Download or read book Probing Ultrafast Dynamics of Photo-initiated Events Using Molecular-frame Electron Angular Distributions written by Shungo Miyabe and published by . This book was released on 2010 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: This thesis will show how the photo-induced fragmentation of molecules into neutrals, ions and electrons can probe molecular and electronic dynamics through combination of ab initio theory with detailed momentum imaging experiments. We report the results of ab initio calculations of cross sections and molecular-frame photoelectron angular distributions for C 1s ionization of CO2 and propose a mechanism for the recently observed asymmetry of those angular distributions with respect to the CO and O ions produced by subsequent Auger decay. The results presented here will show how the Auger decay can be used to probe ultrafast molecular dynamics of the transient molecule. We have also discovered the appearance of vibrational Feshbach resonances in photodetachment of HOCO− that demonstrates how the photoelectron kinetic energy measurements can be used to deduce the properties of dipole-bound anion. Finally, we report the precise quantum mechanical calculations of body-frame photoelectron angular distributions for double photoionization of H2 that identifies the true diffractive energy regime in the smallest molecular two-slit experiment imaginable. In this particular case it is the knowledge of the orientation that makes the discussion of angular diffraction effects possible, demonstrating the unique qualities of this powerful momentum imaging techniques.