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arXiv:2604.06707 · Advanced Photonics

Attosecond quantum spectroscopy with entangled photon pairs

Zijian Lyu, Fengxiao Sun, Sili Yi, Jingze Li, Haodong Liu, Qiongyi He, Qihuang Gong, Misha Ivanov, Yunquan Liu

physics.opticsquant-phSubmitted Apr 8, 2026• Announced Apr 9, 2026• 0 citations
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Abstract

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 $g^{(2)}$ 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.

Journal reference
Advanced Photonics 9(1), 016001 (2026)
DOI
10.1117/1.AP.9.1.016001

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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.
Attosecond spectroscopy comprises several techniques to probe matter through electrons and photons. One frontier of attosecond methods is to reveal complex phenomena arising from quantum-mechanical correlations in the matter system, in the photon fields and among them. Recent theories have laid the groundwork for understanding how quantum-optical properties affect high-field photonics, such as strong-field ionization and acceleration of electrons in quantum-optical fields, and how entanglement between the field modes arises during the interaction. Here we demonstrate a new experimental approach that transduces some properties of a quantum-optical state through a strong-field nonlinearity. We perturb high-harmonic emission from a semiconductor with a bright squeezed vacuum field resulting in the emission of sidebands of the high-harmonics with super-Poissonian statistics, indicating that the emitted photons are bunched. Our results suggest that perturbing strong-field dynamics with quantum-optical states is a viable way to coherently control the generation of these states at short wavelengths, such as extreme ultraviolet or soft X-rays. Quantum correlations will be instrumental to advance attosecond spectroscopy and imaging beyond the classical limits.
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.
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.
Entangled photon pairs are a vital resource for quantum information, computation, and metrology. Although these states are routinely generated at optical frequencies, sources of quantum of light are notably lacking at extreme ultraviolet (XUV) and soft X-ray frequencies. Here, we show that strongly driven systems used for high harmonic generation (HHG) can become versatile sources of entangled photon pairs at these high frequencies. We present a general theory of photon pair emission from non-perturbatively driven systems, which we refer to as "strong field pair generation" (SFPG). We show that strongly driven noble gases can generate thousands of entangled pairs per shot over a large XUV bandwidth. The emitted pairs have distinctive properties in angle and frequency, which can be exploited to discriminate them from the background HHG signal. We connect SFPG theory to the three-step-model of HHG, showing that this pair emission originates from the impact of high frequency vacuum fluctuations on electron recombination. The light produced by SFPG exhibits attosecond Hong-Ou-Mandel correlations, and can be leveraged as a source of heralded single photon attosecond pulses. Our findings aid ongoing efforts to propel quantum optics into the XUV and beyond.