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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

Strong Field Electron Emission Driven by a Bright Squeezed Vacuum

Andrei Rasputnyi, Jonas Heimerl, Jonathan Pölloth, Stefan Meier, Francesco Tani, Maria V. Chekhova, Peter Hommelhoff

Published Jun 23, 2025• 0 citations
Publisher

Abstract

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].

DOI
10.1109/cleo/europe-eqec65582.2025.11110135

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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].
Attosecond science relies on driving photoemitted electrons with the strong optical field of a laser pulse, which represents an intense classical coherent state of light. Bright squeezed vacuum is a quantum state of light that is also intense enough to drive strong-field physics. However, its mean optical electric field is zero, suggesting that, in a semi-classical view, electrons should not experience strong driving. The question arises if and how this quantum state of light can generate signatures of attosecond dynamics in strong-field photoemission. Here we show that the key signatures of strong-field physics-the high energy plateau and subsequent cut-off-also appear under driving of a needle tip by bright squeezed vacuum, but only when we post-select electron energy spectra on the individual photon number of each pulse. When averaging over many shots, we observe broad energy spectra without a plateau. This suggests that electrons driven by bright squeezed vacuum behave as if driven by an ensemble of coherent states of light. Our findings bridge strong-field physics and quantum optics, offering insights into bright squeezed vacuum and other quantum light states, and suggest the use of strongly driven electrons as quantum light sensors.
Abstract High-harmonic generation has been driving the development of attosecond science and sources. More recently, high-harmonic generation in solids has been adopted by other communities as a method to study material properties. However, so far high-harmonic generation has only been driven by classical light, despite theoretical proposals to do so with quantum states of light. Here we observe non-perturbative high-harmonic generation in solids driven by a macroscopic quantum state of light, a bright squeezed vacuum, which we generate in a single spatiotemporal mode. The process driven by a bright squeezed vacuum is considerably more efficient in the generation of high harmonics than classical light of the same mean intensity. Due to its broad photon-number distribution, covering states from 0 to 2 × 10 13 photons per pulse, and strong subcycle electric field fluctuations, a bright squeezed vacuum gives access to free carrier dynamics within a much broader range of peak intensities than accessible with classical light.
Bright squeezed vacuum (BSV) is an intense quantum state of light with zero mean electric field and huge photon number fluctuations, sufficiently intense to drive extreme nonlinear processes and imprint nonclassical statistics. However, the temporal structure of single BSV shots has not been fully characterized. Here, we retrieve the spectral and temporal pulse characteristics of a set of single-peak BSV shots. It is obtained by realizing a femtosecond BSV source at 1040 nm with a single spatial mode and performing single-shot spectral interferometry with a fully characterized coherent-state reference pulse. Our approach reveals that the group delay is consistent between the various shots, resulting in an average pulse duration of 27.2 fs, much shorter than the pump pulse, and a variation of 5.5 fs (standard deviation). We also observe a characteristic nodal structure in the spectral interferograms, demonstrating the BSV’s random phase ambiguity of π rad. Our approach demonstrates that BSV is a viable source of femtosecond light pulses for attosecond sub-cycle metrology of ultrafast electron dynamics.
Strong-field physics uses intense optical fields to probe and control electron motion on ultrafast timescales. Recent advances in bright squeezed vacuum have brought macroscopic quantum states of light into the ultrafast strong-field regime, opening prospects for high-harmonic generation and photoionization. Yet linking its phase-space structure to subcycle electron dynamics remains challenging. Here, we demonstrate strong-field tunneling ionization of xenon using a phase-referenced combination of coherent and squeezed fields, with the coherent field defining the ionization clock and quadrature fluctuations of the zero-mean squeezed field providing control. The squeezed field selectively modulates atomic tunneling barriers and electron wave packets, imprinting signatures on photoelectron momentum distributions, number statistics, and energy spectra. Using coincidence measurements of photon number and phase-sensitive photoelectron momentum distributions, we perform quantum state tomography of the driving field by reconstructing its Wigner function. These results establish a bidirectional interface between quantum optics and nonperturbative strong-field electron dynamics, in which the driving quantum field shapes subcycle electron motion while photoionization provides a phase-sensitive probe of the field's quantum state. This work opens new routes toward controlling electron dynamics with quantum light and phase-sensitive quantum state metrology through ultrafast strong-field electron 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.
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.