arXiv subjects

Nils Wind

Publications and source records attributed to Nils Wind.

5 recordsLinked to original sources

arXiv2023

New insights into the laser-assisted photoelectric effect from solid-state surfaces

Photoemission from a solid surface provides a wealth of information about the electronic structure of the surface and its dynamic evolution. Ultrafast pump-probe experiments are particularly useful to study the dynamic interactions of photons with surfaces as well as the ensuing electron dynamics induced by these interactions. Time-resolved laser-assisted photoemission (tr-LAPE) from surfaces is a novel technique to gain deeper understanding of the fundamentals underlying the photoemission process. Here, we present the results of a femtosecond time-resolved soft X-ray photoelectron spectroscopy experiment on two different metal surfaces conducted at the X-ray Free-Electron Laser FLASH in Hamburg. We study photoemission from the W 4f and Pt 4f core levels using ultrashort soft X-ray pulses in combination with synchronized infrared (IR) laser pulses. When both pulses overlap in time and space, laser-assisted photoemission results in the formation of a series of sidebands that reflect the dynamics of the laser-surface interaction. We demonstrate a qualitatively new level of sideband generation up to the sixth order and a surprising material dependence of the number of sidebands that has so far not been predicted by theory. We provide a semi-quantitative explanation of this phenomenon based on the different dynamic dielectric responses of the two materials. Our results advance the understanding of the LAPE process and reveal new details of the IR field present in the surface region, which is determined by the dynamic interplay between the IR laser field and the dielectric response of the metal surfaces.

cond-mat.mtrl-sci↗

arXiv2023

Real-time observation of phonon-electron energy and angular momentum flow in laser-heated nickel

Identifying the microscopic nature of non-equilibrium energy transfer mechanisms among electronic, spin and lattice degrees of freedom is central for understanding ultrafast phenomena such as manipulating magnetism on the femtosecond timescale. Here we use time and angle-resolved photoemission spectroscopy to go beyond the often-employed ensemble-averaged view of non-equilibrium dynamics in terms of quasiparticle temperature evolutions. We show for ferromagnetic Ni that the non-equilibrium electron and spin dynamics display pronounced variations with electron momentum whereas the magnetic exchange interaction remains isotropic. This highlights the influence of lattice-mediated scattering processes and opens a pathway towards unraveling the still elusive microscopic mechanism of spin-lattice angular momentum transfer.

cond-mat.mtrl-sci↗

arXiv2023

Femtosecond concerted rotation of molecules on a 2D material interface

Interfaces between molecules and 2D materials exhibit energy-driven functionalities, wherein charge transfer directs molecular motion. Unlike equilibrium systems, where molecular assemblies settle into static configurations, continuous energy input can drive transient, collective molecular rearrangements. Here, we reveal ultrafast spectroscopic fingerprints of a collective rotational response of molecules on a 2D material following photoexcitation. Our results suggest that photoinduced charge transfer reshapes the interfacial energy potential, giving rise to macroscopic, unidirectional molecular rotation and the formation of a homochiral molecular arrangement. Using a multiplexed ultrafast photoemission spectroscopy approach, we simultaneously track, electronic states, atomic positions, and orbital wavefunctions with femtosecond and sub-{\aa}ngstr\"om resolution. Multimodal valence and core electron emission analysis disentangles the intertwined electronic-structural dynamics of the molecule and the 2D material, revealing the dynamic modulation of charge distribution and intermolecular forces that drive collective molecular motion. Our findings open a pathway for designing energy-driven molecular systems with tunable interfacial dynamics, with potential applications in chiral engineering and active matter systems.

cond-mat.mtrl-sci↗

arXiv2022

Multispectral time-resolved energy-momentum microscopy using high-harmonic extreme ultraviolet radiation

A 790-nm-driven high-harmonic generation source with a repetition rate of 6 kHz is combined with a toroidal-grating monochromator and a high-detection-efficiency photoelectron time-of-flight momentum microscope to enable time- and momentum-resolved photoemission spectroscopy over a spectral range of $23.6$-$45.5$ eV with sub-100-fs time resolution. Three-dimensional (3D) Fermi surface mapping is demonstrated on graphene-covered Ir(111) with energy and momentum resolutions of $\lesssim$$100$ meV and $\lesssim$$0.1$ $\r{A}^{-1}$, respectively. The table-top experiment sets the stage for measuring the $k_z$-dependent ultrafast dynamics of 3D electronic structure, including band structure, Fermi surface, and carrier dynamics in 3D materials as well as 3D orbital dynamics in molecular layers.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast MHz-rate burst-mode pump-probe laser for the FLASH FEL facility based on nonlinear compression of ps-level pulses from an Yb-amplifier chain

The Free-Electron Laser (FEL) FLASH offers the worldwide still unique capability to study ultrafast processes with high-flux, high-repetition rate XUV and soft X-ray pulses. The vast majority of experiments at FLASH are of pump-probe type. Many of them rely on optical ultrafast lasers. Here, a novel FEL facility laser is reported which combines high average power output from Yb:YAG amplifiers with spectral broadening in a Herriott-type multi-pass cell and subsequent pulse compression to sub-100 fs durations. Compared to other facility lasers employing optical parametric amplification, the new system comes with significantly improved noise figures, compactness, simplicity and power efficiency. Like FLASH, the optical laser operates with 10 Hz burst repetition rate. The bursts consist of 800 $\mu$s long trains of up to 800 ultrashort pulses being synchronized to the FEL with femtosecond precision. In the experimental chamber, pulses with up to 50 $\mu$J energy, 60 fs FWHM duration and 1 MHz rate at 1.03 $\mu$m wavelength are available and can be adjusted by computer-control. Moreover, nonlinear polarization rotation is implemented to improve laser pulse contrast. First cross-correlation measurements with the FEL at the plane-grating monochromator photon beamline are demonstrated, exhibiting the suitability of the laser for user experiments at FLASH.

physics.optics↗