arXiv subjects

Peter M. Kraus

Publications and source records attributed to Peter M. Kraus.

18 recordsLinked to original sources

arXiv2026

Transient High-Harmonic Generation from Solids: From Spectroscopy and Control to Programmable Emission

High-harmonic generation (HHG) from solids has emerged as a powerful probe of electronic structure and ultrafast dynamics in condensed matter systems. In this chapter, we review recent advances in solid-state HHG spectroscopy and control, with a focus on semiconductors and correlated materials. We discuss the theoretical foundations of HHG and summarize experimental approaches for extracting information from harmonic emission. HHG has been shown to be sensitive to a wide range of microscopic properties, including band structure, transition dipole moments, Berry phases, crystal symmetry, carrier populations, dephasing processes, and lattice dynamics. This sensitivity enables access to electronic and structural dynamics on femtosecond and attosecond timescales and has established HHG as a versatile spectroscopic tool. At the same time, the strong dependence of HHG on many coupled material and excitation parameters makes the emitted harmonics intrinsically difficult to associate with a single microscopic quantity. Rather than representing a limitation alone, this sensitivity also provides numerous pathways for control. We review how photoexcitation, multicolor driving fields, waveform engineering, and transient modification of material properties can be used to enhance, suppress, and shape harmonic emission. These developments position solid-state HHG not only as a spectroscopic technique, but also as a platform for programmable nonlinear optics with applications ranging from compact extreme-ultraviolet sources to super-resolution microscopy and ultrafast photonic devices.

physics.optics↗

arXiv2026

Programmable high-harmonic emission in solids through photon pathways

Ultrafast all-optical control of light emission is a central goal of extreme nonlinear optics, with implications for compact short-wavelength sources, petahertz optoelectronics, and label-free superresolution microscopy. High-harmonic generation in solids is a particularly attractive platform for this goal because it is highly sensitive to both the driving field and the material response, yet a generally applicable framework for controlling harmonic emission has remained elusive. Here, we demonstrate programmable control of high-harmonic emission in solids and show that it can be quantitatively described within a photon-pathway framework. We find that harmonic emission can be suppressed or enhanced by tuning two experimentally accessible quantities: the effective nonlinear order and the intrinsic emission phase. Across a wide range of semiconductors and dielectrics, this approach unifies parametric and non-parametric modulation, explains distinct delay-dependent spectral responses, and reproduces strong suppression, enhancement, and higher-order pathway revivals. Semiconductor Bloch equation simulations support the model and provide a complementary time-domain picture in which the control field reshapes the interference of sub-cycle emission events. These results establish high-harmonic generation in solids as a programmable emission process and provide a general route towards ultrafast optical switching, compact coherent short-wavelength sources, and label-free attosecond super-resolution microscopy.

physics.optics↗

arXiv2026

Roadmap on Attosecond Science

Twenty-five years have passed since the first experimental demonstration of attosecond pulses, marking the advent of our ability to resolve and control electron motion in real time. What began as a technological breakthrough - generating the shortest flashes ever produced - has evolved into a powerful approach for probing and steering electronic dynamics in atoms, molecules, and solids. This roadmap, authored by leading experts in the field, surveys the recent rapid progress in the generation and characterization of attosecond pulses, emerging attosecond measurement and control techniques, and their expanding range of applications. It reviews current and future developments in attosecond light sources, including novel laser technologies, waveform synthesizers, new schemes for high-order harmonic generation, attosecond pulse generation at free-electron lasers, and structured light. Advances in attosecond measurement methodologies are also discussed, encompassing all-attosecond pump-probe spectroscopy, attosecond four-wave mixing, attosecond microscopy, spectroscopy with light transients, and attosecond interferometry. Furthermore, the roadmap addresses applications of attosecond spectroscopy to reveal electron dynamics in molecules and condensed matter systems from both theoretical and experimental perspectives, and highlights emerging directions at the interface with quantum optics and quantum entanglement. Overall, this work aims to serve as a comprehensive resource for navigating the evolving landscape of attosecond science.

physics.optics↗

arXiv2025

Attosecond high-harmonic interferometry probes orbital- and band-dependent dipole phase in magnesium oxide

Control over the spatial coherence, wavefront, and focusability of emitted light relies on understanding the intrinsic phase of the emission process, and vice versa, measuring phase can reveal insights about microscopic generation mechanisms. A thorough understanding of the origin of the dipole phase in solid-state high-harmonic generation is currently missing. Here, by employing attosecond interferometry with phase-locked XUV pulses, we directly assess the intensity- and frequency-dependent dipole phases in magnesium oxide (MgO) in solid-state HHG. We also quantify a nonlinear phase shift of the fundamental and disentangle its contribution from the dipole phase. Theoretical models (analytical, two-band, and full-band numerical simulations) support our results. The analytical approach aids future solid-state HHG experiments and simulations, while the full numerical model details orbital- and band-resolved current contributions to the dipole phase. Our research delivers the first combined quantitative measurement and rigorous theoretical description of the harmonic emission phase in solids.

physics.optics↗

arXiv2025

Extreme Ultraviolet High-Harmonic Interferometry of Excitation-Induced Bandgap Dynamics in Solids

Interferometry is a fundamental technique in physics, enabling precise measurements through the interference of waves. High-harmonic generation (HHG) in solids has emerged as a powerful method for probing ultrafast electronic dynamics within crystalline structures. In this study, we employed extreme ultraviolet (XUV) high-harmonic interferometry with phase-locked XUV pulse pairs to investigate excitation-induced bandgap dynamics in solids. Our experiments on amorphous SiO2 and crystalline MgO, complemented by analytical modeling and semiconductor Bloch equation simulations, reveal a correlation between transient bandgap modifications and variations in the phase of harmonic emission. These findings suggest a potential pathway for sub-cycle, all-optical control of band structure modifications, advancing prospects for petahertz-scale electronic applications and attosecond diagnostics of carrier dynamics.

physics.optics↗

arXiv2024

Breaking Abbe's diffraction limit with harmonic deactivation microscopy

Nonlinear optical microscopy provides elegant means for label-free imaging of biological samples and condensed matter systems. The widespread areas of application could even be increased if resolution was improved, which is currently limited by the famous Abbe diffraction limit. Super-resolution techniques can break the diffraction limit but rely on fluorescent labeling. This makes them incompatible with (sub-)femtosecond temporal resolution and applications that demand the absence of labeling. Here, we introduce harmonic deactivation microscopy (HADES) for breaking the diffraction limit in non-fluorescent samples. By controlling the harmonic generation process on the quantum level with a second donut-shaped pulse, we confine the third harmonic generation to three times below the original focus size and use this pulse for scanning microscopy. We demonstrate that resolution improvement by deactivation is more efficient for higher harmonic orders, and only limited by the maximum applicable deactivation-pulse fluence. This provides a route towards sub-100~nm resolution in a regular nonlinear microscope. The new capability of label-free super-resolution can find immediate applications in condensed matter physics, semiconductor metrology, and biomedical imaging.

physics.optics↗

arXiv2024

Spatial polarization gating of high-harmonic generation in solids

High-harmonic generation from solids can be utilized as probe of ultrafast dynamics, but thus far only over extended sample areas, since its spatial resolution is diffraction-limited. Here we propose spatial polarization gating, that is using a spatially varying ellipticity of a driving laser pulse to reduce the spatial profile of high-harmonic emission below the diffraction limit and hence increase spatial resolution. We show experimentally and by numerical simulations that our method is generally applicable as suppressing high harmonics in elliptical fields is a common response in all solids. We also briefly explore the possibility of applying this technique to widefield imaging, specifically to nonlinear structured illumination microscopy. Our findings indicate that spatial polarization gating can enable all-optical femto-to-attosecond label-free imaging beyond the Abbe limit.

physics.optics↗

arXiv2024

Towards complete all-optical emission control of high-harmonic generation from solids

Optical modulation of high-harmonics generation in solids enables the detection of material properties such as the band structure and promising new applications such as super-resolution imaging in semiconductors. Various recent studies have shown optical modulation of high-harmonics generation in solids, in particular, suppression of high-harmonics generation has been observed by synchronized or delayed multi-pulse sequences. Here we provide an overview of the underlying mechanisms attributed to this suppression and provide a perspective on the challenges and opportunities regarding these mechanisms. All-optical control of high-harmonic generation allows for femtosecond, and in the future possibly subfemtosecond, switching, which has numerous possible applications: These range from super-resolution microscopy, to nanoscale controlled chemistry, and highly tunable nonlinear light sources.

physics.optics↗

arXiv2023

Linking High-Harmonic Generation and Strong-Field Ionization in Bulk Crystals

The generation of high-order harmonics in bulk solids subjected to intense ultrashort laser pulses has opened up new avenues for research in extreme nonlinear optics and light-matter interaction on sub-cycle timescales. Despite significant advancement over the past decade, a complete understanding of the involved phenomena is still lacking. High-harmonic generation in solids is currently understood as arising from nonlinear intraband currents, interband recollision and ionization-related phenomena. As all of these mechanisms involve or rely upon laser-driven excitation we combine measurements of the angular dependence of nonlinear absorption and high-order harmonic generation in bulk crystals to demonstrate the relation between high-harmonic emission and nonlinear, laser-induced ionization in solids. An unambiguous correlation between the emission of harmonics and laser-induced ionization is found experimentally, that is supported by numerical solutions of the semiconductor Bloch equations and calculations of orientation-dependent ionization rates using maximally localized Wannier-functions.

physics.optics↗

arXiv2022

Efficient extreme-ultraviolet high-order wave mixing from laser-dressed silica

The emission of high-order harmonics from solids \cite{ghimire11a,schubert14a,luu15a,golde08a} under intense laser-pulse irradiation is revolutionizing our understanding of strong-field solid-light interactions \cite{ghimire11a,schubert14a,luu15a,vampa15b,yoshikawa17a,hafez18a,jurgens20a}, while simultaneously opening avenues towards novel, all-solid, coherent, short-wavelength table-top sources with tailored emission profiles and nanoscale light-field control\cite{franz19a,roscamCLEO21}. To date, broadband spectra have been generated well into the extreme-ultraviolet (XUV) \cite{luu15a,luu18b,han19a,uzan20a}, but the comparatively low conversion efficiency still lags behind gas-based high-harmonic generation (HHG) sources \cite{luu15a,luu18b}, and have hindered wider-spread applications. Here, we overcome the low conversion efficiency by two-color wave mixing. A quantum theory reveals that our experiments follow a novel generation mechanism where the conventional interband and intraband nonlinear dynamics are boosted by Floquet-Bloch dressed states, that make solid HHG in the XUV more efficient by at least one order of magnitude. Emission intensity scalings that follow perturbative optical wave mixing, combined with the angular separation of the emitted frequencies, make our approach a decisive step for all-solid coherent XUV sources and for studying light-engineered materials.

physics.optics↗

arXiv2021

Coherent energy exchange between carriers and phonons in Peierls-distorted bismuth unveiled by broadband XUV pulses

In Peierls-distorted materials, photoexcitation leads to a strongly coupled transient response between structural and electronic degrees of freedom, always measured independently of each other. Here we use transient reflectivity in the extreme ultraviolet to quantify both responses in photoexcited bismuth in a single measurement. With the help of first-principles calculations based on density-functional theory (DFT) and time-dependent DFT, the real-space atomic motion and the temperature of both electrons and holes as a function of time are captured simultaneously, retrieving an anticorrelation between the $A_{1g}$ phonon dynamics and carrier temperature. The results reveal a coherent, bi-directional energy exchange between carriers and phonons, which is a dynamical counterpart of the static Peierls-Jones distortion, providing first-time validation of previous theoretical predictions.

cond-mat.mtrl-sci↗

arXiv2020

XUV Induced Bleaching of a Tin Oxo Cage Photoresist Studied by High Harmonic Absorption Spectroscopy

Inorganic molecular materials such as tin oxo cages are a promising generation of photoresists compatible with the demands of the recently developed Extreme UltraViolet (EUV) lithography technology. Therefore, a detailed understanding of the photon-induced reactions which occur in photoresists after exposure is important. We used XUV broadband laser pulses in the range of 25-40 eV from a table-top high-harmonic source to expose thin films of the tin oxo cage resist to shed light on some of the photo-induced chemistry via XUV absorption spectroscopy. During the exposure, the transmitted spectra were recorded and a noticeable absorbance decrease was observed in the resist. Dill parameters were extracted to quantify the XUV induced conversion and compared to EUV exposure results at 92 eV. Based on the absorption changes, we estimate that approximately 60% of tin-carbon bonds are cleaved at the end of the exposure.

physics.app-ph↗

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

Divergence control of high-harmonic generation

We show that the divergence of extreme ultraviolet pulses from high harmonic generation, which is directly linked to the shape and size of the refocused beam, can be controlled by the relative delay between the fundamental and its intense orthogonally polarized second harmonic in two-color high-harmonic generation. We find that the divergence is minimized close to the delays were the number of emitted photons is maximized. These findings are rationalized as suppression and enhancement of long and short electron trajectories as function of the phase of the two-color laser field, respectively. The orthogonally polarized second harmonic introduces a lateral momentum component that can select one trajectory whereas it deflects the other. At the same time, the second harmonic profoundly influences the tunnel ionization process that initiates high-harmonic generation, which provides another trajectory gate. Our scheme for controlling the divergence facilitates larger numerical apertures for extreme ultraviolet microscopy. In addition, the associated reduction of the size of the focus is beneficial for extreme ultraviolet nonlinear optics and spectroscopy, as well as imaging and metrology of embedded structures.

physics.optics↗

arXiv2019

Efficient table-top dual-wavelength beamline for ultrafast transient absorption spectroscopy in the soft X-ray region

We present a table-top beamline providing a soft X-ray supercontinuum extending up to 350 eV from high-order harmonic generation with sub-13 fs 1300 nm driving pulses and simultaneous production of sub-5 fs pulses centered at 800 nm. Optimization of the high harmonic generation in a long and dense gas medium yields a photon flux of ~2 x 10^7 photons/s/1% bandwidth at 300 eV. The temporal resolution of X-ray transient absorption experiments with this beamline is measured to be 11 fs for 800 nm excitation. This dual-wavelength approach, combined with high flux and high spectral and temporal resolution soft X-ray absorption spectroscopy, is a new route to the study of ultrafast electronic dynamics in carbon-containing molecules and materials at the carbon K-edge.

physics.optics↗

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↗

arXiv2015

Theoretical Study of Molecular Electronic and Rotational Coherences by High-Harmonic Generation

The detection of electron motion and electronic wavepacket dynamics is one of the core goals of attosecond science. Recently, choosing the nitric oxide (NO) molecule as an example, we have introduced and demonstrated a new experimental approach to measure coupled valence electronic and rotational wavepackets using high-harmonic generation (HHG) spectroscopy [Kraus et al., Phys. Rev. Lett. 111, 243005 (2013)]. A short outline of the theory to describe the combination of the pump and HHG probe process was published together with an extensive discussion of experimental results [Baykusheva et al., Faraday Discuss 171, 113 (2014)]. The comparison of theory and experiment showed good agreement on a quantitative level. Here, we present the generalized theory in detail, which is based on a generalized density matrix approach that describes the pump process and the subsequent probing of the wavepackets by a semiclassical quantitative rescattering approach. An in-depth analysis of the different Raman scattering contributions to the creation of the coupled rotational and electronic spin-orbit wavepackets is made. We present results for parallel and perpendicular linear polarizations of the pump and probe laser pulses. Furthermore, an analysis of the combined rotational-electronic density matrix in terms of irreducible components is presented, that facilitates interpretation of the results.

physics.atm-clus↗