Time-dependent linear-response variational Monte Carlo - Sorbonne Université Accéder directement au contenu
Article Dans Une Revue Advances in Quantum Chemistry Année : 2017

Time-dependent linear-response variational Monte Carlo

Résumé

We present the extension of variational Monte Carlo (VMC) to the calculation of electronic excitation energies and oscillator strengths using time-dependent linear-response theory. By exploiting the analogy existing between the linear method for wave-function optimisation and the generalised eigenvalue equation of linear-response theory, we formulate the equations of linear-response VMC (LR-VMC). This LR-VMC approach involves the first-and second-order derivatives of the wave function with respect to the parameters. We perform first tests of the LR-VMC method within the Tamm-Dancoff approximation using single-determinant Jastrow-Slater wave functions with different Slater basis sets on some singlet and triplet excitations of the beryllium atom. Comparison with reference experimental data and with configuration-interaction-singles (CIS) results shows that LR-VMC generally outperforms CIS for excitation energies and is thus a promising approach for calculating electronic excited-state properties of atoms and molecules.
Fichier principal
Vignette du fichier
paper.pdf (289.64 Ko) Télécharger le fichier
Origine : Fichiers produits par l'(les) auteur(s)

Dates et versions

hal-01528081 , version 1 (26-05-2017)

Identifiants

Citer

Bastien Mussard, Emanuele Coccia, Roland Assaraf, Matt Otten, C. J. Umrigar, et al.. Time-dependent linear-response variational Monte Carlo. Advances in Quantum Chemistry, 2017, Novel Electronic Structure Theory: General Innovations and Strongly Correlated Systems. ⟨hal-01528081⟩
298 Consultations
108 Téléchargements

Altmetric

Partager

Gmail Facebook X LinkedIn More