arXiv subjects

Michael Zürch

Publications and source records attributed to Michael Zürch.

7 recordsLinked to original sources

arXiv2020

Attosecond state-resolved carrier motion in quantum materials probed by soft X-ray XANES

Recent developments in attosecond technology led to tabletop X-ray spectroscopy in the soft X-ray range, thus uniting the element- and state-specificity of core-level x-ray absorption spectroscopy with the time resolution to follow electronic dynamics in real time. We describe recent work in attosecond technology and investigations into materials such as Si, SiO2, GaN, Al2O3, Ti, TiO2, enabled by the convergence of these two capabilities. We showcase the state-of-the-art on isolated attosecond soft x-ray pulses for x-ray absorption near edge spectroscopy (XANES) to observe the 3d-state dynamics of the semi-metal TiS2 with attosecond resolution at the Ti L-edge (460 eV). We describe how the element- and state-specificity at the transition metal L-edge of the quantum material allows to unambiguously identify how and where the optical field influences charge carriers. This precision elucidates that the Ti:3d conduction band states are efficiently photo-doped to a density of 1.9 x 10^21 cm^-3 and that the light-field induces coherent motion of intra-band carriers across 38% of the first Brillouin zone. Lastly, we describe the prospects with such unambiguous real-time observation of carrier dynamics in specific bonding or anti-bonding states and speculate that such capability will bring unprecedented opportunities towards an engineered approach for designer materials with pre-defined properties and efficiency. Examples are composites of semiconductors and insulators like Si, Ge, SiO2, GaN, BN, quantum materials like graphene, TMDCs, or high-Tc superconductors like NbN or LaBaCuO. Exiting are prospects to scrutinize canonical questions in multi-body physics such as whether the electrons or lattice trigger phase transitions.

cond-mat.mtrl-sci↗

arXiv2020

Discrete dispersion scan setup for measuring few-cycle laser pulses in the mid-infrared

In this work, we demonstrate a discrete dispersion scan scheme using a low number of flat windows to vary the dispersion of laser pulses in discrete steps. Monte Carlo simulations indicate that the pulse duration can be retrieved accurately with less than 10 dispersion steps, which we verify experimentally by measuring few-cycle pulses and material dispersion curves at 3 and 10 micrometer wavelength. This minimal measuring scheme using only five optical components without the need for high-precision positioners and interferometric alignment can be readily implemented in many wavelength ranges and situations.

physics.optics↗

arXiv2019

Attosecond time-domain measurement of core-excitonic decay in magnesium oxide

Excitation of ionic solids with extreme ultraviolet pulses creates localized core-excitons, which in some cases couple strongly to the lattice. Here, core-excitonic states of magnesium oxide are studied in the time domain at the Mg $\text{L}_{2,3}$ edge with attosecond transient reflectivity spectroscopy. Attosecond pulses trigger the excitation of these short-lived quasiparticles, whose decay is perturbed by time-delayed near infrared optical pulses. Combined with a few-state theoretical model, this reveals that the optical pulse shifts the energy of bright core-exciton states as well as induces features arising from dark core-excitons. We report coherence lifetimes for the first two core-excitons of $2.3 \pm 0.2$ and $1.6 \pm 0.5$ femtoseconds and show that these short lifetimes are primarily a consequence of strong exciton-phonon coupling, disclosing the drastic influence of structural effects in this ultrafast relaxation process.

cond-mat.mtrl-sci↗

arXiv2019

Differentiating Photoexcited Carrier and Phonon Dynamics in the Δ, L, and Γ Valleys of Si(100) with Transient Extreme Ultraviolet Spectroscopy

Transient extreme ultraviolet (XUV) spectroscopy probes core level transitions to unoccupied valence and conduction band states. Uncertainty remains to what degree the core-hole created by the XUV transition modifies the measurement of photoexcited electron and hole energies. Here, the Si {Ł_{2,3}} edge is measured after photoexcitation of electrons to the Δ, L, and Γ valleys of Si(100). The measured changes in the XUV transition probability do not energetically agree with the increasing electron photoexcitation energy. The data therefore experimentally confirm that, for the Si {Ł_{2,3}} edge, the time-dependent electron and hole energies are partially obscured by the core-hole perturbation. A model based on many-body approximations and the Bethe-Salpeter equation is successfully used to predict the core-hole{\apos}s modification of the final transition density of states in terms of both electronic and structural dynamics. The resulting fit time constants match the excited state electron thermalization time and the inter-valley electron-phonon, intra-valley electron-phonon, and phonon-phonon scattering times previously measured in silicon. The outlined approach is a more comprehensive framework for interpreting transient XUV absorption spectra in photoexcited semiconductors.

cond-mat.mtrl-sci↗

arXiv2018

Hot Phonon and Carrier Relaxation in Si(100) Determined by Transient Extreme Ultraviolet Spectroscopy

The thermalization of hot carriers and phonons gives direct insight into the scattering processes that mediate electrical and thermal transport. Obtaining the scattering rates for both hot carriers and phonons currently requires multiple measurements with incommensurate timescales. Here, transient extreme-ultraviolet (XUV) spectroscopy on the silicon 2p core level at 100 eV is used to measure hot carrier and phonon thermalization in Si(100) from tens of femtoseconds to 200 ps following photoexcitation of the indirect transition to the Δ valley at 800 nm. The ground state XUV spectrum is first theoretically predicted using a combination of a single plasmon pole model and the Bethe-Salpeter equation (BSE) with density functional theory (DFT). The excited state spectrum is predicted by incorporating the electronic effects of photo-induced state-filling, broadening, and band-gap renormalization into the ground state XUV spectrum. A time-dependent lattice deformation and expansion is also required to describe the excited state spectrum. The kinetics of these structural components match the kinetics of phonons excited from the electron-phonon and phonon-phonon scattering processes following photoexcitation. Separating the contributions of electronic and structural effects on the transient XUV spectra allows the carrier population, the population of phonons involved in inter- and intra-valley electron-phonon scattering, and the population of phonons involved in phonon-phonon scattering to be quantified as a function of delay time.

cond-mat.mtrl-sci↗

arXiv2017

Direct and Simultaneous Observation of Ultrafast Electron and Hole Dynamics in Germanium

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical/NIR pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by attosecond transient absorption spectroscopy (ATAS) in the extreme ultraviolet at the germanium M_{4,5}-edge (~30 eV). We decompose the ATAS spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8*10^{20}cm^{-3}. Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first order electron and hole decay of ~1 ps suggests a Shockley-Read-Hall recombination mechanism. The simultaneous observation of electrons and holes with ATAS paves the way for investigating few to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.

cond-mat.mtrl-sci↗

arXiv2017

Soliton explosion driven multi-octave supercontinuum generation by geometry-enforced dispersion design in antiresonant hollow-core fibers

Ultrafast supercontinuum generation in gas-filled waveguides is one enabling technology for many intriguing application ranging from attosecond metrology towards biophotonics, with the amount of spectral broadening crucially depending on the pulse dispersion of the propagating mode. Here we show that the structural resonances in gas-filled anti-resonant hollow core optical fiber provide an additional degree of freedom in dispersion engineering, allowing for the generation of more than three octaves of broadband light ranging deep UV wavelength towards the near infrared.Our observation relies on the introduction of a geometric-induced resonance in the spectral vicinity of the pump laser outperforming the gas dispersion, thus yielding a dispersion being independent of core size, which is highly relevant for scaling input powers.Using a Krypton filled fiber we observe spectral broadening from 200 nm towards 1.7 μm at an output energy of about 23 μJ within a single mode across the entire spectral bandwidth. Simulations show that the efficient frequency generation results from a new physical effect the soliton explosion originating from the strongly non-adiabatic mode dispersion profile.This effect alongside with the dispersion tuning capability of the fiber will enable compact ultrabroadband high energy sources spanning from the UV to the mid-infrared spectral range.

physics.optics↗