Time-Dependent Multiconfiguration Theory and Its Application to Ultrafast Electronic Dynamics of Molecules in an Intense Laser Field(Invited papers of DCEN2011,Frontier Issues in Physics of Exotic Nuclei)
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概要
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We outlined a time-dependent multiconfiguration theory to describe electronic dynamics of molecules, where the many-electron wave function at time t, Φ(t), is expanded in terms of different electron configurations Φ_I(t) composed of time-dependent one-electron orbitals (spin-orbitals) as Φ(t)=Σ_IC_I(t)Φ_I(t). The equations of motion (EOMs) for spin-orbitals in coordinate representation are derived together with the EOMs for configuration interaction coefficients C_I(t). As an example of application to molecules, we presented the results of investigation of the ionization dynamics of H_2 interacting with a near-infrared intense laser filed. By extending the concept of Hartree-Fock orbital energy to multiconfiguration theory, we newly introduced the "molecular orbital energies" of natural spin-orbitals (NSOs) {j} of a many-electron system and defined the orbital potentials ε^^-_j(t) and correlation energies V^c_j(t) of NSOs. The total energy E(t) is decomposed into individual components as E(t)=Σ^^j_jω_j(t)ε^^-_j(t) as in thermodynamics, where ω_j(t) are the occupation numbers of {j}. We proved that this type of partition of the total energy is interpreted as the time-dependent chemical potential for the two-electron system. The newly defined correlation energy V^c_j(t) associated with the jth NSO, involved in ε^^-_j(t), reflects dynamical electron correlations on the attosecond timescale. We also compared the energy ζ_j(t) directly supplied by the applied field with the net energy gain Δε^^-_j(t) for respective natural orbitals. The responses of natural orbitals can be classified into three: Δε^^-_j(t)=ζ_j(t) (spectator orbital); Δε^^-_j(t)<ζ_j(t) (energy donor orbital); and Δε^^-_j(t)>ζ_j(t) (energy acceptor orbital). We found that ionization of H_2 most efficiently occurs from a time-developing energy acceptor NSO 2σ_g for the case of the present applied field. We concluded that energy acceptor natural orbitals play a key role in ionization processes.
- 2012-10-22
著者
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Kono Hirohiko
Department Of Chemistry Graduate School Of Science Tohoku University
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Kato Tsuyoshi
Department Of Chemistry Graduate School Of Science Tohoku University
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KOSEKI Shiro
Department of Chemistry, Graduate School of Science, Osaka Prefecture University
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