Dipole-laser coupling delay in two-color (RABBITT) photoionization of polar molecules

TL;DR

This paper develops a theoretical approach to analyze how dipole-laser coupling affects RABBITT photoionization delays in polar molecules, revealing significant effects at low energies and extending existing models.

Contribution

It extends the time-independent molecular R-matrix method to include IR-dressed initial states, improving agreement with non-perturbative simulations for polar molecules.

Findings

Dipole-laser coupling significantly affects sideband delays at low photon energies.

The extended method matches well with time-dependent RABBITT simulations.

In negative ions, sideband delay is proportional to Wigner delay.

Abstract

We study theoretically the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) in strongly polar molecules. The time-dependent energy of a polar molecule in the infrared (IR) field gives rise to an additional dipole-laser coupling contribution to the sideband delay. In a time-independent picture this translates to the initial state becoming a linear combination of IR-dressed states. We extend the recently developed time-independent molecular R-matrix method to include the additional interfering ionization pathways arising from the IR-dressed initial state and obtain very good agreement with a reference non-perturbative time-dependent RABBITT simulation. We discuss the asymptotic behaviour of such ionization amplitudes and recover a known approximate asymptotic formula for the dipole-laser coupling delay derived earlier in the context of attosecond streaking. At low photon energies the dipole-laser coupling contributes significantly even in an unoriented molecular sample. Finally, we show that in photodetachment of polar singly charged negative ions the sideband delay is asymptotically proportional only to Wigner delay.