This work extends quantum optical models of high harmonic generation by considering a quantum stochastic analysis of the field modes coupled to an environment. In particular, we study the open system dynamics by solving the quantum Langevin equation for a non-linear driven cavity coupled to the environment. For an unstructured environment without memory, we show that the emission characteristics of the intense driven cavity is isomorphic to the process of high harmonic generation and a non-linear antenna. This is achieved by using the quantum regression theorem for the Markovian dynamics, and further allows to obtain the upper bound of the radiated power due to the emitter fluctuations. This opens the path to connect current quantum optical approaches of HHG with open system descriptions and towards driven-dissipative systems in the non-linear regime.
This work extends quantum optical models of high harmonic generation by considering a quantum stochastic analysis of the field modes coupled to an environment. In particular, we study the open system dynamics by solving the quantum Langevin equation for a non-linear driven cavity coupled to the environment. For an unstructured environment without memory, we show that the emission characteristics of the intense driven cavity is isomorphic to the process of high harmonic generation and a non-linear antenna. This is achieved by using the quantum regression theorem for the Markovian dynamics, and further allows to obtain the upper bound of the radiated power due to the emitter fluctuations. This opens the path to connect current quantum optical approaches of HHG with open system descriptions and towards driven-dissipative systems in the non-linear regime.
We present an analytical framework for the emergence of nonclassical radiation in strongly laser-driven quantum systems, with a focus on high-order harmonic generation (HHG). Starting from a Pauli-Fierz description, we employ a parametric factorization of the coupled light-matter wavefunction that reduces the dynamics to coupled equations for a field-driven electronic state and a quantized light mode. Within this framework, we identify a simple and predictive mechanism for nonclassicality: it originates from the nonlinear dependence of the electronic dipole response on the light-mode coordinate. An approximately constant dipole yields coherent radiation, a linear dependence produces squeezing, and higher-order nonlinearities give rise to Wigner-function negativity. We illustrate this mechanism for atomic and molecular model systems and analyze its scaling in multi-emitter configurations, indicating routes toward high-photon-number nonclassical radiation in HHG. Our results provide a transparent connection between strong-field dynamics and quantum-optical properties of emitted light, offering a basis for engineering nonclassical states in intense laser-matter interactions.
High harmonic generation (HHG) is a highly nonlinear optical process in which radiation from a strong driving field is up-converted into its high-order harmonics. In atomic systems, this nonlinearity manifests itself through the intensity scaling of the emitted harmonics with the driving field strength. Despite the highly nonlinear nature of HHG, when the driving field is prepared in a classical Gaussian state and atomic depletion remains negligible, the quantum statistical properties of the generated harmonics retains classical Gaussian quantum statistics. Driving HHG with bright squeezed vacuum (BSV) light challenges this paradigm, as its enhanced field fluctuations can modify the statistical properties of the generated harmonics. In this work, we investigate the conditions under which BSV-driven HHG gives rise to non-classical Gaussian states, and identify the regimes where this Gaussian description breaks down. For bichromatic driving by a strong coherent field at frequency ω and a perturbative BSV field at 2ω, the even-harmonic response is approximately linear in the BSV quadrature, leading to non-classical multimode Gaussian entanglement in the harmonic field. We show that this state can be described as a distributed collective squeezed mode over the even-harmonic manifold, and characterize its covariance matrix, entanglement structure, and quantum teleportation fidelity as an operational benchmark. Our results highlight the potential of non-classically driven HHG as a platform for engineering Gaussian and non-Gaussian states of light in the extreme ultraviolet regime.
We develop a theoretical framework for high-harmonic generation (HHG) driven by quantum states of light based on a temporal-mode expansion of the electromagnetic field. This approach extends previous single plane-wave mode treatments to realistic pulse configurations and arbitrary multi-mode states of light, resolving conceptual inconsistencies arising from non-normalizable infinite plane waves and establishing consistency between analytical and numerical methods. We derive a correction factor that quantifies deviations from the diagonal approximation (in which the yield becomes a statistical average over classical-field simulations) both for the response of a single atom and in the many-atom regime. Our results confirms that the HHG spectrum for atoms driven by any quantum state of light in free space is accurately described by averaging semi-classical calculations over the Husimi distribution, with no observable genuine quantum effects in the spectrum. We also demonstrate that in the many-atom regime, the mean-field coherent-state approximation underlying this treatment does not preserve probabilities, although unitarity is restored by in the diagonal approximation. The absence of genuine quantum effects in the HHG yield is attributed to the large photon numbers (∼1011) required to reach HHG intensities in free space, which render quantum fluctuations negligible. We discuss nanophotonic environments with ultrasmall mode volumes as potential platforms where few-photon strong-field processes could exhibit genuine quantum signatures.
The generation of higher-order harmonic radiation originating from the interaction of intense laser pulses with matter is typically described semiclassically: While the electronic structure and dynamics of matter is described quantum mechanically, the intense light field is described classically---and accordingly the generated harmonic radiation. However, pioneering experiments on quantum optical properties of high-order harmonic generation (HHG) in atomic gases from the group of P. Tzallas [I. Gonoskov et al., Sci. Rep. 6, 32821 (2016) and N. Tsatrafyllis et al., Nat. Commun. 8, 15170 (2017)], and theoretical investigations from the group of M. Lewenstein [M. Lewenstein et al., Nat. Phys. 17, 1104 (2021) and P. Stammer et al., Phys. Rev. Lett. 128, 123603 (2022)] have impressively demonstrated that light's quantum properties are observable in the strong-field realm. In this paper, we develop a quantum optical description of HHG in a bulk semiconductor originating from the nonlinear Bloch current. This mechanism of HHG, known as the intraband current, constitutes the major contribution to the emission spectrum for harmonic with energies of quanta roughly below the bandgap. Under certain approximations, employing a quantum description of both light and matter, we obtain analytical solutions, which allow us to analyze the classical and quantum optical characteristics of the fundamental mode of light and the harmonic modes. We find intricate but sufficiently mild modifications of the photon statistics of the fundamental mode and coherent displacements depending on the parameters of the driving laser field. Similar to high-harmonic generation in atoms, the fundamental and emitted harmonic field modes are entangled. Moreover, our analytical model predicts parameter ranges where these quantum optical properties will be most pronounced, allowing protocols for quantum information processing with high photon numbers over a large range of frequencies.
Interactions between photons (nonlinearities) enable a powerful form of control over the state of light. This control has enabled technologies such as light sources at new wavelengths, ultra-short optical pulses, frequency-comb metrology systems, even quantum light sources. Common to a wide variety of nonlinear optical technologies is an equilibrium between an energy source, such as an external laser, and dissipation, such as radiation loss or absorption. In the vast majority of these systems, the coupling between the system and the outside world (which leads to loss) is well described as “Markovian,” meaning that the outside world has no memory of its past state. In this work, we introduce a class of driven-dissipative systems in which a nonlinear cavity experiences non-Markovian coupling to the outside world. In the classical regime, we show that these non-Markovian cavities can have extremely low thresholds for nonlinear effects, as well as self-pulsing instabilities at THz rates, and rich phase diagrams with alternating regions of stability and instability. In the quantum regime, we show how these systems, when implemented on state-of-the-art platforms, can enable generation of strongly squeezed cavity states with intensity fluctuations that can be more than 15 dB below the classical limit, in contrast to the Markovian driven-dissipative cavity, in which the limit is 3 dB. In the regime of few-photon nonlinearity, such non-Markovian cavities can enable a deterministic protocol to generate Fock states of high order, which are long-desired, but still elusive at optical frequencies. We expect that exploiting non-Markovian couplings in nonlinear optics should in the future lead to even richer possibilities than those discussed here for both classical and quantum light manipulations.
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.