Assessment of random phase approximation and second-order Moller-Plesset perturbation theory for many-body interactions in solid ethane, ethylene, and acetylene
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F23%3A10468450" target="_blank" >RIV/00216208:11320/23:10468450 - isvavai.cz</a>
Result on the web
<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=a9MV-xx9I" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=a9MV-xx9I</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1063/5.0142348" target="_blank" >10.1063/5.0142348</a>
Alternative languages
Result language
angličtina
Original language name
Assessment of random phase approximation and second-order Moller-Plesset perturbation theory for many-body interactions in solid ethane, ethylene, and acetylene
Original language description
The relative energies of different phases or polymorphs of molecular solids can be small, less than a kilojoule/mol. A reliable description of such energy differences requires high-quality treatment of electron correlations, typically beyond that achievable by routinely applicable density functional theory (DFT) approximations. At the same time, high-level wave function theory is currently too computationally expensive. Methods employing an intermediate level of approximations, such as Moller-Plesset (MP) perturbation theory and the random phase approximation (RPA), are potentially useful. However, their development and application for molecular solids has been impeded by the scarcity of necessary benchmark data for these systems. In this work, we employ the coupled-cluster method with singles, doubles, and perturbative triples to obtain a reference-quality many-body expansion of the binding energy of four crystalline hydrocarbons with a varying p-electron character: ethane, ethene, and cubic and orthorhombic forms of acetylene. The binding energy is resolved into explicit dimer, trimer, and tetramer contributions, which facilitates the analysis of errors in the approximate approaches. With the newly generated benchmark data, we test the accuracy of MP2 and non-self-consistent RPA. We find that both of the methods poorly describe the non-additive many-body interactions in closely packed clusters. Using different DFT input states for RPA leads to similar total binding energies, but the many-body components strongly depend on the choice of the exchange-correlation functional.
Czech name
—
Czech description
—
Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
—
OECD FORD branch
10403 - Physical chemistry
Result continuities
Project
—
Continuities
R - Projekt Ramcoveho programu EK
Others
Publication year
2023
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
Journal of Chemical Physics
ISSN
0021-9606
e-ISSN
1089-7690
Volume of the periodical
158
Issue of the periodical within the volume
14
Country of publishing house
US - UNITED STATES
Number of pages
18
Pages from-to
144119
UT code for WoS article
000971803700005
EID of the result in the Scopus database
—