Theory of nuclear motion in RABBITT spectra

Abstract

Reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) is a powerful photoelectron spectroscopy, offering direct access to internal dynamics of the target. It is being increasingly applied to molecular systems, but a general, computationally tractable theory of RABBITT spectra in molecules has so far been lacking. We show that under quite general assumptions, RABBITT spectra in molecules can be expressed as a convolution of the vibronic cross-correlation functions and two-electron photoionization matrix elements. We specialize the general expressions to the commonly-encountered special cases. We expect our theory to enable accurate modeling and interpretation of molecular RABBITT spectra in most medium-sized molecules.