Abstract 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.
Abstract 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.
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.
Recent developments in quantum light engineering have enabled the use of infrared bright squeezed vacuum (BSV) femtosecond pulses in nonlinear optics, including strong-field physics and high-harmonic generation. However, theory has focused on single-atom interactions, neglecting the crucial macroscopic aspect of light propagation through media. This raises a key question: How does BSV propagate in nonlinear media, and how this affects the nonlinear signals and the radiation’s quantumness? We address this with a fully quantized framework for propagation in gas media undergoing high-harmonic generation. We find that ionization and the associated photon losses cause decoherence, which limits the propagation length, degrades radiation’s quantumness, and reduces the emitted harmonics. However, these effects are not detrimental. We identify conditions that minimize propagation-induced decoherence while preserving detectable harmonics with super-Poissonian photon statistics. Our results establish fully quantized basis for exploring BSV in nonlinear optics, strong-field-quantum optics, and ultrafast science in all states of matter. Recent developments in strong-field quantum optics are usually modelled with approaches neglecting the propagation dynamics inside the medium. Here, the authors introduce a fully quantized framework for bright squeezed vacuum states propagating inside atomic media undergoing high-harmonic generation, unveiling the role of decoherence effects.
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.
High-harmonic generation (HHG) is a prototypical strong-field process in which intense light drives matter to emit radiation at integer multiples of the driving frequency. Extending HHG into the quantum-optical regime offers new opportunities to probe and control strongly nonlinear light-matter interactions using nonclassical states of light. Yet describing this regime requires a fully quantum treatment of the correlated electron-photon dynamics, which becomes computationally challenging for broadband, strongly squeezed fields. Here we solve the quantum-electrodynamical dynamics of a two-level system driven by bright squeezed vacuum in a converged multimode Hilbert space. Both the driving field and emitted harmonics are fully quantized, with the light-matter interaction treated nonperturbatively. This enables direct access to the multimode quantum state and its higher-order correlations beyond semiclassical sampling or perturbative descriptions. We show that squeezed-vacuum driving produces harmonic emission with qualitatively distinct second- and third-order photon correlations compared with coherent excitation. Moreover, back-action from the driven emitter strongly reshapes the incident squeezed field, generating pronounced Wigner-function negativities that evolve on attosecond timescales. Our results establish a fully quantum framework for broadband strong-field dynamics with squeezed light and provide a route to predicting and interpreting quantum-HHG experiments and their extension to more complex emitters.
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.