arXiv subjects

Cord L. Arnold

Publications and source records attributed to Cord L. Arnold.

At least 19 recordsLinked to original sources

arXiv2026

Near single-cycle pulse generation using a cascaded all-bulk multi-pass cell compression system

We experimentally demonstrate the generation of sub-two-cycle optical pulses using a cascaded post-compression scheme based on two bulk multi-pass cells. Starting from 220 fs, 100 $μ$J pulses around 1030 nm, sequential spectral broadening and pulse compression reduce the pulse duration first to 50 fs and ultimately to 5.5 fs (1.6 optical cycles) at a central wavelength of 1058 nm. The ultra-broadband spectrum is enabled by a dispersion-controlled cavity. Comprehensive spectral, temporal, and spatial characterization confirms excellent pulse quality. Despite operating the second multi-pass cell at peak powers several hundred times above the critical power for self-focusing in fused silica, no significant spatio-spectral or spatio-temporal distortions are observed, enabling direct use of the compressed 40 $μ$J pulses in further experiments. Numerical simulations of the nonlinear spectral broadening show excellent agreement with the experimental results, supporting the underlying physical picture. These findings establish bulk multi-pass cells as an efficient, compact, and robust platform for generating few-cycle pulses with excellent beam quality, offering considerable potential for strong-field and ultrafast applications, including extreme-ultraviolet generation and isolated attosecond pulse production.

physics.optics↗

arXiv2026

Multiscale carrier-envelope phase characterization of 2-μm pulses delivered by a 200-kHz optical parametric amplifier

Light fields with a central wavelength of 2 um are very well suited for strong-field-driven charge carrier control: Their photon energy lies far below the band gap of many materials, while their oscillation period remains significantly shorter than the coherence time of charge carrier oscillations. The resulting potential for field-driven charge carrier control is contingent on the reproducibility of the field structure of such ultrashort laser pulses. Here, we present a compact 200-kHz laser system that delivers ultrashort pulses with a duration of less than 20 fs in the spectral range around 2 um and with a pulse energy of 25 uJ. The electric field structure of the 2-um pulses is characterized in detail. In particular, the carrier-envelope phase (CEP) is measured over a wide range of timescales, from microseconds to hours. Passive stabilization due to difference frequency generation results in a root mean square value of carrier-envelope phase noise of less than 70 mrad over all measured time scales. The applicability of the pulses is demonstrated by measuring CEP-dependent high-order harmonic spectra with energies of up to 160 eV.

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↗

arXiv2026

Optical parametric multi-pass cell amplifier

Ultrafast lasers with simultaneously high average and peak power have become indispensable for driving a multitude of applications, including high-harmonic generation, strong-field physics, and particle source applications. Both parametric amplifiers and post-compressed Ytterbium lasers have emerged as prime platforms to meet these demands. While multi-pass cell (MPC) based post-compression offers broadband output with high beam quality, it provides limited wavelength tunability and suffers from temporal contrast degradation. Conversely, optical parametric amplifiers (OPAs) provide spectral tunability and high temporal contrast but they are limited by low pump-to-signal conversion efficiency and spatial beam inhomogeneities. Here, we introduce the Optical Parametric Multi-Pass Cell Amplifier (OPMPC), a hybrid architecture that overcomes the limitations of both schemes. Our approach utilizes two non-collinearly intersecting MPCs providing broadband parametric amplification of the seed pulses and complete idler removal after each pass through the crystal, thereby suppressing back-conversion. We experimentally demonstrate a record pump-to-signal power conversion efficiency of 43% using a 1030 nm pump at a 1 kHz repetition rate with a pulse energy of 174 $μ$J. The amplified signal at 1500 nm exhibits excellent beam quality, power and spectral stability and is compressed to 48 fs, demonstrating a new platform for ultrafast pulse generation.

physics.optics↗

arXiv2025

Compact, intense attosecond sources driven by hollow Gaussian beams

High-order harmonic generation (HHG) enables the up-conversion of intense infrared or visible femtosecond laser pulses into extreme-ultraviolet attosecond pulses. However, the highly nonlinear nature of the process results in low conversion efficiency, which can be a limitation for applications requiring substantial pulse energy, such as nonlinear attosecond time-resolved spectroscopy or single-shot diffractive imaging. Refocusing of the attosecond pulses is also essential to achieve a high intensity, but difficult in practice due to strong chromatic aberrations. In this work, we address both the generation and the refocusing of attosecond pulses by sculpting the driving beam into a ring-shaped intensity profile with no spatial phase variations, referred to as a Hollow Gaussian beam (HGB). Our experimental and theoretical results reveal that HGBs efficiently redistribute the driving laser energy in the focus, where the harmonics are generated on a ring with low divergence, which furthermore decreases with increasing order. Although generated as a ring, the attosecond pulses can be refocused with greatly reduced chromatic spread, therefore reaching higher intensity. This approach enhances the intensity of refocused attosecond pulses and enables significantly higher energy to be delivered in the driving beam without altering the focusing conditions. These combined advantages open pathways for compact, powerful, tabletop, laser-driven attosecond light sources.

physics.optics↗

arXiv2024

Energy scaling in a compact bulk multi-pass cell enabled by Laguerre-Gaussian single-vortex beams

We report pulse energy scaling enabled by the use of Laguerre-Gaussian single-vortex ($\text{LG}_{0,l}$) beams for spectral broadening in a sub-40 cm long Herriott-type bulk multi-pass cell. Beams with orders ${l= 1-3}$ are generated by a spatial light modulator, which facilitates rapid and precise reconfiguration of the experimental conditions. 180 fs pulses with 610 uJ pulse energy are post-compressed to 44 fs using an $\text{LG}_{0,3}$ beam, boosting the peak power of an Ytterbium laser system from 2.5 GW to 9.1 GW. The spatial homogeneity of the output $\text{LG}_{0,l}$ beams is quantified and the topological charge is spectrally-resolved and shown to be conserved after compression by employing a custom spatio-temporal coupling measurement setup.

physics.optics↗

arXiv2024

XUV yield optimization of two-color high-order harmonic generation in gases

We perform an experimental two-color high-order harmonic generation study in argon with the fundamental of an ytterbium ultrashort pulse laser and its second harmonic. The intensity of the second harmonic and its phase relative to the fundamental are varied, in a large range compared to earlier works, while keeping the total intensity constant. We extract the optimum values for the relative phase and ratio of the two colors which lead to a maximum yield enhancement for each harmonic order in the extreme ultraviolet spectrum. Within the semi-classical three-step model, the yield maximum can be associated with a flat electron return time vs. return energy distribution. An analysis of different distributions allows to predict the required relative two-color phase and ratio for a given harmonic order, total laser intensity, fundamental wavelength, and ionization potential.

physics.atom-ph↗

arXiv2024

Compact, folded multi-pass cells for energy scaling of post-compression

Combining high peak and high average power has long been a key challenge of ultrafast laser technology, crucial for applications such as laser-plasma acceleration and strong-field physics. A promising solution lies in post-compressed ytterbium lasers, but scaling these to high pulse energies presents a major bottleneck. Post-compression techniques, particularly Herriott-type multi-pass cells (MPCs), have enabled large peak power boosts at high average powers but their pulse energy acceptance reaches practical limits defined by setup size and coating damage threshold. In this work, we address this challenge and demonstrate a novel type of compact, energy-scalable MPC (CMPC). By employing a novel MPC configuration and folding the beam path, the CMPC introduces a new degree of freedom for downsizing the setup length, enabling compact setups even for large pulse energies. We experimentally and numerically verify the CMPC approach, demonstrating post-compression of 8 mJ pulses from 1 ps down to 51 fs in atmospheric air using a cell roughly 45 cm in length at low fluence values. Additionally, we discuss the potential for energy scaling up to 200 mJ with a setup size reaching 2.5 m. Our work presents a new approach to high-energy post-compression, with up-scaling potential far beyond the demonstrated parameters. This opens new routes for achieving the high peak and average powers necessary for demanding applications of ultrafast lasers.

physics.optics↗

arXiv2024

The influence of final state interactions in attosecond photoelectron interferometry

Fano resonances are ubiquitous phenomena appearing in many fields of physics, e.g. atomic or molecular photoionization, or electron transport in quantum dots. Recently, attosecond interferometric techniques have been used to measure the amplitude and phase of photoelectron wavepackets close to Fano resonances in argon and helium, allowing for the retrieval of the temporal dynamics of the photoionization process. In this work, we study the photoionization of argon atoms close to the $3s^13p^64p$ autoionizing state using an interferometric technique with high spectral resolution. The phase shows a monotonic $2π$ increase across the resonance or a sigmoïdal less than $π$ variation depending on experimental conditions, e.g. the probe laser bandwidth. Using three different, state-of-the-art calculations, we show that the measured phase is influenced by the interaction between final states reached by two-photon transitions.

physics.atom-ph↗

arXiv2024

Highly versatile, two-color setup for high-order harmonic generation using spatial light modulators

We present a novel, interferometric, two-color, high-order harmonic generation setup, based on a turn-key Ytterbium-doped femtosecond laser source and its second harmonic. Each interferometer arm contains a spatial light modulator, with individual capabilities to manipulate the spatial beam profiles and to stabilize the relative delay between the fundamental and the second harmonic. Additionally, separate control of the relative power and focusing geometries of the two color beams is implemented to conveniently perform automatized scans of multiple parameters. A live diagnostics system gives continuous information during ongoing measurements.

physics.optics↗

arXiv2023

Time-resolved photoemission electron microscopy on a ZnO surface using an extreme ultraviolet attosecond pulse pair

Electrons photoemitted by extreme ultraviolet attosecond pulses derive spatially from the first few atomic surface layers and energetically from the valence band and highest atomic orbitals. As a result, it is possible to probe the emission dynamics from a narrow two-dimensional region in the presence of optical fields as well as obtain elemental specific information. However, combining this with spatially-resolved imaging is a long-standing challenge because of the large inherent spectral width of attosecond pulses as well as the difficulty of making them at high repetition rates. Here we demonstrate an attosecond interferometry experiment on a zinc oxide (ZnO) surface using spatially and energetically resolved photoelectrons. We combine photoemission electron microscopy with near-infrared pump - extreme ultraviolet probe laser spectroscopy and resolve the instantaneous phase of an infrared field with high spatial resolution. Our results show how the core level states with low binding energy of ZnO are well suited to perform spatially resolved attosecond interferometry experiments. We observe a distinct phase shift of the attosecond beat signal across the laser focus which we attribute to wavefront differences between the pump and the probe fields at the surface. Our work demonstrates a clear pathway for attosecond interferometry with high spatial resolution at atomic scale surface regions opening up for a detailed understanding of nanometric light-matter interaction.

physics.optics↗

arXiv2023

Measuring the quantum state of photoelectrons

A photoelectron, emitted due to the absorption of light quanta as described by the photoelectric effect, is often characterized experimentally by a classical quantity, its momentum. However, since the photoelectron is a quantum object, its rigorous characterization requires the reconstruction of the complete quantum state, the photoelectron's density matrix. Here, we use quantum state tomography to fully characterize photoelectrons emitted from helium and argon atoms upon absorption of ultrashort, extreme ultraviolet light pulses. While in helium we measure a pure photoelectronic state, in argon, spin-orbit interaction induces entanglement between the ion and the photoelectron, leading to a reduced purity of the photoelectron state. Our work shows how state tomography gives new insights into the fundamental quantum aspects of light-induced electronic processes in matter, bridging the fields of photoelectron spectroscopy and quantum information, and offering new spectroscopic possibilities for quantum technology.

quant-ph↗

arXiv2023

Spatial aberrations in high-order harmonic generation

We investigate the spatial characteristics of high-order harmonic radiation generated in argon, and observe cross-like patterns in the far field. An analytical model describing harmonics from an astigmatic driving beam reveals that these patterns result from the order and generation position dependent divergence of harmonics. Even small amounts of driving field astigmatism may result in cross-like patterns, coming from the superposition of individual harmonics with spatial profiles elongated in different directions. By correcting the aberrations using a deformable mirror, we show that fine-tuning the driving wavefront is essential for optimal spatial quality of the harmonics.

physics.optics↗

arXiv2023

Post-compression of multi-mJ picosecond pulses to few-cycles approaching the terawatt regime

Advancing ultrafast high-repetition-rate lasers to shortest pulse durations comprising only a few optical cycles while pushing their energy into the multi-millijoule regime opens a route towards terawatt-class peak powers at unprecedented average power. We explore this route via efficient post-compression of high-energy 1.2 ps pulses from an Ytterbium InnoSlab laser to 9.6 fs duration using gas-filled multi-pass cells (MPCs) at a repetition rate of 1 kHz. Employing dual-stage compression with a second MPC stage supporting a close-to-octave-spanning bandwidth enabled by dispersion-matched dielectric mirrors, a record compression factor of 125 is reached at 70% overall efficiency, delivering 6.7 mJ pulses with a peak power of about 0.3 TW. Moreover, we show that post-compression can improve the temporal contrast at picosecond delay by at least one order of magnitude. Our results demonstrate efficient conversion of multi-millijoule picosecond lasers to high-peak-power few-cycle sources, opening up new parameter regimes for laser plasma physics, high energy physics, biomedicine and attosecond science.

physics.optics↗

arXiv2022

Multi-gigawatt peak power post-compression in a bulk multi-pass cell at high repetition rate

The output of a 200 kHz, 34 W, 300 fs Yb amplifier is compressed to 31 fs with > 88 % efficiency to reach a peak power of 2.5 GW, which to date is a record for a single-stage bulk multi-pass cell. Despite operation 80 times above the critical power for self-focusing in bulk material, the setup demonstrates excellent preservation of the input beam quality. Extensive beam and pulse characterizations are performed to show that the compressed pulses are promising drivers for high harmonic generation and nonlinear optics in gases or solids.

physics.optics↗

arXiv2020

Characterizing ultrashort laser pulses with second harmonic dispersion scans

The dispersion scan (d-scan) technique has emerged as a simple-to-implement characterization method for ultrashort laser pulses. D-scan traces are intuitive to interpret and retrieval algorithms that are both fast and robust have been developed to obtain the spectral phase and the temporal pulse profile. Here, we give a review of the d-scan technique based on second harmonic generation. We describe and compare recent implementations for the characterization of few- and multi-cycle pulses as well as two different approaches for recording d-scan traces in single-shot, thus showing the versatility of the technique.

physics.optics↗

arXiv2020

A high-repetition rate attosecond light source for time-resolved coincidencespectroscopy

Attosecond pulses, produced through high-order harmonic generation in gases, have been successfully used for observing ultrafast, sub-femtosecond electron dynamics in atoms, molecules and solid state systems. Today's typical attosecond sources, however, are often impaired by their low repetition rate and the resulting insufficient statistics, especially when the number of detectable events per shot is limited. This is the case for experiments where several reaction products must be detected in coincidence, and for surface science applications where space-charge effects compromise spectral and spatial resolution. In this work, we present an attosecond light source operating at 200 kHz, which opens up the exploration of phenomena previously inaccessible to attosecond interferometric and spectroscopic techniques. Key to our approach is the combination of a high repetition rate, few-cycle laser source, a specially designed gas target for efficient high harmonic generation, a passively and actively stabilized pump-probe interferometer and an advanced 3D photoelectron/ion momentum detector. While most experiments in the field of attosecond science so far have been performed with either single attosecond pulses or long trains of pulses, we explore the hitherto mostly overlooked intermediate regime with short trains consisting of only a few attosecond pulses.e also present the first coincidence measurement of single-photon double ionization of helium with full angular resolution, using an attosecond source. This opens up for future studies of the dynamic evolution of strongly correlated electrons.

physics.atom-ph↗

arXiv2020

Attosecond electron-spin dynamics in Xe 4d photoionization

The photoionization of xenon atoms in the 70-100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe$^+$ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide new insight into the complex electron-spin dynamics of photo-induced phenomena.

physics.atom-ph↗