arXiv subjects

Jan O. Schunck

Publications and source records attributed to Jan O. Schunck.

5 recordsLinked to original sources

arXiv2026

ToF-PAX-RIXS: A Time-of-Flight Spectrometer for combined ARPES and RIXS

We present ToF-PAX-RIXS, a compact instrument that combines time-of-flight momentum-microscopy angle-resolved photoemission spectroscopy (ARPES) with resonant inelastic X-ray scattering (RIXS). The latter is based on photoelectron spectrometry for analysis of X-rays (PAX). The two techniques are implemented with a single multimode electron-optical column, allowing measurements to be performed sequentially on the same sample under identical experimental conditions. In ARPES mode, the instrument records the photoemission intensity as a function of kinetic energy and two in-plane momentum components. In PAX-RIXS mode, scattered soft X-ray photons are absorbed in a thin metallic converter, and the generated photoelectrons are analyzed in energy and position of emission on the converter. The electron kinetic energy retains the spectral information of the scattered photons, while the position is related to the scattering angle and therefore to the momentum transfer, enabling simultaneous access to a finite momentum-transfer interval. We describe the mechanical design, converter assembly, scattering geometry, and multimode electron optics of the instrument. Its PAX-RIXS performance is benchmarked at the Cu $L_3$ edge using CaCuO$_2$, with Au, Ag, and Pt converters. The measured spectra reproduce the principal features obtained with a conventional grating RIXS spectrometer, and deconvolution yields an effective reconstructed energy resolution better than $120$~meV under the present conditions. Finally, combined ARPES and PAX-RIXS measurements on the same Ca-doped YBa$_2$Cu$_3$O$_{6.45}$ sample demonstrate the capability of the instrument to correlate electronic structure and collective excitations within a common compact platform.

cond-mat.str-el↗

arXiv2024

A compact approach to higher-resolution resonant inelastic X-ray scattering detection using photoelectrons

The detection of inelastically scattered soft X-rays with high energy resolution usually requires large grating spectrometers. Recently, photoelectron spectrometry for analysis of X-rays (PAX) has been rediscovered for modern spectroscopy experiments at synchrotron light sources. By converting scattered photons to electrons and using an electron energy analyser, the energy resolution for resonant inelastic X-ray scattering (RIXS) becomes decoupled from the X-ray spot size and instrument length. In this work, we develop PAX towards high energy resolution using a modern photoemission spectroscopy setup studying Ba2Cu3O4Cl2 at the Cu L3-edge. We measure a momentum transfer range of 24% of the first Brillouin zone simultaneously. Our results hint at the observation of a magnon excitation below 100 meV energy transfer and show intensity variations related to the dispersion of dd-excitations. With dedicated setups, PAX can become an alternative to the best and largest RIXS instruments, while at the same time opening new opportunities to acquire RIXS at a range of momentum transfers simultaneously and combine it with angle-resolved photoemission spectroscopy in a single instrument.

cond-mat.mtrl-sci↗

arXiv2022

Electron Dynamics at High-Energy Densities in Nickel from Non-linear Resonant X-ray Absorption Spectra

The pulse intensity from X-ray free-electron lasers (FELs) can create extreme excitation densities in solids, entering the regime of non-linear X-ray-matter interactions. We show L3-edge absorption spectra of metallic nickel thin films with fluences entering a regime where several X-ray photons are incident per absorption cross-section. Main features of the observed non-linear spectral changes are described with a predictive rate model for electron population dynamics during the pulse, utilizing a fixed density of states and tabulated ground-state properties.

cond-mat.mtrl-sci↗

arXiv2022

Ultrafast manipulation of the NiO antiferromagnetic order via sub-gap optical excitation

Wide-band-gap insulators such as NiO offer the exciting prospect of coherently manipulating electronic correlations with strong optical fields. Contrary to metals where rapid dephasing of optical excitation via electronic processes occurs, the sub-gap excitation in charge-transfer insulators has been shown to couple to low-energy bosonic excitations. However, it is currently unknown if the bosonic dressing field is composed of phonons or magnons. Here we use the prototypical charge-transfer insulator NiO to demonstrate that 1.5 eV sub-gap optical excitation leads to a renormalised NiO band-gap in combination with a significant reduction of the antiferromagnetic order. We employ element-specific X-ray reflectivity at the FLASH free-electron laser to demonstrate the reduction of the upper band-edge at the O 1s-2p core-valence resonance (K-edge) whereas the antiferromagnetic order is probed via X-ray magnetic linear dichroism (XMLD) at the Ni 2p-3d resonance (L2-edge). Comparing the transient XMLD spectral line shape to ground-state measurements allows us to extract a spin temperature rise of 65 +/- 5 K for time delays longer than 400 fs while at earlier times a non-equilibrium spin state is formed. We identify transient mid-gap states being formed during the first 200 fs accompanied by a band-gap reduction lasting at least up to the maximum measured time delay of 2.4 ps. Electronic structure calculations indicate that magnon excitations significantly contribute to the reduction of the NiO band gap.

cond-mat.str-el↗

arXiv2021

Probing electron and hole co-localization by resonant four-wave mixing in the extreme-ultraviolet

The extension of nonlinear spectroscopic techniques into the x-ray domain is in its infancy but holds the promise to provide unique insight into the dynamics of charges in photoexcited processes, which are of fundamental as well as applied interest. We report on the observation of a third order nonlinear process in lithium fluoride at a free-electron laser. Exploring the yield of four wave mixing (FWM) in resonance with transitions to strongly localized core exciton states vs. delocalized Bloch states, we find resonant FWM to be a sensitive probe for the degree of charge localization: substantial sum- and difference-frequency generation is observed exclusively when in a one- or three-photon resonance with a LiF core exciton, with a dipole forbidden transition affecting details of the nonlinear response. Our reflection-geometry-based approach to detect FWM signals enables the study of a wide variety of condensed matter sample systems, provides atomic selectivity via resonant transitions and can be easily scaled to shorter wavelengths at free electron x-ray lasers.

physics.app-ph↗