Quantum electrodynamics in high harmonic generation: multi-trajectory Ehrenfest and exact quantum analysis (2409.13614v1)

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 the 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. 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 employed a wide range of basis-sets 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. 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 multi-trajectory Ehrenfest dynamics approach, with the exact minima position sensitive to the level of theory. On the one hand, this motivates using multi-trajectory approaches as an alternative for costly exact calculations. On the other hand, it suggests an inherent limitation of the multi-trajectory formalism, indicating the presence of entanglement. Our work creates a road-map 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.