Quantum light-specifically light in noncoherent quantum states-can now be generated with intensities high enough to induce nonlinear responses in atoms, marking the emergence of a new "quantum era" in strong-field atomic physics. In this Letter, we explore the influence of quantum states of light on one of the key processes in this field: atomic double ionization. We develop a theoretical framework to model the interaction between a two-electron atom and light in arbitrary quantum states, such as phase-squeezed coherent states or bright squeezed vacuum states. Our results reveal that the quantum state of light significantly impacts the atomic double ionization process, leading to substantial changes in ionization probability and correlated electron momentum distribution.
Quantum light-specifically light in noncoherent quantum states-can now be generated with intensities high enough to induce nonlinear responses in atoms, marking the emergence of a new "quantum era" in strong-field atomic physics. In this Letter, we explore the influence of quantum states of light on one of the key processes in this field: atomic double ionization. We develop a theoretical framework to model the interaction between a two-electron atom and light in arbitrary quantum states, such as phase-squeezed coherent states or bright squeezed vacuum states. Our results reveal that the quantum state of light significantly impacts the atomic double ionization process, leading to substantial changes in ionization probability and correlated electron momentum distribution.
Squeezed coherent quantum light is described by the complex squeeze parameter ζ = s e i ϑ and the coherent-state displacement parameter β = | β | e i ϕ β . Our study of strong-field ionization [D. Habibović and D. B. Milošević, ], which focused on bright squeezed vacuum quantum light with β = 0 and s ≫ 1 , is extended to ionization by squeezed coherent light. It is shown that the amplitudes s and | β | strongly influence the ionization process, whereas phases ϑ and ϕ β play a less significant role. The present work provides a unified treatment of coherent, squeezed vacuum, and squeezed coherent light within a single theoretical framework. The quantum nature of the driving field is incorporated by averaging the strong-field ionization probability over the Husimi-Kano phase-space distribution. Using neon as a representative target, we analyze how the parameters characterizing squeezed coherent light modify photoelectron spectra and intensity-dependent enhancements. We show that nonclassical photon statistics can lead to a pronounced steepening of the rescattering plateau and, at low mean intensities, to an effective suppression of the nominal high-energy cutoff. These effects originate from the reduced weight of high-intensity field components inherent to squeezed states and have no analog in strong-field ionization driven by a coherent light. Our results highlight the potential for quantum-statistical control of strong-field ionization and provide a foundation for exploring laser-matter interactions driven by quantum light.
The recently available high-intensity quantum light pulses provide novel tools for controlling light-matter interactions. However, the rigor of the theoretical frameworks currently used to describe the interaction of strong quantum light with atoms and molecules remains unverified. Here, we establish a rigorous benchmark by solving the fully quantized time-dependent Schrödinger equation for an atom exposed to bright squeezed vacuum light. Our \textit{ab initio} simulations reveal a critical limitation of the widely used Q-representation: although it accurately reproduces the total photoelectron spectrum after tracing over photon states, it completely fails to capture the electron-photon joint energy spectrum. To overcome this limitation, we develop a general theoretical framework based on the Feynman path integral that properly incorporates the electron-photon quantum entanglement. Our results provide both quantitative benchmarks and fundamental theoretical insights for the emerging field of strong-field quantum optics.
Strong-field ionization is the cornerstone of attosecond physics, which has been extensively studied under coherent-state driving. Recently, the interface between attosecond physics and quantum optics has emerged as a new frontier. Yet, owing to experimental limitations, the role of the quantum nature of light in atomic strong-field ionization has remained unexplored. Here, we demonstrate strong-field ionization of xenon atoms driven by bright squeezed vacuum (BSV) with average pulse energy up to 10 \textmu J. We show that, as a nonclassical state with zero mean field and strong intensity fluctuations, BSV selectively enhances the spider-like holographic structures in the photoelectron momentum distributions. Using a quantum-light-corrected quantum-trajectory Monte Carlo (q-QTMC) model, we attribute this effect to the intrinsic coherence of trajectory pairs emitted within the same subcycle field fluctuation. These dynamically correlated paths exhibit enhanced phase stability and remain robust against dephasing, whereas asynchronous paths are filtered out by field noise. Our results reveal a quantum-fluctuation-induced mechanism for coherence protection in strong-field processes, positioning BSV as an effective coherence filter and establishing a new regime of quantum-enabled noise-resilient ultrafast dynamics.
Nonlinear optical processes, mediated by multiphoton interactions rather than single-photon response, are routinely exploited to enable a range of light-based functionalities in devices and applications. Nonlinear effects are enhanced through higher intensity fields, which is a limiting strategy owing to potential radiation damage. An alternative strategy relies on the fluctuation redistribution typical of quantum light, but experimental demonstrations at the most fundamental level have been limited. Here we report experimental nonlinear tunnelling ionization of isolated atoms, a pivotal nonlinear process that drives high-harmonic generation and forms the basis of attosecond science, boosted by quantum light -- bright squeezed vacuum (BSV). A BSV light with an average pulse energy of 300 nJ achieves an effective intensity equivalent to that of a coherent light with 7.1 {\textmu}J, demonstrating a more than 20-fold quantum boost in nonlinear effect from BSV light. This boost is revealed by matching the peaks of the photoelectron momentum spectra produced by the BSV and coherent light using angular streaking. Furthermore, we demonstrate control of the effective intensity of the BSV by tuning the correlation function at fixed average pulse energy, establishing a robust method to tailor nonlinear processes via quantum statistics rather than classical intensity scaling. These findings may facilitate the development of quantum-controlled strong-field dynamics using tailored quantum light sources.
The extreme light-matter interaction has brought unique tools for the subfemtosecond control of electron dynamics [1] and ultra-fast spectroscopy [2]. Until recently, the strong-field regime was accessible only with coherent states of light, which can be well described by classical electric fields when many photons are present (Fig. 1a). With the use of intense states of non-classical light, this situation has changed. New opportunities emerge with bright squeezed vacuum (BSV), which can be generated from optical parametric amplification of quantum vacuum fluctuations. Unlike classical light, BSV is a quantum superposition of coherent states with an amplitudes spanning a range from zero to very high values, up to ~1 TW/cm2[3]. BSV has a zero mean electric field and the variance of the electric field oscillates at the double carrier frequency (Fig. 1a). How such a non-classical electric field can affect the dynamics of photoemitted electrons was theoretically demonstrated recently [4]. Furthermore, the photon-number distribution of BSV has a very long tail in contrast to coherent light. These photon-number distributions can be imprinted onto the photon statistics of optical harmonics [3] and the statistics of electrons [5].
Recently we have demonstrated the quantum nature of light in strongly laser driven atoms, and we have shown how the process of high harmonic generation can be used for the creation of highly non-classical light states, in particular superpositions of two coherent states, i.e., optical Schr\{o}dinger states [M. Lewenstein et al., Generation of optical Schr\odinger cat states in intense laser-matter interactions, Nat. Phys., 17 1104-1108 (2021)]. Here, we investigate the quantum optical description of the interaction, incorporating many atoms and the back-action of the high harmonic generation or above threshold ionization processes on the coherent state of the driving laser field. We show how the conditioning on high harmonic generation and above threshold ionization can lead to non-classical light states, and we discuss the key parameters that can be used for controlling and characterizing the non-classical states obtained after high harmonic generation. The theoretical results have been experimentally confirmed by demonstrating how the obtained coherent state superposition changes from an optical to kitten state by changing the number of atoms participating in the high harmonic generation process. Additionally, we experimentally verify the applicability of the approach for generating high photon number non-classical light states. This is shown by demonstrating the generation of a 9--photon optical state which, to our knowledge, is the highest photon number optical state experimentally reported. Our findings anticipate the development of new methods that naturally lead to the creation of high photon number controllable coherent state superpositions, advancing investigations in quantum technology.