Dual vibration configuration interaction (DVCI). An efficient factorization of molecular Hamiltonian for high performance infrared spectrum computation

Abstract

Here is presented an original program based on molecular Schrodinger equations. It is dedicated to target specific states of infrared vibrational spectrum in a very precise way with a minimal usage of memory. An eigensolver combined with a new probing technique accumulates information along the iterations so that desired eigenpairs rapidly tend towards the variational limit. Basis set is augmented from the maximal components of residual vectors that usually require the construction of a big matrix block that here is bypassed with a new factorisation of the Hamiltonian. The latest borrows the mathematical concept of duality and the second quantization formalism of quantum theory.

Added benchmarks with PyVCI_VPT2, explanations on the construction of the pruned space and more references

References in corpus (3)

• Calculating vibrational spectra with sum of product basis functions without storing full-dimensional vectors or matrices
• Vibrational Density Matrix Renormalization Group
• Calculating vibrational spectra of molecules using tensor train decomposition

Cited by in corpus (2)

• Low-rank Riemannian eigensolver for high-dimensional Hamiltonians
• Benchmarking vibrational spectra: 5000 accurate eigenstates of acetonitrile using tree tensor network states