Macroscopic Spin-Orbit Interaction through Strong-Field Pumping of Inhomogeneously Aligned Molecular Ensemble
arXiv:2602.09625
The paper investigates how a helical bi‑chromatic strong‑field pump interacting with a radially aligned molecular ensemble generates high‑harmonic radiation that carries orbital angular momentum, with the OAM sign set by the pump helicity, demonstrated via TDDFT simulations for H₂⁺ and N₂.
Abstract
We study the strong-field interaction of a helical bi-chromatic pump with an anisotropic and inhomogeneous molecular system in the form of planar distribution of radially aligned molecular ensemble. This setting gives rise to macroscopic spin-orbit interaction where High Harmonic radiation is emitted while imbued with Orbital Angular Momentum (OAM) whose sign is directly dictated by the helicity of the pump field. We demonstrate this phenomenon in ensembles of and molecules with Time-Dependent Density Functional Theory (TDDFT) simulations.