PROJECTS

Ab initio electron dynamics with the multi-configuration (explicitly) time-dependent Hartree-Fock (MCTDHF) method

PRINCIPAL INVESTIGATOR

Prof. Dr. Peter Saalfrank Universität Potsdam Theoretische Chemie Karl-Liebknecht-Straße 24-25 D-14476 Golm +49(0)331-977-5232 petsaal@rz.uni-potsdam.de

TOGETHER WITH

ABSTRACT

During the first application period the Multi-Configuration Time-Dependent Hartree-Fock (MCTDHF) method was implemented and applied to one dimensional model problems, using a grid basis to also be able to treat unbound electron motion. A variety of algorithmic developments and coding were carried through. The MCTDHF method is applicable to explicitly time-dependent problems, systematically improvable, and contains the TD-HF (Time-Dependent HF) and TD-FCI (Time-Dependent Full Configuration Interaction) methods as two limits. Other TD-CI methods, such as TD-CIS (Time-Dependent CI Singles) can be viewed as special variants of MCTDHF, and were also further developed and applied within this project. In particular TD-CIS was implemented within an LCAO-MO form to treat real-world molecules in three dimensions.
It is the prime goal of the present proposal to also adapt the multi-configuration time-dependent Hartree-Fock (MCTDHF) method for realistic, three-dimensional systems. Another goal is to accelerate the program by algorithmic improvements. After this methodological work, we plan several applications in the realm of “femtosecond" and “attosecond" electron dynamics: (i) The calculation of cross sections for multiple ionization of atoms and molecules in strong laser fields; (ii) the calculation of cross sections for electron scattering and (iii) the relaxation of excited electron configurations via electron-electron scattering.

PUBLICATIONS

P. Krause, T. Klamroth, P. Saalfrank,
Time-dependent configuration interaction calculations of laser-pulse
driven many electron dynamics: Controlled dipole switching in lithium cyanide
J. Chem. Phys. submitted.

M. Nest, T. Klamroth,
Correlated many electron dynamics: Application to inelastic electron
scattering at a metal film
Phys. Rev. A, accepted.

P. Saalfrank, T. Klamroth, C. Huber, P. Krause,
Laser-driven electron dynamics at interfaces
Isr. J. Chem. (2005) (in press).

M. Nest, T. Klamroth, P. Saalfrank,
The multiconfiguration time-dependent Hartree-Fock method for
quantum chemical calculations
J. Chem. Phys. 122, 124102 (2005).