Multiconfiguration time-dependent theory

Joubert-Doriol L, Lasome B, Gatti F, Schroder M, Vendrell O, Meyer H-D (2012) Suitable coordinates for quantum dynamics applications using the multiconfiguration time-dependent Hartree (MCTDH) algorithm. Comput Theor Chem 990 75-89 Chemical reactivity, from accurate theories to simple models, in honor of Professor Jean-Claude Rayez... 

Chapter 3 treats nuclear motions on the adiabatic potential energy surfaces (PES). One of the most powerful and simplest means to study chemical dynamics is the so-called ab initio molecular dynamics (or the first principle dynamics), in which nuclear motion is described in terms of the Newtonian d3mamics on an ab initio PES. Next, we review some of the representative time-dependent quantum theory for nuclear wavepackets such as the multiconfigurational time-dependent Hartree approach. Then, we show how such nuclear wavepacket d3mamics of femtosecond time scale can be directly observed with pump>-probe photoelectron spectroscopy. 

Wang H, Thoss M (2003) Multilayer formulation of the multiconfiguration time-dependent Haitree theory. J Chem Phys 119 1289-1299... 

The three-pulse EOM-PMA can be formulated not only in terms of density matrices and master equations but also in terms of wavefunctions and Schrodinger equations [29]. The EOM-PMA can therefore be straightforwardly incorporated into computer programs which provide the time evolution of the density matrix or the wavefunction of material systems. Besides the multilevel Redlield theory, the EOM-PMA can be combined with the Lindblad master equation [49], the surrogate Hamiltonian approach [49], the stochastic Liouville equation [18], the quantum Fokker-Planck equation [18], and the density matrix [50] or the wavefunction [14] multiconfigurational time-dependent Hartree (MCTDH) methods. When using the... 

Olsen J and J0rgensen P 1995 Time-dependent response theory with applications to self-consistent field and multiconfigurational self-consistent field wave functions Modern Electronic Structure Theory vo 2, ed D R Yarkony (Singapore World Scientific) pp 857-990... 

The time dependence of the molecular wave function is carried by the wave function parameters, which assume the role of dynamical variables [19,20]. Therefore the choice of parameterization of the wave functions for electronic and nuclear degrees of freedom becomes important. Parameter sets that exhibit continuity and nonredundancy are sought and in this connection the theory of generalized coherent states has proven useful [21]. Typical parameters include molecular orbital coefficients, expansion coefficients of a multiconfigurational wave function, and average nuclear positions and momenta. We write... 

J. Olsen and P. Jorgensen. Time-Dependent Response Theory with Applications to Self-Consistent Field and Multiconfigurational Self-Consistent Field Wave Functions, in Modern Electronic Structure Theory, edited by D. R. Yarkony, volume 2, chapter 13, pp. 857-990. World Scientific, Singapore, 1995. 

Olsen, J., lorgcnsen, P. Time dependent response theory with appUcations in to self consistence field (SCF and multiconfigurational self consistent field (MCSCF) wave functions, l.F.A. PRINT, Aarhus Universitet, 1994... 

The excited-state quantum chemical methods used in the research presented in this chapter are based on time-dependent density functional theory (TD-DFT) [61, 62] or multiconfigurational ab initio theory. Since many excellent reviews of these... 

T. Kato, H. Kono, Time-dependent multiconfiguration theory for electronic dynamics of molecules in an intense laser field, Chem. Phys. Lett. 392 (2004) 533. 

The linear response methods offer a viable alternative to the Cl procedure [38]. A time-dependent (TD) perturbation theory (e.g. involving an oscillating electric field), combined with the SCF or MCSCF method is referred to as the TD-SCF (or random phase approximation, RPA) or the TD-MCSCF (or multiconfigurational linear response, MCLR), respectively. Let us consider the time development of the dipole moment (z-component for simplicity) ... 

E. Dalgaard,. Chem. Phys., 72, 816 (1980). Time-Dependent Multiconfigurational Hartree-Fock Theory. 

As in the Hartree-Fock molecular orbital theory, which is based on the independent particle model, the above Hartree product method also lacks enough correlation among the orbitals, and thereby the resultant accuracy is limited. To overcome the drawback, one can take account of the interaction among possible configurations (or the Hartree products) as in the configuration interaction method and multiconfiguration SCF methods in electronic structure theory. The multiconfigulational time-dependent Hartree... 

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