Global Management of Atmospheric Trace Gases – A Theoretical Approach –

Research Project , Research Report 2002

Kimihiko HIRAO Dept. of Applied Chemistry, The Univ. of Tokyo
Koichi YAMASHITA Dept. of Chem. Sys. Engineering, The Univ. of Tokyo,
Kazuo TAKATSUKA Graduate School of Arts and Sciences, The Univ. of Tokyo(Research Partners)
Martin QUACK Professor, ETH Zurich, Laboratory of Physical Chemistry, Switzerland
Jeffrey STEINFELD Professor, Department of Chemistry, MIT, USA

Abstract

In order to understand the electronic, dynamics and spectroscopic features of trace gases in the atmosphere, we have performed the following projects: (1) We construct next-generation molecular theory for real systems, and develop an integrative theoretical chemistry program package, “UTChem”. The code has been applied to the analysis of the neutral-ion phase transitions in a charge transfer complex and the adsorption of organic molecules on Fe and Au surfaces. (2) Propagation delay of signals by interlayer dielectrics in LSI interconnects is becoming a dominant issue. Materials of low dielectric constant have been widely studied in order to reduce the delay of signals. In this study we try to design theoretically novel low-k materials of carbon nitrides. (3) We have developed an extension of our formulation of energy- an angle-resolved photoelectron spectra for femtosecond pump-probe ionization of wavepackets to nonadiabatically coupled states and present results of its applications to wavepacket motion on the ionic (Na+I-) and covalent (NaI) states of sodium iodide. The results of these studies suggest that the energy and angular distributions of these photoelectron spectra provide a useful mapping of the bifurcation of the wavepackets through the crossing region and a valuable window on the intramolecular electron transfer occurring between the covalent and ionic states.

Keywords:

Next-generation molecular theory, Theoretical chemistry program package “UTChem”, interlayer dielectrics, low-k materials, femtosecond pump-probe ionization, intramolecular electron transfer