Global Management of Atmospheric Trace Gases – A Theoretical Approach –

Research Project , Research Report 2001

Kimihiko HIRAO Dept. of Applied Chemistry, the University 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 ETH Zurich, Laboratory of Physical Chemistry, Switzerland
Jeffrey STEINFELD 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”. We have developed the following theory; a multiconfigurational many-body perturbation theory (GMC-QDPT) where the parent electron configurations are selected in accordance with the character of a system, a regional self-interaction correction scheme that improves underestimated chemical reaction barriers in DFT calculations, a high-speed computational algorithm of the 4-component Dirac equation, and so forth. (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 based on ab initio quantum chemical methods and the density functional perturbation theory (DFPT). (3) We report semiclassical energy spectra of vibrational state of a cluster composed of 7 identical atoms in terms of our previously developed semiclassical wave function, which we call the action-decomposed function. The classical dynamics of this vibrational state is strongly chaotic and undergoes a large amplitude motion due to structural isomerization, which demands a long run of trajectory calculation.

Keywords:

Next-generation molecular theory, Theoretical chemistry program package “UTChem”, interlayer dielectrics, low-k materials, cluster, vibrational spectrum, chaos