Unraveling actinide–actinide bonding in fullerene cages: a DFT versus ab initio methodological study
Identifikátory výsledku
Kód výsledku v IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388963%3A_____%2F23%3A00578866" target="_blank" >RIV/61388963:_____/23:00578866 - isvavai.cz</a>
Nalezeny alternativní kódy
RIV/00216208:11310/23:10478969
Výsledek na webu
<a href="https://doi.org/10.1039/D3CP03606E" target="_blank" >https://doi.org/10.1039/D3CP03606E</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1039/d3cp03606e" target="_blank" >10.1039/d3cp03606e</a>
Alternativní jazyky
Jazyk výsledku
angličtina
Název v původním jazyce
Unraveling actinide–actinide bonding in fullerene cages: a DFT versus ab initio methodological study
Popis výsledku v původním jazyce
Actinide-actinide bonding poses a challenge for both experimental and theoretical chemists because of both the scarcity of experimental data and the exotic nature of actinide bonding due to the involvement and mixing of actinide 7s-, 6p-, 6d-, and particularly 5f-orbitals. Only a few experimental examples of An-An bonding have been reported so far. Here, we perform a methodological study of actinide-actinide bonding on experimentally known Th2@C80 and U2@C80 systems. We compared selected GGA, meta-GGA, hybrid-GGA and range-separated hybrid-GGA functionals with the results obtained using a multireference CASPT2 method, which we consider as a reference point. We show that functionals such as BP86, PBE or TPSS perform well for predicting geometries, while range-separated hybrids are superior in the description of the chemical bonding. None of the tested functionals were deemed reliable regarding the correct electronic spin ground state. Based on the results of this methodological study, we re-evaluate selected previously studied diactinide fullerene systems using more reliable protocol.
Název v anglickém jazyce
Unraveling actinide–actinide bonding in fullerene cages: a DFT versus ab initio methodological study
Popis výsledku anglicky
Actinide-actinide bonding poses a challenge for both experimental and theoretical chemists because of both the scarcity of experimental data and the exotic nature of actinide bonding due to the involvement and mixing of actinide 7s-, 6p-, 6d-, and particularly 5f-orbitals. Only a few experimental examples of An-An bonding have been reported so far. Here, we perform a methodological study of actinide-actinide bonding on experimentally known Th2@C80 and U2@C80 systems. We compared selected GGA, meta-GGA, hybrid-GGA and range-separated hybrid-GGA functionals with the results obtained using a multireference CASPT2 method, which we consider as a reference point. We show that functionals such as BP86, PBE or TPSS perform well for predicting geometries, while range-separated hybrids are superior in the description of the chemical bonding. None of the tested functionals were deemed reliable regarding the correct electronic spin ground state. Based on the results of this methodological study, we re-evaluate selected previously studied diactinide fullerene systems using more reliable protocol.
Klasifikace
Druh
J<sub>imp</sub> - Článek v periodiku v databázi Web of Science
CEP obor
—
OECD FORD obor
10403 - Physical chemistry
Návaznosti výsledku
Projekt
<a href="/cs/project/GA21-17806S" target="_blank" >GA21-17806S: Endohedrální fullereny pro molekulární součástky: Memristory a spinristory</a><br>
Návaznosti
I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace
Ostatní
Rok uplatnění
2023
Kód důvěrnosti údajů
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Údaje specifické pro druh výsledku
Název periodika
Physical Chemistry Chemical Physics
ISSN
1463-9076
e-ISSN
1463-9084
Svazek periodika
25
Číslo periodika v rámci svazku
45
Stát vydavatele periodika
GB - Spojené království Velké Británie a Severního Irska
Počet stran výsledku
14
Strana od-do
31500-31513
Kód UT WoS článku
001104999800001
EID výsledku v databázi Scopus
2-s2.0-85176803302