In the field of attosecond science, photoelectron spectroscopy and interferometry stand as a central topic not only for its ability to characterise attosecond pulses but also for its ability to make time resolved measurements of electron dynamics. This feature allows for its application across the many fields which depend on the behaviour of electrons. For these reasons, there is significant interest in improving these techniques. One such candidate is the implementation of quantum light states to replace the typical coherent light used for interferometry. In the past, this was not possible due to the weakness of quantum light sources. However, recent development has shown that high intensity bright squeezed vacuum sources are possible and can be made to have high enough intensities in order to drive nonlinear processes, which allows for possibilities within attosecond science. For this work, we will begin developing and characterising an intense bright squeezed vacuum source to be used for applications in photoelectron metrology.
In the field of attosecond science, photoelectron spectroscopy and interferometry stand as a central topic not only for its ability to characterise attosecond pulses but also for its ability to make time resolved measurements of electron dynamics. This feature allows for its application across the many fields which depend on the behaviour of electrons. For these reasons, there is significant interest in improving these techniques. One such candidate is the implementation of quantum light states to replace the typical coherent light used for interferometry. In the past, this was not possible due to the weakness of quantum light sources. However, recent development has shown that high intensity bright squeezed vacuum sources are possible and can be made to have high enough intensities in order to drive nonlinear processes, which allows for possibilities within attosecond science. For this work, we will begin developing and characterising an intense bright squeezed vacuum source to be used for applications in photoelectron metrology.
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.
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.
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.
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.
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.
Nonclassical states of light are central resources for quantum metrology and quantum information, yet most high performance squeezing platforms operate in narrowband or continuous-wave regimes where the quantum noise is effectively stationary. This work advances ultrafast quantum optics by demonstrating how squeezed states can be generated, measured, and engineered on femtosecond and attosecond time scales, so that quantum fluctuations become a controllable property of the optical waveform itself. In this work, broadband few-cycle coherent drivers are produced using the light field synthesizer (LFS) setup that coherently combines UV/VIS/NIR channels with independently adjustable delays and amplitudes. Ultrafast squeezed light is generated via degenerate four-wave mixing (DFWM) in fused silica using a three-beam interaction geometry, implemented as a quantum light field squeezer (QLFS) that enables quasi-collinear phase matching across a wide bandwidth. A metrology framework compatible with ultrashort pulses is developed: amplitude (intensity) uncertainty is extracted from shot-to-shot spectral statistics, while relative phase fluctuations are retrieved from spectral-interference fringes in channel-overlap regions. These observables are connected to a displaced squeezed state model by fitting variance expressions, enabling phase-space visualization through Wigner function reconstruction. Beyond static squeezing, the QLFS provides attosecond-resolved control of the generated quantum state by tuning inter-pulse delay and phase matching geometry, allowing the redistribution of uncertainty between conjugate quadratures and revealing time-dependent (sub-cycle) structure of the intensity uncertainty within the optical cycle. Finally, the work extends ultrafast quantum optics into solid-state systems by demonstrating squeezed light driven tunneling in a graphene-silicon-graphene phototransistor, where state-dependent modulation of current noise is observed alongside simultaneous optical uncertainty measurements. Together, these results establish a practical route to waveform-level quantum state engineering and motivate future ultrafast quantum metrology, strong field quantum optics control, and hybrid photonic electronic quantum technologies.