Jonathan Dubois, Viviane Cotte, Richard Taïeb, Camille Lévêque, Jérémie Caillat, Pranshu Dave, Pascal Salières, David Bresteau, Charles Bourassin-Bouchet, Anne L'Huillier, David Busto
quant-phphysics.atom-phSubmitted Jun 11, 2026• Announced Jun 12, 2026• 0 citations
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.
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.
Reconstruction of attosecond beating by interference of two-photon transitions is a cornerstone technique of attosecond chronoscopy, routinely used to extract photoemission delays from the phase of sideband oscillations. Here, we theoretically investigate the reconstruction of attosecond beating by interference of two-photon transitions protocol driven by quantum light and demonstrate that it is intrinsically sensitive to the quantum nature of the driving field. When the probe field is prepared in a nonclassical state, its photon statistics are imprinted onto photoelectrons via continuum-continuum transitions, giving rise to an additional time delay of several tens of attoseconds. We trace this delay to the phase associated with the second-order anomalous moment ⟨a[over ^]^{2}⟩ of the probe field. Extending the framework to a three-sideband configuration, which enables retrieval of the fourth-order anomalous moment ⟨a[over ^]^{4}⟩, we show that the interferometer exhibits significantly enhanced sensitivity to quantum fluctuations. Our work illustrates quantum attosecond photoelectron interferometry as a phase-sensitive probe of quantum light, offering a promising route for time-resolved quantum metrology at the attosecond scale.
A recurring structural pattern in recent quantum optics and quantum information preprints is that **photon statistics**—the full hierarchy of photon-number correlations, not merely mean intensities—serve as both a diagnostic and a control resource across physically distinct platforms. This paper synthesizes five to seven findings from the recent arXiv corpus (primary categories: physics.optics, physics.atom-ph, quant-ph) into a candidate heuristic framework: that the mapping between photon-statistical structure and physical observables constitutes a broadly applicable design primitive for quantum sensing, quantum communication, and light-matter control. We emphasize from the outset that this is a *heuristic reading*, not a derivation from a single unified formalism. The sources share vocabulary and structural analogies but do not derive from a common mathematical scaffold. Specifically, we draw on: (1) a general theoretical framework linking photon autocorrelation and cross-correlation functions directly onto photoelectron spectra in attosecond RABBIT spectroscopy [corpus:arxiv:2606.13447]; (2) the observation of collective emission from subwavelength solid-state emitter arrays despite strong inhomogeneous broadening, enabled by local superatom formation [corpus:arxiv:2606.07458]; (3) amplified optomechanical susceptibility as a resource for quantum Fisher information enhancement accessible via heterodyne detection [corpus:arxiv:2606.09716]; (4) the Tavis-Cummings accidental symmetry and its consequences for controllability of multi-qubit bosonic systems [corpus:arxiv:2606.12813, corpus:arxiv:2606.12906]; (5) ultra-high-Q superconducting tantalum resonators on 300 mm wafers as a scalable bosonic mode platform [corpus:arxiv:2606.10719]; and (6) bosonic cyclic codes that trade error-protection properties for fault-tolerant logical gate access via passive Gaussian rotations [corpus:arxiv:2606.11010]. A weakly connected addendum discusses the Stark echo technique for Rydberg atoms near surfaces [corpus:arxiv:2606.09759] as an analogy for coherence preservation under inhomogeneous field environments. The central falsification path is concrete: if photon-statistical structure does *not* improve parameter estimation precision beyond classical intensity-based bounds in a controlled RABBIT or optomechanical experiment with independently characterized quantum light sources, the framework's core claim fails. --- Authorship: Saluca Agentic AI Research Team (Saluca LLC). AI-drafted from arXiv preprint corpus on the date in the filename. Cited arXiv preprints: 2606.07458, 2606.09716, 2606.09759, 2606.10719, 2606.11010, 2606.12813, 2606.12906, 2606.13447
Correlations between optical modes, ranging from classical fluctuations to quantum entanglement, are a cornerstone of modern optics and emerging quantum technologies. However, probing these correlations on the natural timescale of electronic motion - the attosecond regime - remains a major challenge. Here, we generate and characterize correlated attosecond extreme-ultraviolet (XUV) emission by perturbing gas-phase high-harmonic generation with two-mode bright squeezed vacuum. The signal and idler fields imprint their correlated amplitude and phase fluctuations onto two families of harmonics, thereby transferring these correlations from the infrared to broadband XUV modes. Even harmonics serve as an intrinsic attosecond phase-sensitive probe of these correlations through interference between indistinguishable XUV pathways. Shot-resolved covariance measurements reveal the amplitude correlations, while even-harmonics resolve the phase correlations with sub-cycle precision. Time-domain reconstruction of the correlated emission reveals a transition from maximal fluctuations to near-silence within only 30 as. Whereas the signal and idler driven attosecond pulse trains exhibit excess fluctuations individually, their joint reconstruction shows strongly suppressed fluctuations, reflecting their shared correlations. These results establish a framework for generating and probing quantum correlations on attosecond timescales, opening the door to quantum attosecond science.
Abstract Correlations between optical modes, ranging from classical fluctuations to quantum entanglement, are a cornerstone of modern optics and emerging quantum technologies. However, probing these correlations on the natural timescale of electronic motion - the attosecond regime - remains a major challenge. Here, we generate and characterize correlated attosecond extreme-ultraviolet (XUV) emission by perturbing gas-phase high-harmonic generation with two-mode bright squeezed vacuum. The signal and idler fields imprint their correlated amplitude and phase fluctuations onto two families of harmonics, thereby transferring these correlations from the infrared to broadband XUV modes. Even harmonics serve as an intrinsic attosecond phase-sensitive probe of these correlations through interference between indistinguishable XUV pathways. Shot-resolved covariance measurements reveal the amplitude correlations, while even-harmonics resolve the phase correlations with sub-cycle precision. Time-domain reconstruction of the correlated emission reveals a transition from maximal fluctuations to near-silence within only 30 as. Whereas the signal and idler driven attosecond pulse trains exhibit excess fluctuations individually, their joint reconstruction shows strongly suppressed fluctuations, reflecting their shared correlations. These results establish a framework for generating and probing quantum correlations on attosecond timescales, opening the door to quantum attosecond science.
Until recently, attosecond optical spectroscopy and quantum optics evolved along non-overlapping directions. In attosecond science, attosecond pulses have been regarded as classical waves, applied to probe electron dynamics on their natural time scale. Here, we transfer fundamental concepts of quantum optics into attosecond physics, enabling control of both the properties of the XUV attosecond pulses and the quantum fluctuations of matter on attosecond time scales. By combining bright squeezed vacuum (BSV) with a strong laser field to drive high-harmonic generation, we transfer the quantum properties of the BSV onto the resulting XUV attosecond pulses. Applying advanced attosecond interferometry, we reconstruct the quantum state of the XUV high harmonics and their associated attosecond pulses with attosecond precision. Finally, we resolve the squeezing of the electron's wavepacket during one of the most fundamental strong-field phenomena - field induced tunneling. The ability to measure and control quantum correlations in both electrons and XUV attosecond pulses establishes a foundation for attosecond quantum electrodynamics, manipulating the quantum state of electrons and photons with sub-cycle precision.
For decades, ultrafast light-matter interactions have provided a powerful means to observe electrons in motion across a wide range of physical systems. This dissertation builds new theoretical frameworks to make sense of the emergent phenomena that arise when light drives matter into the strong-field regime, spanning atomic, molecular, and condensed-matter systems. The resulting dynamics leave their fingerprints on a variety of observables, such as photoionization spectra, high-harmonic generation, and nonlinear spectroscopic signals, each of which provides a different window onto the underlying electronic motion. The work is organized into two parts.The first part focuses on the electric-field observables of nonlinear optical signals. Because both the amplitude and phase of the emitted field are experimentally accessible through techniques such as spectral interferometry and electro-optic sampling, the full field itself serves as a rich observable for characterizing nonlinear responses in atomic, molecular, and condensed-matter systems. Leveraging this, the simulations presented here uncover novel and largely unexplored physical phenomena encoded in these field observables. The second part turns to optical spectroscopy with quantum light. Although nonlinear optical processes are conventionally modeled within a semiclassical framework, treating the matter quantum mechanically while the driving ultrafast fields remain classical, the resulting signals can nonetheless exhibit intrinsically non-classical properties. Building on this insight, a framework for interpreting experimental data is introduced and used to show that four-wave mixing driven by ultrafast femtosecond laser pulses generates bright squeezed light. Beyond squeezed light, strong field-matter interactions can also produce attosecond entangled photons, a distinct form of quantum light. Several strategies are proposed to enhance the efficiency of their generation, with the developed theory predicting rates of energy-time entangled biphoton production orders of magnitude beyond those achievable with conventional spontaneous parametric down-conversion (SPDC) sources. The studies presented here are initial steps toward investigating quantum properties of these systems through quantum phynonlinear spectroscopy, which is not achievable with classical light.