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Towards systematically improvable models for actinides in condensed phase: the electronic spectrum of uranyl in Cs2UO2Cl4 as a test case.
Physical Chemistry Chemical Physics, Royal Society of Chemistry, 21-08-2013, 15; 36, 15153-62Compte-rendu et recension critique d'ouvrage -
Molecules in condensed phase, the ab initio way: using embedding methods to calculate local properties of large-scale systems
Réunion du GDR2758 ``Agrégation, fragmentation et thermodynamique de systèmes moléculaires complexes isolés'', Toulouse, 01-11-2009, 01-11-2009 -
Modeling the Spectra of Heavy Elements in Condensed Phase Using WFT-in-DFT and DFT-in-DFT Embedding
7th Molecular Quantum Mechanics, Lugano, 02-06-2013, 02-06-2013Autre communication scientifique (congrès sans actes - poster - séminaire...) -
Electronic structure of actinide systems from relativistic correlated and quantum embedding approaches
Topical meeting on Condensed-Matter Chemistry on Actinides: The Kumatori meeting 2021, Kyoto, 10-02-2021, 10-02-2021 -
Benchmarking Electronic Structure Calculations on the Bare UO<sub>2</sub><sup>2+</sup> ion: How Different are Single and Multireference Electron Correlation Methods?
Journal of Physical Chemistry A, American Chemical Society, 16-07-2009, 113, 12504---12511Compte-rendu et recension critique d'ouvrage -
Methods based on the coupled cluster ansatz and employing four-component Hamiltonians are particularly appealing in treating the electronic structure of molecules containing heavy centers, due to their ecient treatment of electron correlation and spin-orbit coupling (SOC) [1] on the same footing, up to and including the superheavy elements, as well as to serve as benchmark to more approximate relativistic Hamiltonians, notably those where SOC is treated more approximately (see for instance [2] and references therein).In this contribution we discuss our recent implementation [3] in the Dirac program [4] of the equation of motion coupled cluster method for excitation energies (EOM-EE-CCSD), single electron attachment (EOM-EA-CCSD) and single electron detachment (EOM-IPCCSD). We showcase the method by addressing the determination of the low-lying statesof oxide radicals of group 17 elements (XO, X = Cl, Br, I, At, Ts), the excited and ionized states of the PuO<sub>2</sub> molecule in the gas phase [5], as well as the ionization energies of halide ions in water droplets [6]. In the latter case, we use the frozen density embedding approach to combine EOM-IP-CCSD (for the halogens) and the SAOP model potential (for the water molecules) to determine the ionization energies for the complete halide droplet system, while sampling different nuclear configurations with snapshots obtained from classical molecular dynamics simulations with polarizable force fields [7].This work has been supported by the French national agency for research, contract ANR-11-LABX-0005 chemical and physical properties of the atmosphere (CaPPA).<b>References</b>1. T. Fleig, Chem. Phys., 2 (2012) 395 ; T. Saue, ChemPhysChem, 12 (2011) 30772. E. Epifanovsky et al, J. Phys. Chem., 143 (2015) 064102 ; Z. Cao, Z. Li, F. Wang,W. Liu, Phys. Chem. Chem. Phys., 19 (2017) 3713 ; L. Cheng, F. Wang, J. F. Stanton,J. Gauss, J. Phys. Chem., 148 (2018) 0441083. A. Shee, T. Saue, L. Visscher, A. S. P. Gomes, J. Phys. Chem., 149 (2018) 1741134. http://diracprogram.org5. S. Kervazo, F. Real, F. Virot, A. S. P. Gomes, V. Vallet arXiv:1906.03157 (2019)6. Y. Bouchafra, A. Shee, F. Real, V. Vallet, A. S. P. Gomes Phys. Rev. Lett., 121 (2018)2660017. F. Real et al, J. Chem. Phys., 144, (2016) 124513
ISTCP 2019 - 10th Triennial Congress of the International Society for Theoretical Chemical Physics, Tromsø, 11-07-2019, 11-07-2019 -
Modeling the Spectra of Heavy Elements in Condensed Phase Using WFT-in-DFT and DFT-in-DFT Embedding
48th Symposium on Theoretical Chemistry (STC 2012), Karlsruhe, 23-09-2012, 23-09-2012Autre communication scientifique (congrès sans actes - poster - séminaire...)