Multidimensional Analysis of Time-Resolved Charged Particle Imaging Experiments

Abstract

We present a tutorial to realize a multidimensional fitting procedure capable of extracting all the relevant information contained in a sequence of charged particle images acquired as a function of time in femtosecond pump–probe experiments. The images are reproduced using a 3D fitting method, which provides the velocity (or center-of-mass kinetic energy) and angular distributions contained in the images and their time evolution. A detailed example of the method is shown through the analysis of the time-resolved predissociation dynamics of CH3I on the B-band origin (Gitzinger et al., J. Chem. Phys.2010, 133, 234313). We show that the multidimensional approach is essential for the analysis of complex images that contain several overlapping contributions where reduced dimensionality analyses cannot provide a reliable description of the features present in the image sequence. This methodology can be generalized to many types of multidimensional data analysis.