arXiv subjects

David N. Purschke

Publications and source records attributed to David N. Purschke.

7 recordsLinked to original sources

arXiv2026

Sub-cycle metrology of bright quantum light

In quantum optics, quantization of the electromagnetic field typically occurs in a finite volume - a cavity - which results in discrete frequency modes where photons are created, annihilated and exchanged between such modes. As a result, evolution of quantum optical states is periodic in the carrier wave of the field, measurement protocols return cycle-averaged information, and any sub-cycle evolution that is foundational to many light-matter interactions, especially at high field strengths, remains hidden. Adapting an attosecond technique, here we capture the electric-field evolution of a quantum optical state, femtosecond bright squeezed vacuum, with sub-cycle precision. We find that it consists of many stochastic, time-localized bursts within each pump pulse whose phase randomly switches between two values. We exploit the random phase flips to generate quantum random bit sequences with a generation rate that can reach petahertz frequencies. In addition, the sub-cycle resolution allows us to measure coherence functions of the waveforms between any two times, which we explain with a superposition of time-limited modes. These results bridge attosecond metrology and quantum optics and pave the way to measuring quantum light-matter interactions as they evolve on a few-femtosecond time scale, and integrate quantum randomness in petahertz electronics.

quant-ph↗

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

Phonon-driven decoherence of high-harmonic generation in the solid-state

High-harmonic generation in solids has emerged as a powerful probe of ultrafast electron dynamics and lattice motion, and recent theoretical work has suggested that thermally driven lattice fluctuations can act as an effective source of decoherence in the harmonic-generation process. However, a direct experimental link between high-harmonic emission and temperature-driven incoherent phonons has remained unclear. Here, we investigate the temperature dependence of high-harmonic generation in ultrapure silicon using reflection-geometry measurements over a wide temperature range. We observe that the harmonic yield increases significantly with decreasing temperature. To interpret these results, we introduce a one-dimensional atomic-chain model in which finite temperature is represented by random lattice displacements that mimic incoherent phonon fluctuations. The simulations reproduce the magnitude of temperature-dependent change of the harmonic signal and support a picture in which thermally induced lattice disorder enhances electron-hole decoherence, thereby reducing high-harmonic emission. Our results establish incoherent phonons as an important source of decoherence in solid-state high-harmonic generation.

cond-mat.mes-hall↗

arXiv2025

Effects of Zero-Point Motion in the High Harmonic Generation Spectrum of Solids

The interpretation of high-harmonic generation (HHG) in solids typically relies on phenomenological dephasing times far shorter than what is expected from microscopic scattering processes. Here we show that zero-point fluctuations associated with optical phonons naturally suppress long-range electronic coherences and generate clean harmonic spectra without introducing ad-hoc decoherence parameters. Using a 1D semiconductor composed of two distinct sites per unit cell and realistic phonon amplitudes, we demonstrate that random per-site optical-phonon jitter reproduces the spectral sharpening typically attributed to ultrafast $T_2$ dephasing. In contrast, acoustic phonons and local strain, whose distortions are correlated over nanometer scales, produce negligible spectral cleaning. We further show that such long-range site coherence leads to carrier-envelope-phase-dependent effects in the HHG spectrum driven by long pulses, but these effects collapse once optical-phonon-induced decoherence is included. Our results (i) identify optical zero-point motion as a key mechanism governing coherence in solid-state HHG, (ii) demonstrate that it can be qualitatively modeled in periodic solids through site-distance-dependent dephasing, and (iii) suggest that CEP-resolved measurements can probe electronic coherence lengths and atomic fluctuations in crystalline materials.

physics.optics↗

arXiv2025

Quantum engineering of high harmonic generation

In quantum sideband high harmonic generation (QSHHG), high harmonic generation is perturbed by a bright quantum field resulting in harmonic sidebands, with the intent to transfer non-classical properties from the quantum perturbation to the harmonic sidebands. So far, non-classical features have not been found in QSHHG yet. The closed form theory of QSHHG in atoms and solids developed here answers the question under which conditions non-classical features can be realized. QSHHG results in a multi-mode entanglement between harmonic sideband modes and perturbative quantum mode. A projective measurement on either creates a variety of non-classical states commonly used in quantum information science. This opens a pathway towards quantum engineering high harmonic generation as a short wavelength source for quantum information science.

quant-ph↗

arXiv2025

High Harmonic Generation from a Noble Metal

High-harmonic generation (HHG) in solids has typically been explored in transparent dielectrics and semiconductors. Metals have long been dismissed due to their strong reflectivity at infrared wavelengths. Here, we demonstrate HHG from silver - a noble metal - using few-cycle near-infrared laser pulses at near-normal incidence. Our results show that sub-cycle electron dynamics within the material's penetration depth can drive high-order harmonics, challenging the prevailing notion that metals are unsuited for infrared-driven strong-field processes. Despite silver's high reflectivity and large free-electron density, we observe nonperturbative harmonics extending into the extreme ultraviolet (up to 20 eV). Moreover, silver's multi-shot damage threshold proves surprisingly high (30 TW/cm^2) - comparable to large-bandgap dielectrics like magnesium oxide - thereby enabling intense strong-field processes in a metallic environment. Measuring the orientation dependence of the emitted harmonics reveals that the process arises from coherent electron dynamics in the crystal lattice, rather than from a plasma-driven mechanism. Time-dependent density-matrix simulations based on maximally localized Wannier functions show that low-order harmonics predominantly originate from conduction electrons near the Fermi surface (s- and p-type orbitals), whereas higher harmonics rely on bound d-electron excitations. These findings establish metals - long thought unfavorable for HHG - as a promising platform for ultrafast strong-field physics, extending high-harmonic spectroscopy to regimes in which lattice order and plasma formation directly intersect. This work expands the frontier of solid-state HHG to all-metallic attosecond pulse generation and underscores the potential of metals as robust XUV sources for advanced attosecond metrology.

physics.optics↗

arXiv2021

Ultrafast photoconductivity and terahertz vibrational dynamics in double-helix SnIP nanowires

Tin iodide phosphide (SnIP), an inorganic double-helix material, is a quasi-1D van der Waals semiconductor that shows promise in photocatalysis and flexible electronics. However, our understanding of the fundamental photophysics and charge transport dynamics of this new material is limited. Here, we use time-resolved terahertz (THz) spectroscopy to probe the transient photoconductivity of SnIP nanowire films and, with insight into the highly anisotropic electronic structure from quantum chemical calculations, measure an electron mobility as high as 280 $cm^2V^{-1}s^{-1}$. Additionally, the THz vibrational spectrum reveals a photoexcitation-induced charge redistribution that reduces the amplitude of a twisting mode of the outer SnI helix on picosecond timescales. Finally, we show that the carrier lifetime and mobility are limited by a trap density greater than $10^{18}\,cm^{-3}$. Our results provide insight into the optical excitation and relaxation pathways of SnIP and demonstrate a remarkably high carrier mobility for such a soft and flexible material.

cond-mat.mtrl-sci↗