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arXiv:2604.12838

2D quantum-path interference in high-harmonic generation driven by highly-bichromatic fields

Xiaozhou Zou, Lucie Jurkovičová, Anne Weber, Cong Zhao, Martin Albrecht, Ondřej Finke, Alexandr Vendl, Annika Grenfell, Wojciech Szuba, Jaroslav Nejdl, Eric Constant, Margarita Khokhlova, Emilio Pisanty, Ondřej Hort, Amelle Zaïr

quant-phphysics.opticsSubmitted Apr 14, 2026• Announced Apr 15, 2026
v1 · Apr 14, 2026v2 · Apr 20, 2026
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Abstract

We experimentally observe a new type of quantum-path interference, in two-dimensional(2D-QPI), in high-harmonic generation (HHG) driven by an orthogonally-polarised highly-bichromatic field. This regime is marked by comparable intensities of the two orthogonal colours. In this highly-bichromatic regime, we demonstrate that 2D-QPI is encoded in the measured harmonic intensity modulations with respect to the relative phase of the two-colour field. The modulations of the odd-order harmonics show a monomodal behaviour, whereas the even harmonics are modulated in a bimodal structure. Our calculations using the strong-field approximation and saddle-point method disentangle contributions from multiple quantum orbits in this HHG regime, revealing that the dipole response for both odd and even harmonics inherits the dynamic symmetry of the orthogonally-polarised driving field. This new type of 2D-QPI offers a novel route to HHG spectroscopy of attosecond electron dynamics by lifting up the dimensionality of the quantum paths involved in the interference.

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physics.opticsCross-listedarXiv:2606.20372•Jun 19, 2026•0 citations
We experimentally observe a new type of quantum-path interference, in two-dimensional(2D-QPI), in high-harmonic generation (HHG) driven by an orthogonally-polarised highly-bichromatic field. This regime is marked by comparable intensities of the two orthogonal colours. In this highly-bichromatic regime, we demonstrate that 2D-QPI is encoded in the measured harmonic intensity modulations with respect to the relative phase of the two-colour field. The modulations of the odd-order harmonics show a monomodal behaviour, whereas the even harmonics are modulated in a bimodal structure. Our calculations using the strong-field approximation and saddle-point method disentangle contributions from multiple quantum orbits in this HHG regime, revealing that the dipole response for both odd and even harmonics inherits the dynamic symmetry of the orthogonally-polarised driving field. This new type of 2D-QPI offers a novel route to HHG spectroscopy of attosecond electron dynamics by lifting up the dimensionality of the quantum paths involved in the interference.
We present a theoretical study of the high-order-harmonic generation (HHG) from coherent superposition states of a three-level system driven by monochromatic cw laser fields. The HHG spectrum can be enhanced by about 105{10}^{5}105 times via tuning the relative phase between the states which are initially prepared. Even if the ionization effects are taken into account, the enhancement factors are still up to about 102{10}^{2}102 times. The enhancement is interpreted as the quantum constructive interference of different dipole transitions between quasienergy states. To realize the interference, the intensity of the driving laser field is chosen such that frequencies of the harmonics generated from the different dipole-transition paths, which are dependent on the ac Stark shifted energy separation of quasienergy states, are equal to each other. Moreover, the case studies of HHG spectra from a coherent superposition state of a three-level system show that the enhancement of harmonics is closely related to the harmonic strengths of the dipole transitions, as well as the parity of quasienergy states which are involved in the dipole-transition paths. The reduction of enhancement factors due to ionization effects is also qualitatively analyzed.
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.
High-harmonic generation (HHG) driven by intense quantum light has recently emerged as a new frontier in strong-field physics. Yet, the mechanism underlying HHG with nonclassical fields such as bright squeezed vacuum (BSV) light—characterized by a vanishing mean electric field—remains elusive. In this work, we develop a fully quantum theory for HHG under arbitrary quantum driving fields. We show that the fluctuation component of the dipole correlation operator plays a central role in HHG with quantum light and is essential for BSV-driven HHG. Furthermore, our framework reveals the photon statistics distribution within individual harmonics and across different harmonics, demonstrating that the statistics inherit the statistical properties of the driving field. This theory overcomes key limitations of existing approaches and uncovers new quantum features of HHG in the presence of nonclassical light.
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 ωωω and a perturbative BSV field at 2ω2ω2ω, 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.
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.
High-harmonic generation (HHG) is governed by interference between electron trajectories. We propose that the dominant short and long trajectories define an experimentally addressable two-level subsystem: an attosecond path qubit (APQ). We formulate a trajectory-resolved density matrix to identify two distinct coherence-loss mechanisms: classical dephasing from ensemble averaging and quantum decoherence arising from the trace-out of unobserved degrees of freedom. By investigating shot-to-shot fluctuations and unresolved transverse momentum, we demonstrate that while dephasing suppresses coherence through averaging, the ``trace-out'' channel produces mixed states even for fixed driving parameters. We explore how these mechanisms modify APQ purity and show that mode selection and conditioning provide operational routes to isolate them. These results establish a reduced-state framework for diagnosing coherence loss in HHG and for engineering trajectory-based quantum states in attosecond interferometry.