Geometric Control of Cat States in High Harmonic Generation
Arti Gaharwar, Rocío Borrego-Varillas, Marcelo F. Ciappina, Anna G. Ciriolo, Javier Rivera-Dean, Philipp Stammer, Paraskevas Tzallas, Emilio Pisanty, Maciej Lewenstein
physics.opticsquant-phSubmitted Aug 20, 2026• Announced Aug 21, 2026• 0 citations
High-harmonic generation (HHG) provides a powerful platform for exploring the interaction between intense laser fields and matter on ultrafast timescales. Beyond its conventional description in terms of emitted radiation and electron dynamics, a fully quantum treatment of HHG reveals that the nonlinear light-matter interaction can modify the quantum state of the driving field itself, establishing correlations between the fundamental and harmonic modes. This perspective opens new possibilities for using HHG as a tool to engineer and control nonclassical states of light. In this work, we investigate the geometric properties of optical Schroedinger cat states generated in HHG via conditioning and post-selection. By analyzing the coherent-state displacements induced by different structured driving fields, we characterize the resulting phase-space evolution and the associated geometric phases of the generated quantum states. Particular emphasis is placed on how the polarization and spatial-mode structure of the driving light influence the geometry and evolution of displaced coherent states. Our results demonstrate that structured light offers a versatile means of controlling the geometric dynamics of HHG-generated cat states across the parameter space. Furthermore, we discuss the prospects for realizing genuinely topological optical cat states by exploiting more complex structured light configurations.
High-harmonic generation (HHG) provides a powerful platform for exploring the interaction between intense laser fields and matter on ultrafast timescales. Beyond its conventional description in terms of emitted radiation and electron dynamics, a fully quantum treatment of HHG reveals that the nonlinear light-matter interaction can modify the quantum state of the driving field itself, establishing correlations between the fundamental and harmonic modes. This perspective opens new possibilities for using HHG as a tool to engineer and control nonclassical states of light. In this work, we investigate the geometric properties of optical Schroedinger cat states generated in HHG via conditioning and post-selection. By analyzing the coherent-state displacements induced by different structured driving fields, we characterize the resulting phase-space evolution and the associated geometric phases of the generated quantum states. Particular emphasis is placed on how the polarization and spatial-mode structure of the driving light influence the geometry and evolution of displaced coherent states. Our results demonstrate that structured light offers a versatile means of controlling the geometric dynamics of HHG-generated cat states across the parameter space. Furthermore, we discuss the prospects for realizing genuinely topological optical cat states by exploiting more complex structured light configurations.
High-order harmonic generation (HHG) is a significant nonlinear phenomenon triggered by the interaction of intense laser fields with matter. As a high-quality coherent light source, it has found extensive applications in areas such as attosecond pulse generation and ultrafast spectroscopy. Recent studies have revealed the prevalent existence of nonclassical effects in high-harmonic radiation, including nonclassical photon statistics, intermodal correlations, and entanglement. It holds broad development prospects in directions including the generation of nonclassical states with high photon numbers, precise control of entanglement in solid-state systems, and integration with cavity quantum electrodynamics. This review systematically summarizes the research progress concerning the nonclassical effects in HHG. It begins with an overview of the semiclassical model and strong-field quantum theory, clarifying the differences in the quantum properties of harmonic fields when driven by coherent states versus nonclassical states. Subsequently, it focuses on various physical schemes for generating nonclassical optical field states, such as optical cat states and squeezed states, via this process. Research on strong-field HHG not only deepens our understanding of the fundamental nature of intense laser physics but also opens new avenues for the generation and application of quantum light sources in the extreme ultraviolet to X-ray spectral regions.
High-harmonic generation (HHG) involves the up-conversion of a high-intensity driving field into its harmonic orders. This process is intrinsically nonclassical, requiring from quantum mechanics for a complete explanation as, under suitable conditions, involves phenomena such as particle tunneling through a potential barrier. When exposed to a high-intensity, low-frequency laser field, bound electrons ionize via tunneling, accelerate under the driving field, and recombine with the parent ion, emitting high-harmonic radiation. However, electrons can follow two distinct pathways, short and long trajectories, during these steps. In this work, we evaluate the signatures left by these trajectories on the quantum-optical state after HHG, and observe that they lead to entanglement between the driving field and the generated harmonics. By leveraging these correlations, we use harmonic generation to herald the creation of optical Schr\"odinger-cat-like states in the driving field. Additionally, using an ab initio approach, we examine how propagation effects, which spatially separate the harmonic contributions from short and long trajectories, influence the nonclassical characteristics of the emitted light.
High-harmonic generation (HHG) involves the up-conversion of a high-intensity driving field into its harmonic orders. This process is intrinsically non-classical, requiring from quantum mechanics for a complete explanation as, under suitable conditions, involves phenomena such as particle tunneling through a potential barrier. When exposed to a high-intensity, low-frequency laser field, bound electrons ionize via tunneling, accelerate under the driving field, and recombine with the parent ion, emitting high-harmonic radiation. However, electrons can follow two distinct pathways -- short and long trajectories -- during these steps. In this work, we evaluate the signatures left by these trajectories on the quantum optical state after HHG, and observe that they lead to entanglement between the driving field and the generated harmonics. By leveraging these correlations, we use harmonic generation to herald the creation of optical Schrödinger cat-like states in the driving field. Additionally, using an ab-initio approach, we examine how propagation effects, which spatially separate the harmonic contributions from short and long trajectories, influence the non-classical characteristics of the emitted light.
Tailoring optical Schrödinger cat states via orientation-dependent high-harmonic generation in H2+
We theoretically demonstrate that the molecular orientation angle θ provides a structurally intrinsic, continuously tunable control parameter for engineering optical Schrödinger cat states via high-harmonic generation (HHG) in H2+. Coupling time-dependent Schrödinger equation simulations to the fully quantized HHG framework, we evaluate the Wigner functions of the post-selected harmonic-mode states under two complementary conditioning strategies. Conditioning on resonance-enhanced low-order harmonics exploits the complementary dipole selection rules of the 1σg→1σu and 1σg→1πu transitions, driving a kitten-cat crossover whose direction is opposite in the two channels as θ is varied. Conditioning on plateau harmonics instead exploits two-center destructive interference, producing a reentrant cat→kitten→cat transition controlled by the order-dependent interference angle θ∗(q). In both cases the crossover is decoupled from the laser intensity, focal geometry, and molecular density, offering a degree of control with no counterpart in atomic targets.
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.
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.