arXiv subjects

Camille Lévêque

Publications and source records attributed to Camille Lévêque.

At least 19 recordsLinked to original sources

arXiv2026

Quantum optical photoelectron interferometry

We present a general theoretical framework for multiphoton processes driven by quantum light fields, establishing a direct link between photon statistics and photoelectron observables. Our results show that the autocorrelation and cross-correlation functions, which quantify the underlying photon statistics, are directly mapped onto the resulting photoelectron spectra. Although our framework is broadly applicable, we demonstrate specifically in the example of reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) the influence of the light statistical properties. In this approach, the amplitude, contrast and phase of the oscillations of the sideband signal as a function of pump-probe delay reveal the quantum nature of light. We analyze these observables across several quantum configurations, including correlated infrared and harmonic modes, as well as the uncorrelated case with non-classical harmonic statistics, thereby establishing a general framework for quantum-light RABBIT spectroscopy. We compare the analytical theory with numerical simulations for the case of classical harmonics and an infrared field in a squeezed coherent state, obtaining excellent agreement. Our results reveal how the interplay between classical and quantum correlations dictates the coherence of the photoemission process, providing a new window into the quantum-optical foundations of attosecond science.

quant-ph↗

arXiv2026

High-order harmonic generation from an atom in a disordered environment

Using one-dimensional simulations analyzed through the lens of open quantum systems, we study the photoelectron's strong-field dynamics from an atom surrounded by a scattering environment stochastically structured. We theoretically investigate high-order harmonic generation from this situation. We show that local dephasing of the photoelectron wavepacket induced by elastic scattering leads to global decoherence. This drives a transition from quantum to classical behavior, as witnessed by the photoelectron probability density localizing around specific trajectories of the classical analog system: unstable periodic orbits. This phenomenon mirrors quantum scars traditionally observed in the eigenfunctions of time-independent systems, such as quantum billiards. Here, it emerges in-situ within a time-dependent framework, manifesting directly in the real-time dynamics from the ground state rather than solely through spectral analysis.

quant-ph↗

arXiv2025

Time-domain interferences as the source of electron-ion entanglement in Rabi-dressed photoemission

We investigate bipartite entanglement between a photoelectron and its parent ion when the latter undergoes Rabi oscillations, following the recent experiment of [Nandi et al. Science Advances 10, eado0668 (2024)]. Using numerical simulations on a model atom, we show that this entanglement results from ionization events occurring at different times, with the photoelectron leaving the ion in distinct superpositions of internal states due to the Rabi coupling. Our interpretation brings forward the possibility to access the purity of the photoion state from photoelectron spectra. Furthermore, we demonstrate a tomographic reconstruction of the dressed ionic state dynamics from the observable spectra.

physics.atom-ph↗

arXiv2025

Attosecond tunneling time measurements through momentum squeezing in strong field ionization

Tunneling of a particle through a potential barrier is a fundamental physical process and a major thought-provoking outcome of quantum physics. It is at the basis of multiple scientific and technological advances and strongly influences both the structuring and the dynamics of matter at the microscopic scale. Without a classical counterpart, it defies our intuitive perception and understanding of the motion of a particle. Thus, the temporal characterization of tunneling, typically in terms of the time spent "under the barrier", referred to as tunneling time, raises several debates and questions on its interpretation and measurability. Here we show that an electron wavepacket tunneling out of an atom through the potential barrier induced by a strong electric field, carries in its momentum profile the value of the corresponding tunneling time, in a self-probing manner. In a revisited interpretation of the attoclock setup, we view a circularly polarized light pulse as a temporal prism which maps the barrier configuration, and hence the tunneling dynamics, onto different photoelectron ejection directions. From our simulations, we find that tunneling times in the infrared regime are of the order of hundreds of attoseconds, in agreement with previous theories.

physics.atom-ph↗

arXiv2024

Complete retrieval of attosecond photoelectron dynamics from partially-coherent states in entangled photoemission

We show that the complete photoemission dynamics in situations of electron-ion entanglement can be retrieved from photoelectron spectral measurements without information on the ion. To this end, we develop an energy-time analysis of the photoelectron's reduced density matrix based on first principles. We test and assess our approach with numerical simulations on a low dimensional model molecule in interaction with broadband composite pulses occulting the vibrational resolution. Our method is directly applicable to recent experimental schemes measuring the photoelectron reduced density matrices in atomic and molecular photoemission. Therefore, it opens a new window on the dynamics of decoherence and entanglement at the attosecond timescale.

physics.chem-ph↗

arXiv2024

Probing Wigner time delays with photoelectron interferometry: Anisotropic long-range imprint of the short-range centrifugal potential

We consider the two-photon ionization of Hydrogen-like atoms. We find an approximate expression of the long-range phase based on an asymptotic expansion of the continuum eigenfunctions within the Wentzel-Kramers-Brillouin approximation. Combined with commonly used perturbative approaches, the resulting analytic formalism can treat, at the same time, the two-photon propensity rules, the anisotropy in the continuum-continuum photoionization time delay and the soft-photon regime.

physics.atom-ph↗

arXiv2024

Vibronic correlations in molecular strong field dynamics

We investigate ultrafast vibronic dynamics triggered by intense femtosecond infrared pulses in small molecules. Our study is based on numerical simulations performed with 2D model molecules, and analyzed in the perspective of the renown Lochfrass and Bond-Softening models. We give a new interpretation of the observed nuclear wave packet dynamics, with a focus on the phase of the bond oscillations. Our simulations also reveal intricate features in the field-induced nuclear motion that are not accounted for by existing models. Our analyses assign these features to strong dynamic correlations between the active electron and the nuclei, which significantly depend on the carrier envelope phase of the pulse, even for relatively ``long'' pulses, which should make them experimentally observable.

physics.chem-ph↗

arXiv2024

Anisotropic molecular photoemission dynamics: Interpreting and accounting for the nuclear motion

We investigate how vibration affects molecular photoemission dynamics, through simulations on two-dimension asymmetric model molecules including the electronic and nuclear motions in a fully correlated way. We show that a slight anisotropy in the electron-ion momentum sharing is sufficient to prevent one from unambigously characterizing the vibrationnaly averaged photoemission dynamics in terms of stereo Wigner delays. We further show that vibrational resolution can be retrieved in fixed-nuclei simulations, using effective molecular conformations that are specific to each vibrational channel. The optimal internuclear distances found empirically in 1-photon processes can be identified a priori using simple physical arguments. They also turn out to be efficient to simulate vibrationnally-resolved \rabbit measurements and to account for interchannel coherences in broadband 1-photon ionization.

physics.chem-ph↗

arXiv2023

Strong-field photoionization by circularly polarized light

We demonstrate that strong-field ionization of atoms driven by circularly polarized light becomes an adiabatic process when described in the frame rotating with the laser field. As a direct consequence, a conservation law emerges: in the rotating frame the energy of the tunneling electron is conserved for rotationally invariant potentials. This conservation law, arising from a classical picture, is retrieved through a proper classical-quantum correspondence when considering the full quantum system, beyond the Strong Field Approximation.

physics.atom-ph↗

arXiv2021

Fermionization via cavity-assisted infinite-range interactions

We study a one-dimensional array of bosons with infinite-range interactions mediated by a laser-driven dissipative optical cavity. The cavity-mediated infinite-range interactions open up a new pathway to fermionization, hitherto only known for dipolar bosons due to their long-range interactions. In parameter ranges attainable in state-of-the-art experiments, we systematically compare observables for bosons and fermions with infinite-range interactions. At large enough laser pump power, many observables, including density distributions in real and momentum space, correlation functions, eigenvalues of the one-body density matrix, and superradiance order parameter, become identical for bosons and fermions. We map out the emergence of this cavity-induced fermionization as a function of pump power and contact interactions. We discover that cavity-mediated interactions can compensate a reduction by several orders of magnitude in the strength of the contact interactions needed to trigger fermionization.

cond-mat.quant-gas↗

arXiv2021

Many-body density and coherence of trapped cold bosons

Many-body densities and correlation functions are of paramount importance for understanding quantum many-body physics. Here, we present a method to compute them; our approach is general and based on the action of bosonic or fermionic annihilation field operators on the many-body wavefunction. We analyze $N = 6$ quasi-one-dimensional harmonically-trapped bosons with weak to strong contact interaction strength up to the Tonks-Girardeau limit with infinite repulsion using the MultiConfigurational Time-Dependent Hartree method for indistinguishable particles (MCTDH-X). We compare our MCTDH-X solutions to the analytical ones in the infinite repulsion regime as well as to the so-called correlated pair wavefunction approach and find a good agreement. Since numerical approximations are not bound to the cases where analytical solutions are known, we thus demonstrate a general method to investigate high-order reduced density matrices and correlation functions in systems for which analytical solutions are unknown. We trace the build-up of correlation features in the crossover from weak interactions to the Tonks-Girardeau limit and find that the higher-order correlation functions and densities resemble those in the Tonks-Girardeau limit for way smaller interactions than anticipated from just the one-body density.

cond-mat.quant-gas↗

arXiv2020

Dynamics of Ultracold Bosons in Artificial Gauge Fields: Angular Momentum, Fragmentation, and the Variance of Entropy

We consider the dynamics of two-dimensional interacting ultracold bosons triggered by suddenly switching on an artificial gauge field. The system is initialized in the ground state of a harmonic trapping potential. As a function of the strength of the applied artificial gauge, we analyze the emergent dynamics by monitoring the angular momentum, the fragmentation as well the entropy and variance of the entropy of absorption or single-shot images. We solve the underlying time-dependent many-boson Schrödinger equation using the multiconfigurational time-dependent Hartree method for indistinguishable particles (MCTDH-X). We find that the artificial gauge field implants angular momentum in the system. Fragmentation -- multiple macroscopic eigenvalues of the reduced one-body density matrix -- emerges in sync with the dynamics of angular momentum: the bosons in the many-body state develop non-trivial correlations. Fragmentation and angular momentum are experimentally difficult to assess; here, we demonstrate that they can be probed by statistically analyzing the variance of the image entropy of single-shot images that are the standard projective measurement of the state of ultracold atomic systems.

cond-mat.quant-gas↗

arXiv2020

Optimized Observable Readout from Single-shot Images of Ultracold Atoms via Machine Learning

Single-shot images are the standard readout of experiments with ultracold atoms -- the tarnished looking glass into their many-body physics. The efficient extraction of observables from single-shot images is thus crucial. Here, we demonstrate how artificial neural networks can optimize this extraction. In contrast to standard averaging approaches, machine learning allows both one- and two-particle densities to be accurately obtained from a drastically reduced number of single-shot images. Quantum fluctuations and correlations are directly harnessed to obtain physical observables for bosons in a tilted double-well potential at an unprecedented accuracy. Strikingly, machine learning also enables a reliable extraction of momentum-space observables from real-space single-shot images and vice versa. This obviates the need for a reconfiguration of the experimental setup between in-situ and time-of-flight imaging, thus potentially granting an outstanding reduction in resources.

cond-mat.quant-gas↗

arXiv2020

Detecting One-Dimensional Dipolar Bosonic Crystal Orders via Full Distribution Functions

We explore the groundstates of a few dipolar bosons in optical lattices with incommensurate filling. The competition of kinetic, potential, and interaction energies leads to the emergence of a variety of crystal state orders with characteristic one- and two-body densities. We probe the transitions between these orders and construct the emergent state diagram as a function of the dipolar interaction strength and the lattice depth. We show that the crystal state orders can be observed using the full distribution functions of the particle number extracted from simulated single-shot images.

cond-mat.quant-gas↗

arXiv2020

Multiconfigurational time-dependent Hartree approaches for indistinguishable particles

In this Colloquium, the wavefunction-based Multiconfigurational Time-Dependent Hartree approaches to the dynamics of indistinguishable particles (MCTDH-F for Fermions and MCTDH-B for Bosons) are reviewed. MCTDH-B and MCTDH-F or, together, MCTDH-X are methods for describing correlated quantum systems of identical particles by solving the time-dependent Schrödinger equation from first principles. MCTDH-X is used to accurately model the dynamics of real-world quantum many-body systems in atomic, molecular, and optical physics. The key feature of these approaches is the time-dependence and optimization of the single-particle states employed for the construction of a many-body basis set, which yields nonlinear working equations. We briefly describe the historical developments that have lead to the formulation of the MCTDH-X methods and motivate the necessity for wavefunction-based approaches. We sketch the derivation of the unified MCTDH-F and MCTDH-B equations of motion for complete and also specific restricted configuration spaces. The strengths and limitations of the MCTDH-X approach are assessed via benchmarks against an exactly solvable model and via convergence checks. We highlight some applications to instructive and experimentally-realized quantum many-body systems: the dynamics of atoms in Bose-Einstein condensates in magneto-optical and optical traps and of electrons in atoms and molecules. We discuss the current development and frontiers in the field of MCTDH-X: theories and numerical methods for indistinguishable particles, for mixtures of multiple species of indistinguishable particles, the inclusion of nuclear motion for the nonadiabatic dynamics of atomic and molecular systems, as well as the multilayer and second-quantized-representation approaches, and the orbital-adaptive time-dependent coupled-cluster theory are discussed.

cond-mat.quant-gas↗

arXiv2020

MCTDH-X: The multiconfigurational time-dependent Hartree method for indistinguishable particles software

We introduce and describe the multiconfigurational time-depenent Hartree for indistinguishable particles (MCTDH-X) software. This powerful tool allows the investigation of ground state properties and dynamics of interacting quantum many-body systems in different spatial dimensions. The MCTDH-X software is a set of programs and scripts to compute, analyze, and visualize solutions for the time-dependent and time-independent many-body Schrödinger equation for indistinguishable quantum particles. As the MCTDH-X software represents a general solver for the Schrödinger equation, it is applicable to a wide range of problems in the fields of atomic, optical, molecular physics as well as condensed matter systems. In particular, it can be used to study light-matter interactions, correlated dynamics of electrons, as well as some aspects related to quantum information and computing. The MCTDH-X software solves a set of non-linear coupled working equations based on the application of the variational principle to the Schrödinger equation. These equations are obtained by using an ansatz for the many-body wavefunction that is a time-dependent expansion in a set of time-dependent many-body basis states. The time-dependence of the basis set enables MCTDH-X to deal with quantum dynamics at a superior accuracy as compared to, for instance, exact diagonalization approaches. Herein, we give an introduction to the MCTDH-X software via an easy-to-follow tutorial with a focus on accessibility. We use the double well to illustrate the fermionization of bosonic particles, the crystallization of fermionic particles, characteristics of the superfluid and Mott-insulator quantum phases in Hubbard models, and even dynamical quantum phase transitions. Our tutorial guides the potential user to apply the MCTDH-X software also to more complex systems.

cond-mat.quant-gas↗

arXiv2018

Dynamical distortions of structural signatures in molecular High Harmonic Spectroscopy

We study the signature of two-center interferences in molecular high-order harmonic spectra, with an emphasis on the spectral phase. With the help of both ab initio computations based on the time-dependent Schrödinger equation and the molecular Strong-Field Approximation (SFA) as developed by Chirila et al. [Physical Review A, 73, 023410 (2006)] and Faria [Physical Review A, 76, 043407 (2007)], we observe that the phase behavior is radically different for the short and the long trajectory contributions. By means of Taylor expansions of the molecular SFA, we link this effect to the dynamics of the electron in the continuum. More precisely, we find that the value of the electric field at recombination time plays a crucial role on the shape of the destructive interference phase-jump.

physics.atom-ph↗

arXiv2018

Multispecies time-dependent restricted-active-space self-consistent-field theory for ultracold atomic and molecular gases

We discuss the multispecies time-dependent restricted-active-space self-consistent-field theory, an \textit{ab initio} wavefunction-based theory for mixtures of ultracold atomic and molecular gases. We present the general theory, based on the time-dependent variational principle, and derive the equations of motion. The theory captures in a time-dependent setting, via the specification of the restricted-active-space scheme, different levels of approximation from the mean-field to the full configuration interaction approach. To assess its accuracy and to illustrate its ability to identify correlation effects at successive approximation levels, we apply the theory to compute the ground state energy of a Bose-Bose mixture interacting through a harmonic potential, for which the exact ground state energy is known analytically. We focus on the case of an ideal Bose gas interacting with a few impurities. The intra-species interaction between the impurities is relatively strong compared to the inter-species interaction between the impurities and the ideal noninteracting Bose gas. For this system, we find that an accurate description of the ground state necessitates the possibility of the theory to account for few-particle excitations out of the condensed phase; a situation well accounted for by the present restricted-active-space theory for mixtures; and not within reach for approaches not incorporating orbital-restriction schemes.

quant-ph↗