This book presents the latest theoretical studies giving new predictions and interpretations on the quantum correlation in molecular dynamics induced by ultrashort laser pulses. The author quantifies the amount of correlation in terms of entanglement by employing methods developed in quantum information science, in particular applied to the photoionization of a hydrogen molecule. It is also revealed that the photoelectron–ion correlation affects the vibrational dynamics of the molecular ion and induces the attosecond-level time delay in the molecular vibration. Furthermore, the book also presents how molecular vibration can couple to photons in a plasmoic nanocavity. Physicists and chemists interested in the ultrafast molecular dynamics would be the most relevant readers. They can learn how we can employ the quantum-information-science tools to understand the correlation in the molecular dynamics and why we should consider the correlation between the photoelectron and the molecular ion to describe the ion’s dynamics. They can also learn how to treat a molecule coupled to photons in a nanocavity. All the topics are related to the state-of-the-art experiments, and so, it is important to publish these results to enhance the understanding and to induce new experiments to confirm the theory presented.

Despite decades of progress in quantum mechanics, electron correlation effects are still only partially understood. Experiments in which both electrons are ejected from an oriented hydrogen molecule by absorption of a single photon have recently demonstrated a puzzling phenomenon: The ejection pattern of the electrons depends sensitively on the bond distance between the two nuclei as they vibrate in their ground state. Here we report a complete numerical solution of the Schrodinger equation for the double photoionization of H2. The results suggest that the distribution of photoelectrons emitted from aligned molecules reflects electron correlation effects that are purely molecular in origin.

Pulsed field ionization (PFI) has been used in conjunction with coherent VUV radiation to investigate the rotational state distributions of molecular cations following single photon ionization. For photoionization of the H2X (X = O, S) molecules, transitions between asymmetric top levels involving the rotational angular momentum projections, K{sub a} and K{sub c}, permit resolution of the photoelectron continua according to symmetry. The observed spectra also clearly demonstrate the importance of the non-spherical nature of the molecular ion potential which leads to photoelectron final states which are unexpected from atomic-like analogies.

Part II. 13. Dissociative electron-ion recombination studies using ion synchrotrons / Mats Larsson -- 14. Dissociative photodetachment studies of transient molecules by coincidence techniques / R.E. Continetti -- 15. Mass selected anion-zero kinetic energy photoelectron spectroscopy / Ulrich Boesl, Carsten Bäßmann and Edward W. Schlag -- 16. Photodetachment photoelectron spectroscopy of transition metal oxide species / Lai-Sheng Wang -- 17. Detachment processes for molecular anions / Jack Simons -- 18. Competition between autoionization and predissociation in molecular Rydberg states / S.T. Pratt -- 19. Electron capture processes by free and bound molecules / Eugen Illenberger -- 20. Visualization of electron correlations in doubly and triply excited states of atoms / C.D. Lin and Toru Morishita -- 21. High-resolution angle-resolved studies of atoms and molecules using advanced electron spectroscopy at the ALS / Nora Berrah -- 22. X-ray scattering and fluorescence from atoms and molecules / S.H. Southworth [und weitere]