Artykuł w czasopiśmie
Brak miniatury
Licencja
ClosedAccessDostęp zamknięty
 

Explicitly Correlated Electronic Structure Calculations with Transcorrelated Matrix Product Operators

Uproszczony widok
cris.lastimport.scopus2024-02-12T18:58:52Z
dc.abstract.enn this work, we present the first implementation of the transcorrelated electronic Hamiltonian in an optimization procedure for matrix product states by the density matrix renormalization group (DMRG) algorithm. In the transcorrelation ansatz, the electronic Hamiltonian is similarity-transformed with a Jastrow factor to describe the cusp in the wave function at electron-electron coalescence. As a result, the wave function is easier to approximate accurately with the conventional expansion in terms of one-particle basis functions and Slater determinants. The transcorrelated Hamiltonian in first quantization comprises up to three-body interactions, which we deal with in the standard way by applying robust density fitting to two- and three-body integrals entering the second-quantized representation of this Hamiltonian. The lack of hermiticity of the transcorrelated Hamiltonian is taken care of along the lines of the first work on transcorrelated DMRG [ J. Chem. Phys. 2020, 153, 164115 ] by encoding it as a matrix product operator and optimizing the corresponding ground state wave function with imaginary-time time-dependent DMRG. We demonstrate our quantum chemical transcorrelated DMRG approach at the example of several atoms and first-row diatomic molecules. We show that transcorrelation improves the convergence rate to the complete basis set limit in comparison to conventional DMRG. Moreover, we study extensions of our approach that aim at reducing the cost of handling the matrix product operator representation of the transcorrelated Hamiltonian
dc.affiliationUniwersytet Warszawski
dc.contributor.authorReiher, Markus
dc.contributor.authorLesiuk, Michał
dc.contributor.authorBaiardi, Alberto
dc.date.accessioned2024-01-25T00:09:58Z
dc.date.available2024-01-25T00:09:58Z
dc.date.issued2022
dc.description.financeNie dotyczy
dc.description.number7
dc.description.volume18
dc.identifier.doi10.1021/ACS.JCTC.2C00167
dc.identifier.issn1549-9618
dc.identifier.urihttps://repozytorium.uw.edu.pl//handle/item/106793
dc.identifier.weblinkhttps://pubs.acs.org/doi/pdf/10.1021/acs.jctc.2c00167
dc.languageeng
dc.pbn.affiliationchemical sciences
dc.relation.ispartofJournal of Chemical Theory and Computation
dc.relation.pages4203-4217
dc.rightsClosedAccess
dc.sciencecloudnosend
dc.titleExplicitly Correlated Electronic Structure Calculations with Transcorrelated Matrix Product Operators
dc.typeJournalArticle
dspace.entity.typePublication