In this work, we explore the scheme of attosecond quantum interferometry (AQI), the quantum optical version of classical attosecond interferometry, which allows to measure quantum optical properties on the attosecond time-scale. We develop how the scheme of AQI can be used for quantum state engineering of the emitted harmonics, by varying the relative phase of a two-color driving field, and further enables one to manipulate the field correlations as well as their entanglement characteristics. In addition, this scheme allows us to learn properties of the phase-space distribution of the harmonic quantum state, by means of measuring an attosecond quantum tomography trace. This serves as a new type of protocol for in situ attosecond measurements of quantum optical observables. With this, we achieve to further connect all-optical attosecond measurement schemes with quantum optics, allowing for a rich manifold of observations.
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14 pages (7 main text + 7 Supplementary Material), 9 figures (4 main text + 5 Supplementary Material). Comments are welcome
In this work, we explore the scheme of attosecond quantum interferometry (AQI), the quantum optical version of classical attosecond interferometry, which allows to measure quantum optical properties on the attosecond time-scale. We develop how the scheme of AQI can be used for quantum state engineering of the emitted harmonics, by varying the relative phase of a two-color driving field, and further enables one to manipulate the field correlations as well as their entanglement characteristics. In addition, this scheme allows us to learn properties of the phase-space distribution of the harmonic quantum state, by means of measuring an attosecond quantum tomography trace. This serves as a new type of protocol for in situ attosecond measurements of quantum optical observables. With this, we achieve to further connect all-optical attosecond measurement schemes with quantum optics, allowing for a rich manifold of observations.
Abstract In this work, we explore the scheme of attosecond quantum interferometry (AQI), the quantum optical version of classical attosecond interferometry, which allows to measure quantum optical properties on the attosecond time-scale. We develop how the scheme of AQI can be used for engineering the phase-space and photon statistics properties of the emitted harmonics, using the relative phase of a two-color driving field as a control, and further enables to manipulate the field correlations as well as their entanglement characteristics. In addition, this scheme allows us to learn properties of the phase-space distribution of the harmonic quantum state, by means of measuring an attosecond quantum tomography trace. This serves as a new type of protocol for in situ attosecond measurements of quantum optical observables. With this, we achieve to further connect all-optical attosecond measurement schemes with quantum optics, allowing for a rich manifold of observations.
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.
The generation and control of extreme ultraviolet (XUV) radiation by high harmonic generation (HHG) have advanced ultrafast science, providing direct insights into electron dynamics on their natural time scale. Attosecond science has established the capability to resolve ultrafast quantum phenomena in matter by characterizing and controlling the classical properties of the high harmonics. Recent theoretical proposals have introduced novel schemes for generating and manipulating XUV HHG with distinct quantum features, paving the way to attosecond quantum optics. In this work, we transfer fundamental concepts in quantum optics into attosecond science. By driving the HHG process with a combination of an infrared bright squeezed vacuum (BSV, a non-classical state of light), and a strong coherent field, we imprint the quantum correlations of the input BSV onto both the ultrafast electron wavefunction and the harmonics' field. Performing in-situ HHG interferometry provides an insight into the underlying sub-cycle dynamics, revealing squeezing in the statistical properties of one of the most fundamental strong-field phenomena -- field induced tunneling. Our measurement allows the reconstruction of the quantum state of the harmonics through homodyne-like tomography, resolving correlated fluctuations in the harmonic field that mirror those of the input BSV. By controlling the delay between the two driving fields, we manipulate the photon statistics of the emitted attosecond pulses with sub-cycle accuracy. The ability to measure and control quantum correlations in both electrons and XUV attosecond pulses establishes a foundation for attosecond electrodynamics, manipulating the quantum state of electrons and photons with sub-cycle precision.
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.
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.
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.