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arXiv:2305.17263 · New Journal of Physics

Single photon zeptosecond interferometry

Geoffrey R. Harrison, Tobias Saule, R. Esteban Goetz, George N. Gibson, Camilo Granados, Bikash K Das, Marcelo F. Ciappina, Anh-Thu Le, Carlos A Trallero-Herrero

Published Sep 1, 2026• 1 citation
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Abstract

Abstract We demonstrate the generation of a train of attosecond XUV pulses that are in a superposition of wavefront states. Such superposition yields a high precision, self-referencing, common path XUV interferometer setup to produce pairs of spatially separated and independently controllable XUV pulses that are locked in phase and time with a temporal jitter of 3.5 zs (zs = zeptoseconds = 10 − 21 s ). In our approach, we can independently control the relative phase/delay of the two optical beams with a resolution of 52 zs. Since the jitter is on the order of the Compton time scale τ C = λ C / m e c 2 , we explore the level of correlation between the non-local photons by comparing different spatial mode superpositions. Further, thanks to the stability of the interferometer we can retrieve the interference pattern through photon counting. Through post-selection of different particle events we can analyze one, two or more photon events. We argue that this zeptosecond level of temporal precision will open the door for new dynamical quantum electrodynamics (QED) tests at lower intensities while photon counting experiments can also have an impact on the emerging field of quantum light in strong fields. We also discuss the potential impact on other areas, such as time-dependent QED, imaging, measurements of non-locality, and molecular quantum tomography.

DOI
10.1088/1367-2630/aea639

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Abstract We demonstrate the generation of a train of attosecond XUV pulses that are in a superposition of wavefront states. Such superposition yields a high precision, self-referencing, common path XUV interferometer setup to produce pairs of spatially separated and independently controllable XUV pulses that are locked in phase and time with a temporal jitter of 3.5 zs (zs = zeptoseconds = 10 − 21 s ). In our approach, we can independently control the relative phase/delay of the two optical beams with a resolution of 52 zs. Since the jitter is on the order of the Compton time scale τ C = λ C / m e c 2 , we explore the level of correlation between the non-local photons by comparing different spatial mode superpositions. Further, thanks to the stability of the interferometer we can retrieve the interference pattern through photon counting. Through post-selection of different particle events we can analyze one, two or more photon events. We argue that this zeptosecond level of temporal precision will open the door for new dynamical quantum electrodynamics (QED) tests at lower intensities while photon counting experiments can also have an impact on the emerging field of quantum light in strong fields. We also discuss the potential impact on other areas, such as time-dependent QED, imaging, measurements of non-locality, and molecular quantum tomography.
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.
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.
Bright squeezed light from parametric down-conversion in the infrared (IR) frequency range has triggered the emergence of attosecond quantum optics -- a new research field at the interface of quantum optics, strong-field physics, and attosecond technology. Two challenges arise at this interface: transferring quantum features of the IR light sources to the ultraviolet (UV) and extreme ultraviolet (XUV) frequency range via strong-field nonlinearities, and exploiting quantum optical properties of the nonlinear optical response as a new probe in ultrafast dynamics. Here, we address both by driving high-harmonic generation (HHG) in solids with entangled photon pairs either in degenerate or non-degenerate frequency modes. In the degenerate mode, single-shot measurements of harmonics up to the 10th order reveal strong photon bunching whose g(2)g^{(2)}g(2) first grows and then decreases with the harmonic order. We show that this behavior tracks different microscopic mechanisms responsible for harmonic emission, demonstrating the potential of attosecond quantum optical spectroscopy. In the non-degenerate case, the harmonics retain quantum-induced correlations, verified by wavelength-resolved second-order cross-correlation maps. Our findings demonstrate transfer of quantum photon correlations into the XUV domain and open a pathway toward quantum-enhanced attosecond spectroscopy and control of ultrafast dynamics in solids.