Nonadiabatic tunnel ionization of current-carrying orbitals of prealigned linear molecules in strong circularly polarized laser fields

Abstract

We derive the analytical formula of the ratio of the ionization rates of degenerate valence ${\ensuremath{\pi}}_{\ifmmode\pm\else\textpm\fi{}}$ orbitals of prealigned linear molecules in strong circularly polarized (CP) laser fields. Interestingly, our theory shows that the ionization ratio for molecular orbitals with opposite azimuthal quantum numbers $\ifmmode\pm\else\textpm\fi{}|m|$ (e.g., ${\ensuremath{\pi}}_{\ifmmode\pm\else\textpm\fi{}}$) is identical to that for atomic orbitals with the same $\ifmmode\pm\else\textpm\fi{}|m|$ (e.g., ${p}_{\ifmmode\pm\else\textpm\fi{}}$). In general, the electron counter-rotating to the CP laser field tunnels more easily, not only for atoms but also for linear molecules. Our theoretical predictions are then verified by numerically solving the three-dimensional time-dependent Schr\"odinger equation for the ionization of the prealigned nitric oxide (NO) molecule in strong CP laser fields. Due to the spin-orbital coupling in the electronic ground state of NO and the sensitivity of ionization to the sense of electron rotation, the ionization of NO in CP fields can produce spin-polarized photoelectrons with high controllability of spin polarization up to $100%$.