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.
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) 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.
The past thirty years witnessed rapid developing of strong field physics that leads to the first generation of attosecond (10−18 s) pulses. The duration of available pulses has recently been reduced to less than 100 as, approaching the Kepler period of a classical electron revolving around the nucleus. For the first time, electron motions inside atoms, molecules and solids can be traced, probed and even steered in real time. It pushed the study on ultrafast dynamic processes into a new frontier, giving birth to attosecond physics. The development of attosecond pulses provides unprecedented coherent ultrashort XUV (extreme ultra-violet) of soft X-ray sources that enable imaging the atomic structure and resolving the related quantum dynamics for matter science. In particular, it allows the probing and monitoring of electron dynamics in the natural time scale of attoseconds with atomic spatial resolution. The generation and applications of attosecond pulses are directly related to the control and manipulation of the sub-cycle electron dynamics. Recent studies on the correlated multielectron dynamics have provided insight into the optical and dynamical properties of matter in the perspectives of time, phase and entanglement. It deepens our understanding on some of the fundamental questions, e.g., how the single or multiple photons are absorbed and how short are the quantum processes such as photoionization, tunneling ionization and charge migration. Although currently attosecond pulses are limited by the flux and pulse duration, the combination of attosecond pulses with intense infrared laser pulses paves new ways of controlling and probing electron dynamics in the domains of energy, time and space that lays the foundation for petahertz optoelectronics and attosecond pulse based transient spectroscopy. In this review, we will first briefly summarize the advancement of strong field and ultrafast physics including the relevant experimental findings, the theoretical explorations, the related technologies and the possible applications. Then we focus on the sub-cycle electron or multielectron dynamics and their manifestation on the ionization and coherent radiation properties. We start with the time behavior of Fano resonance and how it can be probed in time domain. In section 2, the correlated electron dynamics is discussed in term of anti-screening effect and Pauli effect that influence strong field ionization and high harmonic generation processes. In section 3, the coherent emission with frequency from terahertz to soft XUV and their joint measurement are discussed by emphasizing the generation mechanism of terahertz wave in two-color laser pulses. The developed high-harmonic and terahertz wave spectroscopy (HATS) is shown capable of imaging the molecular structure and dynamics. In section 4, the time-resolving of electron and hole dynamics and their coherence is proposed based on attosecond transient absorption technique. The coherence of ionization and the correlated electron dynamics is hinted crucial for electron-hole interaction. The topics are very limited and mainly selected from the perspectives of our group.
Attosecond quantum light, formed by the superposition of high-order harmonics driven by intense quantum light, opens new routes to probe quantum-mechanical correlations in matter. In this study, we have investigated the macroscopic propagation effects of quantum high-order harmonics generated by the combination of strong coherent and weak bright squeezed vacuum (BSV) lasers interacting with atomic gas. Our results reveal that the pressure-dependent intensity of harmonics arising from absorbing or emitting BSV photons differs from that of harmonics generated using only strong coherent pulses. Macroscopic propagation simulations indicate that the action phase of harmonics is perturbed by the weak BSV pulses. This perturbation modulates the phase mismatch of sub-cycle attosecond bursts and affects their quantum properties when the gas pressure varies. The ability to generate bright quantum high-order harmonics lays a foundation for the establishment and application of attosecond quantum spectroscopy.