Academic Journal
Multiconfigurational short-range density-functional theory for open-shell systems
| العنوان: | Multiconfigurational short-range density-functional theory for open-shell systems |
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| المؤلفون: | Hedegård, Erik, Donovan, Toulouse, Julien, Jensen, Hans Jørgen, Aa. |
| المساهمون: | Department of Theoretical Chemistry, Skane University Hospital Lund, Laboratoire de chimie théorique (LCT), Institut de Chimie - CNRS Chimie (INC-CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Department of Physics, Chemistry, and Pharmacy, University of Southern Denmark (SDU) |
| المصدر: | ISSN: 0021-9606. |
| بيانات النشر: | HAL CCSD American Institute of Physics |
| سنة النشر: | 2018 |
| مصطلحات موضوعية: | range-separated DFT, MCSCF, open shells, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], [PHYS.PHYS.PHYS-COMP-PH]Physics [physics]/Physics [physics]/Computational Physics [physics.comp-ph] |
| الوصف: | International audience ; Many chemical systems cannot be described by quantum chemistry methods based on a singlereference wave function. Accurate predictions of energetic and spectroscopic properties require a delicate balance between describing the most important configurations (static correlation) and obtaining dynamical correlation efficiently. The former is most naturally done through a multiconfigurational (MC) wave function, whereas the latter can be done by, e.g., perturbation theory. We have employed a different strategy, namely, a hybrid between multiconfigurational wave functions and density functional theory (DFT) based on range separation. The method is denoted by MC short-range DFT (MC–srDFT) and is more efficient than perturbative approaches as it capitalizes on the efficient treatment of the (short-range) dynamical correlation by DFT approximations. In turn, the method also improves DFT with standard approximations through the ability of multiconfigurational wave functions to recover large parts of the static correlation. Until now, our implementation was restricted to closed-shell systems, and to lift this restriction, we present here the generalization of MC–srDFT to open-shell cases. The additional terms required to treat open-shell systems are derived and implemented in the DALTON program. This new method for open-shell systems is illustrated on dioxygen and [Fe(H2O)6]3+ . |
| نوع الوثيقة: | article in journal/newspaper |
| اللغة: | English |
| Relation: | info:eu-repo/semantics/altIdentifier/arxiv/1711.03882; hal-01832349; https://hal.sorbonne-universite.fr/hal-01832349; https://hal.sorbonne-universite.fr/hal-01832349/document; https://hal.sorbonne-universite.fr/hal-01832349/file/srdft_open_shell.pdf; ARXIV: 1711.03882 |
| DOI: | 10.1063/1.5013306 |
| الاتاحة: | https://hal.sorbonne-universite.fr/hal-01832349 https://hal.sorbonne-universite.fr/hal-01832349/document https://hal.sorbonne-universite.fr/hal-01832349/file/srdft_open_shell.pdf https://doi.org/10.1063/1.5013306 |
| Rights: | info:eu-repo/semantics/OpenAccess |
| رقم الانضمام: | edsbas.CC3E34C7 |
| قاعدة البيانات: | BASE |
| DOI: | 10.1063/1.5013306 |
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