Quantum Electrodynamics in High-Harmonic Generation: Multitrajectory Ehrenfest and Exact Quantum Analysis.

Abstract

High-harmonic generation (HHG) is a nonlinear process in which a material sample is irradiated by intense laser pulses, causing the emission of high harmonics of incident light. HHG has historically been explained by theories employing a classical electromagnetic field, successfully capturing its spectral and temporal characteristics. However, recent research indicates that quantum-optical effects naturally exist or can be artificially induced in HHG, such as entanglement between emitted harmonics. Even though the fundamental equations of motion for quantum electrodynamics (QED) are well-known, a unifying framework for solving them to explore HHG is missing. So far, numerical solutions have employed a wide range of basis-sets, methods, and untested approximations. Based on methods originally developed for cavity polaritonics, here we formulate a numerically accurate QED model consisting of a single active electron and a single quantized photon mode. Our framework can, in principle, be extended to higher electronic dimensions and multiple photon modes to be employed in ab initio codes for realistic physical systems. We employ it as a model of an atom interacting with a photon mode and predict a characteristic minimum structure in the HHG yield vs phase-squeezing. We find that this phenomenon, which can be used for novel ultrafast quantum spectroscopies, is partially captured by a multitrajectory Ehrenfest dynamics approach, with the exact minima position sensitive to the level of theory. On the one hand, this motivates using multitrajectory approaches as an alternative for costly exact calculations. On the other hand, it suggests an inherent limitation of the multitrajectory formalism, indicating the presence of entanglement and true quantum effects (especially prominent for atomic and molecular resonances). Our work creates a roadmap for a universal formalism of QED-HHG that can be employed for benchmarking approximate theories, predicting novel phenomena for advancing quantum applications, and for the measurements of entanglement and entropy.