arXiv subjects

David M. Villeneuve

Publications and source records attributed to David M. Villeneuve.

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

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

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↗

arXiv2020

High-harmonic generation in metallic titanium nitride

High-harmonic generation is the cornerstone of nonlinear optics. It has been demonstrated in a wide range of crystalline systems including dielectrics, semiconductors, and semi-metals, as well as in gases, leaving metals out due to their low damage threshold. Here, we report on the high-harmonic generation in metallic titanium nitride (TiN) films. TiN is a refractory plasmonic metal, known for its high melting temperature and laser damage threshold, with optical properties similar to those of gold. We show that TiN can withstand laser pulses with peak intensities as high as 13 TW/cm$^2$, one order of magnitude higher than gold, enabling the emission of intraband harmonics up to photon energies of 11 eV. These harmonics can pave the way for compact and efficient plasmonic devices producing vacuum ultraviolet (VUV) frequency combs. Through numerical calculations and experimental studies, we show that the intensity scaling and angular anisotropy of the emitted VUV radiation stem from the anisotropic conduction band structure of TiN, thus confirming its intraband origin.

physics.optics↗

arXiv2019

Streaking strong-field double ionization

Double ionization in intense laser fields can comprise electron correlations, which manifest in the non-independent emission of two electrons from an atom or molecule. However, experimental methods that directly access the electron emission times have been scarce. Here, we explore the application of an all-optical streaking technique to strong-field double ionization both theoretically and experimentally. We show that both sequential and non-sequential double ionization processes lead to streaking delays that are distinct from each other and single ionization. Moreover, coincidence detection of ions and electrons provides access to the emission time difference, which is encoded in the two-electron momentum distributions. The experimental data agree very well with simulations of sequential double ionization. We further test and discuss the application of this method to non-sequential double ionization, which is strongly affected by the presence of the streaking field.

physics.atom-ph↗

arXiv2019

Spatiotemporal imaging of valence electron motion

Electron motion on the (sub-)femtosecond time scale constitutes the fastest response in many natural phenomena such as light-induced phase transitions and chemical reactions. Whereas static electron densities in single molecules can be imaged in real-space using scanning tunnelling and atomic force microscopy, probing real-time electron motion inside molecules requires ultrafast laser pulses. Here, we demonstrate an all-optical approach to imaging an ultrafast valence electron wave packet in real-time with a time-resolution of a few femtoseconds. We employ a pump-probe-deflect scheme that allows us to prepare an ultrafast wave packet \textit{via} strong-field ionization and directly image the resulting charge oscillations in the residual ion. This approach extends and overcomes limitations in laser-induced orbital imaging and may enable the real-time imaging of electron dynamics following photoionization such as charge migration and charge transfer processes.

physics.atom-ph↗

arXiv2017

Streak Camera for Strong-Field Ionization

Ionization of an atom or molecule by a strong laser field produces sub-optical cycle wave packets whose control has given rise to attosecond science. The final states of the wave packets depend on ionization and deflection by the laser field, which are convoluted in conventional experiments. Here, we demonstrate a technique enabling efficient electron deflection, separate from the field driving strong-field ionization. Using a mid-infrared deflection field permits one to distinguish electron wave packets generated at different field maxima of an intense few-cycle visible laser pulse. We utilize this capability to trace the scattering of low-energy electrons driven by the mid-infrared field. Our approach represents a general technique for studying and controlling strong-field ionization dynamics on the attosecond time scale.

physics.optics↗