Multi-Level Coupled-Cluster Description of Crystal Lattice Energies

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F25%3A10510886" target="_blank" >RIV/00216208:11320/25:10510886 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=k5Ln-n63TY" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=k5Ln-n63TY</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jctc.5c00428" target="_blank" >10.1021/acs.jctc.5c00428</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Multi-Level Coupled-Cluster Description of Crystal Lattice Energies

Popis výsledku v původním jazyce

The many-body expansion (MBE) of the lattice energy enables an ab initio description of molecular solids using correlated wave function approximations. However, the practical application of MBE requires computing the large number of n-body contributions efficiently. To this end, we employ a multi-level coupled-cluster approach which adapts the approximation level based on interaction type and intermolecular distance. The high-level method, including connected triple excitations, is applied only to monomer relaxation and dimer interactions roughly within the first and second coordination shells. Long-range dimers and trimers are treated using a simplified coupled-cluster description based on the random-phase approximation (RPA). A key feature is an energy correction which mitigates the underbinding error of the base RPA. Convergence to the bulk limit is accelerated by the addition of the periodic Hartree-Fock correction. The proposed approach is validated against recent diffusion Monte Carlo reference data for the X23 data set, achieving a mean absolute error of 3.1 kJ/mol, i.e., chemical accuracy for absolute lattice energies.

Název v anglickém jazyce

Multi-Level Coupled-Cluster Description of Crystal Lattice Energies

Popis výsledku anglicky

The many-body expansion (MBE) of the lattice energy enables an ab initio description of molecular solids using correlated wave function approximations. However, the practical application of MBE requires computing the large number of n-body contributions efficiently. To this end, we employ a multi-level coupled-cluster approach which adapts the approximation level based on interaction type and intermolecular distance. The high-level method, including connected triple excitations, is applied only to monomer relaxation and dimer interactions roughly within the first and second coordination shells. Long-range dimers and trimers are treated using a simplified coupled-cluster description based on the random-phase approximation (RPA). A key feature is an energy correction which mitigates the underbinding error of the base RPA. Convergence to the bulk limit is accelerated by the addition of the periodic Hartree-Fock correction. The proposed approach is validated against recent diffusion Monte Carlo reference data for the X23 data set, achieving a mean absolute error of 3.1 kJ/mol, i.e., chemical accuracy for absolute lattice energies.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Journal of Chemical Theory and Computation

ISSN

1549-9618

e-ISSN

1549-9626

Svazek periodika

21

Číslo periodika v rámci svazku

11

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

12

Strana od-do

5533-5544

Kód UT WoS článku

001498871600001

EID výsledku v databázi Scopus

2-s2.0-105006802647