arXiv subjects

David Busto

Publications and source records attributed to David Busto.

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

Disentangling the Effect of Ionic Coupling and Multiple Interfering Terms in Attosecond Molecular Interferometry

Attosecond interferometry in a two-color field is central to attosecond metrology and spectroscopy. In this technique, a photoelectron wave packet is released when a single photon from an extreme ultraviolet comb is absorbed. The wave packet then either emits or absorbs one or more near-infrared photons, leading to the formation of sidebands of the main photoelectron peaks. This picture applies well to atoms and assumes that the near-infrared laser pulse only acts on the photoelectron leaving the parent ion. The effect of the near-infrared pulse on the electronic structure of the cation is not considered, since the field usually cannot induce transitions between its electronic levels. Here, we demonstrate how dynamics induced by the near-infrared field in the cation can significantly impact the amplitude and phases of the sideband signal of the photoelectrons associated with specific dissociative channels of CO$_2$ molecules. This coupling of the near-infrared field with the molecular cation opens a third quantum pathway contributing to the signal measured in attosecond interferometry. Through angle- and energy-resolved characterization of the sideband oscillations, we observe reduction of interference amplitude over specific energy range upon angle integration. By comparison with theoretical predictions, we can isolate the contributions of specific interfering pathways to the two-color multi-pathway photoionization process. The scheme investigated in our work is general, and our observations highlight the importance of the additional pathway for accurately interpreting attosecond interferometry experiments involving molecules and more complex quantum systems.

physics.atom-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

Breakdown of the isotropic asymptotic approximation in two-colour photoionisation

The Wigner delay is defined as the energy derivative of the scattering phase of a particle in a given potential, unveiling the time taken (or gained) due to the interaction. The characterisation of this delay plays a central role in attosecond science, where the time resolution allows to gain information on the time interval required for a photoelectron to be emitted into the continuum after the absorption of a single photon. Attosecond interferometric techniques, based on two-colour (extreme ultraviolet and near-infrared) photoionisation schemes, cannot provide a direct measurement of the Wigner delay, because the low-frequency photon contributes with an additional delay, which is imprinted on the outgoing photoelectron. The isolation of the Wigner delay is usually achieved by appealing to the asymptotic approximation, which assumes that the two-photon delay is separable into a Wigner and a near-infrared-induced phase and provides a universal analytical expression for the latter. In this study, we introduce a self-referencing approach based on the implementation of non-consecutive extreme ultraviolet harmonics, in order to test the validity of the asymptotic approximation. We demonstrate its breakdown by observing a deviation of a few tens of milliradians (corresponding to a few attoseconds) between its predictions and the experimentally measured phases of the sideband oscillations generated in our scheme, in agreement with full-dimensional simulations.

physics.atom-ph↗

arXiv2025

Photoionization time delays probe electron correlations

The photoelectric effect, explained by Einstein in 1905, is often regarded as a one-electron phenomenon. However, in multi-electron systems, the interaction of the escaping electron with other electrons, referred to as electron correlation, plays an important role. For example, electron correlations in photoionization of the outer $s$-subshells of rare gas atoms lead to a substantial minimum in the ionization probability, which was theoretically predicted in 1972 and experimentally confirmed using synchrotron radiation. However, recent attosecond photoionization time delay measurements in argon strongly disagree with theory, thus raising questions on the nature of electron correlations leading to this minimum. In this work, combining high-spectral resolution attosecond interferometry experiments and novel theoretical calculations allows us to identify the most essential electron correlations affecting the photoemission. The measurement of time delays gives unprecedented insight into the photoionization process, unraveling details of the atomic potential experienced by the escaping electron and capturing its dynamics.

physics.atom-ph↗

arXiv2025

Testing Born's rule via photoionization of helium

It is shown how state-of-the-art attosecond photoionization experiments can test Born's rule -- a postulate of quantum mechanics -- via the so-called Sorkin test. A simulation of the Sorkin test under consideration of typical experimental noise and data acquisition efficiencies infers an achievable measurement precision in the range of the best Sorkin tests to date. The implementation of further fundamental tests of quantum mechanics is discussed.

quant-ph↗

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 $2{\pi}$ increase across the resonance or a sigmo\"idal less than ${\pi}$ 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

A multidimensional approach to quantum state tomography of photoelectron wavepackets

There is a growing interest in reconstructing the density matrix of photoelectron wavepackets, in particular in complex systems where decoherence can be introduced either by a partial measurement of the system or through coupling with a stochastic environment. To this end, several methods to reconstruct the density matrix, quantum state tomography protocols, have been developed and tested on photoelectrons ejected from noble gases following absorption of extreme ultraviolet (XUV) photons from attosecond pulses. It remains a challenge to obtain model-free, single scan protocols that can reconstruct the density matrix with high fidelities. Current methods require extensive measurements or involve complex fitting of the signal. Efficient single-scan reconstructions would be of great help to increase the number of systems that can be studied. We propose a new and more efficient protocol that is able to reconstruct the continuous variable density matrix of a photoelectron in a single time delay scan. It is based on measuring the coherences of a photoelectron created by absorption of an XUV pulse using a broadband infrared (IR) probe that is scanned in time and a narrowband IR reference that is temporally fixed to the XUV pulse. We illustrate its performance for a Fano resonance in He as well as mixed states in Ar arising from spin-orbit splitting. We show that the protocol results in excellent fidelities and near-perfect estimation of the purity.

quant-ph↗

arXiv2024

Anisotropy parameters for two-color photoionization phases in randomly oriented molecules: theory and experiment in methane and deuteromethane

We present a combined theoretical and experimental work investigating the angle-resolved phases of the photoionization process driven by a two-color field consisting of an attosecond pulse train and an infrared pulse in an ensemble of randomly oriented molecules. We derive a general form for the two-color photoelectron (and time-delay) angular distribution valid also in the case of chiral molecules and when relative polarizations of the photons contributing to the attosecond photoelectron interferometer differ. We show a comparison between the experimental data and the theoretical predictions in an ensemble of methane and deuteromethane molecules, discussing the effect of nuclear dynamics on the photoionization phases. Finally, we demonstrate that the oscillating component and the phase of the two-color signal can be fitted using complex asymmetry parameters, in perfect analogy with the atomic case.

physics.chem-ph↗

arXiv2023

Generation of entanglement using a short-wavelength seeded free-electron laser

Quantum entanglement between the degrees of freedom encountered in the classical world is challenging to observe due to the surrounding environment. To elucidate this issue, we investigate the entanglement generated over ultrafast timescales in a bipartite quantum system comprising two massive particles: a free-moving photoelectron, which expands to a mesoscopic length-scale, and a light-dressed atomic ion, which represents a hybrid state of light and matter. Although the photoelectron spectra are measured classically, the entanglement allows us to reveal information about the dressed-state dynamics of the ion and the femtosecond extreme ultraviolet pulses delivered by a seeded free-electron laser. The observed generation of entanglement is interpreted using the time-dependent von Neumann entropy. Our results unveil the potential for using short-wavelength coherent light pulses from free-electron lasers to generate entangled photoelectron and ion systems for studying spooky action at a distance.

quant-ph↗

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

Isotopic effects in molecular attosecond photoelectron interferometry

Isotopic substitution in molecular systems can affect fundamental molecular properties including the energy position and spacing of electronic, vibrational and rotational levels, thus modifying the dynamics associated to their coherent superposition. In extreme ultraviolet spectroscopy, the photoelectron leaving the molecule after the absorption of a single photon can trigger an ultrafast nuclear motion in the cation, which can lead, eventually, to molecular fragmentation. This dynamics depends on the mass of the constituents of the cation, thus showing, in general, a significant isotopic dependence. In time-resolved attosecond photoelectron interferometry, the absorption of the extreme ultraviolet photon is accompanied by the exchange of an additional quantum of energy (typically in the infrared spectral range) with the photoelectron-photoion system, offering the opportunity to investigate in time the influence of isotopic substitution on the characteristics of the photoionisation dynamics. Here we show that attosecond photoelectron interferometry is sensitive to isotopic substitution by investigating the two-color photoionisation spectra measured in a mixture of methane (CH$_4$) and deuteromethane (CD$_4$). The isotopic dependence manifests itself in the modification of the amplitude and contrast of the oscillations of the photoelectron peaks generated in the two-color field with the two isotopologues. The observed effects are interpreted considering the differences in the time evolution of the nuclear autocorrelation functions in the two molecules.

physics.atom-ph↗

arXiv2023

Ultra-stable and versatile high-energy resolution setup for attosecond photoelectron spectroscopy

Attosecond photoelectron spectroscopy is often performed with interferometric experimental setups that require outstanding stability. We demonstrate and characterize in detail an actively stabilized, versatile, high spectral resolution attosecond beamline. The active-stabilization system can remain ultra-stable for several hours with an RMS stability of 13 as and a total pump-probe delay scanning range of \sim 400 fs. A tunable femtosecond laser source to drive high-order harmonic generation allows for precisely addressing atomic and molecular resonances. Furthermore, the interferometer includes a spectral shaper in 4f-geometry in the probe arm as well as a tunable bandpass filter in the pump arm, which offer additional high flexibility in terms of tunability as well as narrowband or polychromatic probe pulses. We show that spectral phase measurements of photoelectron wavepackets with the rainbow RABBIT technique (reconstruction of attosecond beating by two photon transitions) with narrowband probe pulses can significantly improve the photoelectron energy resolution. In this setup, the temporal-spectral resolution of photoelectron spectroscopy can reach a new level of accuracy and precision.

physics.atom-ph↗

arXiv2022

Ultrastable, high-repetition-rate attosecond beamline for time-resolved XUV-IR coincidence spectroscopy

The implementation of attosecond photoelectron-photoion coincidence spectroscopy for the investigation of atomic and molecular dynamics calls for a high-repetition-rate driving source combined with experimental setups characterized by excellent stability for data acquisition over time intervals ranging from a few hours up to a few days. This requirement is crucial for the investigation of processes characterized by low cross sections and for the characterization of fully differential photoelectron(s) and photoion(s) angular and energy distributions. We demonstrate that the implementation of industrial-grade lasers, combined with a careful design of the delay line implemented in the pump-probe setup, allows one to reach ultrastable experimental conditions leading to an error in the estimation of the time delays of only 12 as. This result opens new possibilities for the investigation of attosecond dynamics in simple quantum systems.

physics.atom-ph↗

arXiv2022

Theory of nuclear motion in RABBITT spectra

Reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) is a powerful photoelectron spectroscopy, offering direct access to internal dynamics of the target. It is being increasingly applied to molecular systems, but a general, computationally tractable theory of RABBITT spectra in molecules has so far been lacking. We show that under quite general assumptions, RABBITT spectra in molecules can be expressed as a convolution of the vibronic cross-correlation functions and two-electron photoionization matrix elements. We specialize the general expressions to the commonly-encountered special cases. We expect our theory to enable accurate modeling and interpretation of molecular RABBITT spectra in most medium-sized molecules.

physics.chem-ph↗

arXiv2022

Resonant two-photon ionization of helium atoms studied by attosecond interferometry

We study resonant two-photon ionization of helium atoms via the $1s3p$, $1s4p$ and $1s5p^1$P$_1$ states using the 15$^\mathrm{th}$ harmonic of a titanium-sapphire laser for the excitation and a weak fraction of the laser field for the ionization. The phase of the photoelectron wavepackets is measured by an attosecond interferometric technique, using the 17$^\mathrm{th}$ harmonic. We perform experiments with angular resolution using a velocity map imaging spectrometer and with high energy resolution using a magnetic bottle electron spectrometer. Our results are compared to calculations using the two-photon random phase approximation with exchange to account for electron correlation effects. We give an interpretation for the multiple $\pi$-rad phase jumps observed, both at and away from resonance, as well as their dependence on the emission angle.

physics.atom-ph↗

arXiv2022

Continuous variable quantum state tomography of photoelectrons

We propose a continuous variable quantum state tomography protocol of electrons which result from the ionization of atoms or molecules by the absorption of extreme ultraviolet light pulses. Our protocol is benchmarked against a direct calculation of the quantum state of photoelectrons ejected from helium and argon in the vicinity of a Fano resonance. In the latter case, we furthermore distill ion-photoelectron entanglement due to spin-orbit splitting. This opens new routes towards the investigation of quantum coherence and entanglement properties on the ultrafast timescale.

physics.atom-ph↗

arXiv2022

Studying ultrafast Rabi dynamics with a short-wavelength seeded free-electron laser

Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field. They are ubiquitous in physics with applications in different areas such as photonics, nano-electronics, electron microscopy, and quantum information. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light-matter interaction within the rotating wave approximation\cite. Although intense nanometer-wavelength light-sources have been available for more than a decade, Rabi dynamics at such short wavelengths have not been observed directly. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser can drive Rabi oscillations between the ground state and an excited state in helium atoms. The measured photoemission signal revealed an Autler-Townes doublet as well as an avoided crossing, phenomena that are both trademarks of quantum optics. Using theoretical analyses that go beyond the strong-field approximation, we found that the ultrafast build-up of the doublet structure follows from a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond and few-femtosecond extreme-ultraviolet pulses, our results offer opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

quant-ph↗