiv2026

Subcycle videography of lightwave-driven Landau-Zener-Majorana transitions in graphene

Strong light fields have unlocked previously unthinkable possibilities to tailor coherent electron trajectories, engineer band structures and shape emergent phases of matter all-optically. Unravelling the underlying quantum mechanisms requires a visualisation of the lightwave-driven electron motion directly in the band structure. While photoelectron momentum microscopy has imaged optically excited electrons averaged over many cycles of light, actual subcycle band-structure videography has been limited to small electron momenta. Yet lightwave-driven elementary processes in quantum materials often occur throughout momentum space. Here, we introduce attosecond-precision, subcycle band-structure videography covering the entire first Brillouin zone (BZ) and visualize one of the most fundamental but notoriously elusive strong-field processes: non-adiabatic Landau-Zener-Majorana (LZM) tunnelling. The interplay of field-driven acceleration within the Dirac-like band structure of graphene and periodic LZM interband tunnelling manifest in a coherent displacement and distortion of the momentum distribution at the BZ edge. The extremely non-thermal electron distributions also allow us to disentangle competing scattering processes and assess their impact on coherent electronic control through electron redistribution and thermalization. Our panoramic view of strong-field-driven electron motion in quantum materials lays the foundation for a microscopic understanding of some of the most discussed light-driven phenomena in condensed matter physics.

cond-mat.mes-hall↗

arXiv2021

Momentum-resolved observation of exciton formation dynamics in monolayer WS$_2$

The dynamics of exciton formation in transition metal dichalcogenides is difficult to measure experimentally, since many momentum-indirect exciton states are not accessible to optical interband spectroscopy. Here, we combine a tuneable pump, high-harmonic probe laser source with a 3D momentum imaging technique to map photoemitted electrons from monolayer WS$_2$. This provides momentum-, energy- and time-resolved access to excited states on an ultrafast timescale. The high temporal resolution of the setup allows us to trace the early-stage exciton dynamics on its intrinsic timescale and observe the formation of a momentum-forbidden dark K$Σ$ 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 WS$_2$.

cond-mat.mtrl-sci↗

arXiv2020

Ultrafast dynamics of photocurrents in surface states of 3D topological insulators

This article reviews experimental work on the ultrafast electron dynamics in the topological surface state (TSS) of three-dimensional (3D) topological insulators (TIs) observed with time- and angle-resolved two-photon photoemission (2PPE). The focus is laid on the generation of ultrafast photocurrents and the time-resolved observation of their decay. 2PPE not only allow to unambiguously relate the photocurrents to the spin-polarized electronic surface states. Probing of the asymmetric momentum distribution of the electrons carrying the current makes it possible to study the microscopic scattering processes that governs the unusual electron transport in the time domain. Ultrashort mid-infrared pump pulses permit not only a direct optical excitation of the TSS in Sb$_2$Te$_3$ but also lead to a strong asymmetry of the TSS population in momentum space. Two-dimensional band mapping of the TSS shows that this asymmetry is in fact representative for a macroscopic photocurrent while the helicity-dependence of the photocurrent is found to be small. The time-resolved observation of the photocurrent decay reveals a huge mean free path of the electrons in the TSS.

cond-mat.mes-hall↗

arXiv2020

Tracing orbital images on ultrafast time scales

Frontier orbitals, i.e., the highest occupied and lowest unoccupied orbitals of a molecule, generally determine molecular properties, such as chemical bonding and reactivities. Consequently, there has been a lot of interest in measuring them, despite the fact that, strictly speaking, they are not quantum-mechanical observables. Yet, with photoemission tomography a powerful technique has recently been introduced by which the electron distribution in orbitals of molecules adsorbed at surfaces can be imaged in momentum space. This has even been used for the identification of reaction intermediates in surface reactions. However, so far it has been impossible to follow an orbital's momentum-space dynamics in time, for example through an excitation process or a chemical reaction. Here, we report a key step in this direction: we combine time-resolved photoemission employing high laser harmonics and a recently developed momentum microscope to establish a tomographic, femtosecond pump-probe experiment of unoccupied molecular orbitals. Specifically, we measure the full momentum-space distribution of transiently excited electrons. Because in molecules this momentum-space distribution is closely linked to orbital shapes, our experiment offers the extraordinary possibility to observe ultrafast electron motion in time and space. This enables us to connect their excited states dynamics to specific real-space excitation pathways.

physics.chem-ph↗

arXiv2016

Intervalley scattering in MoS$_2$ 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 MoS$_2$ 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 ($k_x, k_y, E$) electron spectrometer. We show that optical excitation slightly above the A exciton resonance results in an immediate occupation of the conduction band at $\overline{K}$ followed by an ultrafast transfer ($< 50$~fs) to the conduction band minimum at $\overlineΣ$. Both signals, at $\overline{K}$ and $\overlineΣ$, 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.

cond-mat.mes-hall↗

arXiv2016

Spectroscopy and Dynamics of a Two-Dimensional Electron Gas on top of 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 (2PPE) at very low temperatures under ultra-high 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 two 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 one monolayer of helium increases its lifetime by one order of magnitude compared to the bare Cu(111) surface.

cond-mat.mes-hall↗