ABSTRACT

Constructing experiments capable of performing time-resolved measurements of quantum dynamics is a formidable task. This chapter examines two incoherent approaches for measuring vibrational dynamics in one dimension: laser-induced fluorescence (LIF) and time-resolved ionization spectroscopy. It discusses of how one measures electron dynamics in atomic and molecular systems, focusing on examples that can be thought of as one dimensional. The chapter considers using LIF to measure dynamics in a one-dimensional system where there is coupling between two (adiabatic) potential energy surfaces (PES). In contrast with LIF, the probe pulse does not interact with the molecule directly, but instead is used to “gate” the fluorescence from the excited PES through a nonlinear interaction separate from the molecular sample. As with LIF, a pump pulse launches a vibrational wave packet on an excited PES. The primary difference as compared to LIF is that the final state is in the electronic continuum, leading to a molecular cation and an emitted electron.