Time-resolved photoelectron angular distributions as a probe of intramolecular dynamics: Connecting the molecular frame and the laboratory frame

A formalism is presented in which the laboratory frame photoelectron angula r distribution (PAD) is expressed as a convolution of the molecular frame P AD with the laboratory frame molecular axis distribution. Molecular and lab oratory frame PADs are discussed in the context of probing intramolecular d ynamics in the time domain. Model calculations for a C-3v molecule are pres ented as an illustration of the differences between measurements in these t wo reference frames, and the effect of the degree of molecular alignment up on the laboratory frame measurements. Different symmetries of the orbital u ndergoing ionization are also considered in order to illustrate the sensiti vity of PADs to nonadiabatic processes. (C) 2000 American Institute of Phys ics. [S0021-9606(00)01327-1].