arXiv subjects

Henry Kapteyn

Publications and source records attributed to Henry Kapteyn.

10 recordsLinked to original sources

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

Soft X-ray high-harmonic generation in an anti-resonant hollow core fiber driven by a 3 $\mu$m ultrafast laser

High-harmonic upconversion driven by a mid-infrared femtosecond laser can generate coherent soft X-ray beams in a tabletop-scale setup. Here, we report on a compact ytterbium-pumped optical parametric chirped pulse amplifier (OPCPA) laser system seeded by an all-fiber front-end and employing periodically-poled lithium niobate (PPLN) nonlinear media operated near the pulse fluence limits of current commercially available PPLN crystals. The OPCPA delivers 3 $\mu$m wavelength pulses with 775 $\mu$J energy at 1 kHz repetition rate, with transform-limited 120 fs pulse duration, diffraction-limited beam quality, and ultrahigh 0.33% rms energy stability over >18 hours. Using this laser, we generate soft X-ray high harmonics (HHG) in argon gas by focusing into a low-loss, high-pressure gas-filled anti-resonant hollow core fiber (ARHCF), generating coherent light at photon energies up to the argon L-edge (250 eV) and carbon K-edge (284 eV), with high beam quality and ~1% rms energy stability. This work demonstrates soft X-ray HHG in a high-efficiency guided-wave phase matched geometry, overcoming the high losses inherent to mid-IR propagation in unstructured waveguides, or the short interaction lengths of gas cells or jets. The ARHCF can operate long term without damage, and with the repetition rate, stability and robustness required for demanding applications in spectro-microscopy and imaging. Finally, we discuss routes for maximizing the soft X-ray HHG flux by driving He at higher laser intensities using either 1.5 $\mu$m or 3 $\mu$m - the signal and idler wavelengths of the laser.

physics.optics↗

arXiv2022

Extension of the bright high-harmonic photon energy range via nonadiabatic critical phase matching

Extending the photon energy range of bright high-harmonic generation to cover the entire soft X-ray region is important for many applications in science and technology. The concept of critical ionization fraction has been essential, because it dictates the maximum driving laser intensity that can be used while preserving bright harmonic emission. In this work, we reveal a second, nonadiabatic critical ionization fraction that substantially extends the maximum phase-matched high-harmonic photon energy, that arises due to strong reshaping of the intense driving laser field. We validate this understanding through a systematic comparison between experiment and theory, for a wide range of pulse durations and driving laser wavelengths. In particular, high harmonics driven by intense few-cycle pulses experience the most pronounced spectral reshaping, significantly extending the bright photon energy range. We also present an analytical model that predicts the spectral extension that can be achieved for different driving lasers. This reveals an increasing role of nonadiabatic critical phase matching when driven by few-cycle mid-infrared lasers. These findings are important for the development of high-brightness soft X-ray sources for applications in spectroscopy and imaging.

physics.optics↗

arXiv2022

Bipolaronic nature of the pseudogap in (TaSe4)2I revealed via weak photoexcitation

The origin of the pseudogap in many strongly correlated materials has been a longstanding puzzle. Here, we uncover which many-body interactions underlie the pseudogap in quasi-one-dimensional (quasi-1D) material (TaSe4)2I by weak photo-excitation of the material to partially melt the ground state order and thereby reveal the underlying states in the gap. We observe the appearance of both dispersive and flat bands by using time- and angle-resolved photoemission spectroscopy. We assign the dispersive band to a single-particle bare band, while the flat band to a collection of single-polaron sub-bands. Our results provide direct experimental evidence that many-body interactions among small Holstein polarons i.e., the formation of bipolarons, are primarily responsible for the pseudogap in (TaSe4)2I. Recent theoretical studies of the Holstein model support the presence of such a bipolaron-to-polaron crossover. We also observe dramatically different relaxation times for the excited in-gap states in (TaSe4)2I (~600 fs) compared with another quasi-1D material Rb0.3MoO3 (~60 fs), which provides a new method for distinguishing between pseudogaps induced by polaronic or Luttinger-liquid many-body interactions.

cond-mat.str-el↗

arXiv2021

Spatially homogeneous few-cycle compression of Yb lasers via all-solid-state free-space soliton management

The high power and variable repetition rate of Yb femtosecond lasers make them very attractive for ultrafast science. However, for capturing sub-200 fs dynamics, efficient, high-fidelity, and high-stability pulse compression techniques are essential. Spectral broadening using an all-solid-state free-space geometry is particularly attractive, as it is simple, robust, and low-cost. However, spatial and temporal losses caused by spatio-spectral inhomogeneities have been a major challenge to date, due to coupled space-time dynamics associated with unguided nonlinear propagation. In this work, we use all-solid-state free-space compressors to demonstrate compression of 170 fs pulses at a wavelength of 1030nm from a Yb:KGW laser to ~9.2 fs, with a highly spatially homogeneous mode. This is achieved by ensuring that the nonlinear beam propagation in periodic layered Kerr media occurs in soliton modes and confining the nonlinear phase through each material layer to less than 1.0 rad. A remarkable spatio-spectral homogeneity of ~0.87 can be realized, which yields a high efficiency of >50% for few-cycle compression. The universality of the method is demonstrated by implementing high-quality pulse compression under a wide range of laser conditions. The high spatiotemporal quality and the exceptional stability of the compressed pulses are further verified by high-harmonic generation. This work represents the highest efficiency and the best spatio-spectral quality ever achieved by an all-solid-state free-space pulse compressor for few-cycle-pulse generation.

physics.optics↗

arXiv2020

X-ray linear dichroic ptychography

Biominerals such as seashells, corals skeletons, bone, and enamel are optically anisotropic crystalline materials with unique nano- and micro-scale organization that translates into exceptional macroscopic mechanical properties, providing inspiration for engineering new and superior biomimetic structures. Here we use particles of Seriatopora aculeata coral skeleton as a model and demonstrate, for the first time, x-ray linear dichroic ptychography. We map the aragonite (CaCO3) crystal c-axis orientations in coral skeleton with 35 nm spatial resolution. Linear dichroic phase imaging at the O K-edge energy shows strong polarization-dependent contrast and reveals the presence of both narrow (< 35{\deg}) and wide (> 35{\deg}) c-axis angular spread in sub-micrometer coral particles. These x-ray ptychography results were corroborated using 4D scanning transmission electron nano-diffraction on the same particles. Evidence of co-oriented but disconnected corallite sub-domains indicates jagged crystal boundaries consistent with formation by amorphous nanoparticle attachment. Looking forward, we anticipate that x-ray linear dichroic ptychography can be applied to study nano-crystallites, interfaces, nucleation and mineral growth of optically anisotropic materials with sub-ten nanometers spatial resolution in three dimensions.

physics.app-ph↗

arXiv2019

Coherent modulation of the electron temperature and electron-phonon couplings in a 2D material

Ultrashort light pulses can selectively excite charges, spins and phonons in materials, providing a powerful approach for manipulating their properties. Here we use femtosecond laser pulses to coherently manipulate the electron and phonon distributions, and their couplings, in the charge density wave (CDW) material 1T-TaSe$_2$. After exciting the material with a short light pulse, spatial smearing of the electrons launches a coherent lattice breathing mode, which in turn modulates the electron temperature. This indicates a bi-directional energy exchange between the electrons and the strongly-coupled phonons. By tuning the laser excitation fluence, we can control the magnitude of the electron temperature modulation, from ~ 200 K in the case of weak excitation, to ~ 1000 K for strong laser excitation. This is accompanied by a switching of the dominant mechanism from anharmonic phonon-phonon coupling to coherent electron-phonon coupling, as manifested by a phase change of $\pi$ in the electron temperature modulation. Our approach thus opens up possibilities for coherently manipulating the interactions and properties of quasi-2D and other quantum materials using light.

cond-mat.mtrl-sci↗

arXiv2019

Ultrafast electron calorimetry uncovers a new long-lived metastable state in 1T-TaSe$_2$ mediated by mode-selective electron-phonon coupling

Quantum materials represent one of the most promising frontiers in the quest for faster, lightweight, energy efficient technologies. However, their inherent complexity and rich phase landscape make them challenging to understand or manipulate in useful ways. Here we present a new ultrafast electron calorimetry technique that can systematically uncover new phases of quantum matter. Using time- and angle-resolved photoemission spectroscopy, we measure the dynamic electron temperature, band structure and heat capacity. We then show that this is a very sensitive probe of phase changes in materials, because electrons react very quickly, and moreover generally are the smallest component of the total heat capacity. This allows us to uncover a new long-lived metastable state in the charge density wave material 1T-TaSe$_2$, that is distinct from all of the known equilibrium phases: it is characterized by a significantly reduced effective heat capacity that is only 30% of the normal value, due to selective electron-phonon coupling to a subset of phonon modes. As a result, significantly less energy is required to melt the charge order and transform the state of the material than under thermal equilibrium conditions.

cond-mat.mtrl-sci↗

arXiv2017

Revealing the nature of the ultrafast magnetic phase transition in Ni by correlating extreme ultraviolet magneto-optic and photoemission spectroscopies

By correlating time- and angle-resolved photoemission and time-resolved transverse- magneto- optical Kerr effect measurements, both at extreme ultraviolet wavelengths, we uncover the universal nature of the ultrafast photoinduced magnetic phase transition in Ni. This allows us to explain the ultrafast magnetic response of Ni at all laser fluences - from a small reduction of the magnetization at low laser fluences, to complete quenching at high laser fluences. Both probe methods exhibit the same demagnetization and recovery timescales. We further show that the ultrafast demagnetization in Ni is indeed a magnetic phase transition that is launched within 20 fs, followed by demagnetization of the material within ~200 fs, and subsequent recovery of the magnetization on timescales ranging from 500 fs to >70 ps. We also provide evidence of two competing channels with two distinct timescales in the recovery process, that suggest the presence of coexisting phases in the material.

cond-mat.mtrl-sci↗

arXiv2014

Generation of phase-matched circularly-polarized extreme ultraviolet high harmonics for magnetic circular dichroism spectroscopy

Circularly-polarized extreme UV and X-ray radiation provides valuable access to the structural, electronic and magnetic properties of materials. To date, this capability was available only at large-scale X-ray facilities such as synchrotrons. Here we demonstrate the first bright, phase-matched, extreme UV circularly-polarized high harmonics and use this new light source for magnetic circular dichroism measurements at the M-shell absorption edges of Co. We show that phase matching of circularly-polarized harmonics is unique and robust, producing a photon flux comparable to the linearly polarized high harmonic sources that have been used very successfully for ultrafast element-selective magneto-optic experiments. This work thus represents a critical advance that makes possible element-specific imaging and spectroscopy of multiple elements simultaneously in magnetic and other chiral media with very high spatial and temporal resolution, using tabletop-scale setups.

physics.optics↗