Theories and Quantum Chemical Calculations of Linear and Sum-Frequency Generation Spectroscopies, and Intramolecular Vibrational Redistribution and Density Matrix Treatment of Ultrafast Dynamics
Journal
Advances in Chemical Physics
Journal Volume
156
Pages
295-391
ISBN
978-111894970-2
978-111894969-6
Date Issued
2014
Author(s)
Abstract
Recent rapid progress in quantum chemical calculations has made it possible to perform the first principle calculations of various molecular spectroscopies and photophysical processes. Anharmonic effect on molecular electronic absorption and luminescence like fluorescence and phosphorescence spectroscopies and electronic relaxation processes like internal conversion and intersystem crossing has been theoretically developed 10 years ago. This chapter reviews its applications to pyridine, pyrimdine, pyrazine, and fluorobenzene. It then presents the molecular theories of all types of sum-frequency generation (SFG) including both vibrational SFG (VSFG) and electronic SFG (ESFG). A couple of SFG examples based on the quantum chemical calculations are included for demonstration. The chapter presents how to perform the calculations of the intramolecular vibrational redistribution (IVR) for water clusters and amino acid molecules and their peptides. It applies the femto-second (fs) time-resolved density matrix method to treat the Bixon–Jortner (B-J) model which is a popular method for studying photophysical process.
Type
book part