Sum-of-products form of the molecular electronic Hamiltonian and application within the MCTDH method

Abstract

We introduce two different approaches to represent the second-quantized electronic Hamiltonian in a sum-of-products form. These procedures aim at mitigating the quartic scaling of the number of terms in the Hamiltonian with respect to the number of spin orbitals, and thus enable applications to larger molecular systems. Here we describe the application of these approaches within the multi-configuration time-dependent Hartree framework. This approach is applied to the calculation of eigen energies of LiH and electronic ionization spectrum of H2O.

13 pages, 7 Figures. Accepted in J. Chem. Phys

References in corpus (7)

• The density-matrix renormalization group in the age of matrix product states
• From density-matrix renormalization group to matrix product states
• Multilayer multi-configuration time-dependent Hartree method: implementation and applications to a Henon-Heiles Hamiltonian and to pyrazine
• The multi-configurational time-dependent Hartree method for bosons: Many-body dynamics of bosonic systems
• Multiconfiguration time-dependent Hartree impurity solver for nonequilibrium dynamical mean-field theory
• Non-adiabatic quantum dynamics without potential energy surfaces based on second-quantized electrons: application within the framework of the MCTDH method
• The multi-configurational time-dependent Hartree approach in optimized second quantization: imaginary time propagation and particle number conservation

Cited by in corpus (1)

• Compact sum-of-products form of the molecular electronic Hamiltonian based on canonical polyadic decomposition