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Challenges in relativistic electronic structure calculations of gas-phase reactivity and thermodynamics of actinide species
Plutonium Futures 2020, Montpellier, 07-06-2020, 07-06-2020Communication dans un congrès avec actes -
Accurate Predictions of Volatile Plutonium Thermodynamic Properties
Inorganic Chemistry, American Chemical Society, 14-10-2019, 58, 14507-14521Compte-rendu et recension critique d'ouvragetexte intégral -
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 -
Theoretical modelling of optical and thermodynamical properties of actinide (U, Np, Pu,...) complexes
46th Conference of the European Group on Atomic Systems, Lille, 01-07-2014, 01-07-2014Autre communication scientifique (congrès sans actes - poster - séminaire...) -
Challenges in relativistic electronic structure calculations of gas-phase reactivity and thermodynamics of actinide species
International Workshop on Theory Frontiers in Actinide Sciences: Chemistry and Materials, Santa Fe, 02-02-2020, 02-02-2020 -
Apports de la modélisation théorique à la radiochimie moléculaire
2es Rencontres Rayonnement Radio-Chimie, Nice, 31-08-2022, 31-08-2022 -
Investigation of thermodynamics properties of gaseous plutonium oxides through a deep dive into electronic structure
Strasbourg satellite meeting to the 16th ICQC: Strong correlation in electronic structure theory, Strasbourg, 24-06-2018, 24-06-2018 -
Challenges in relativistic electronic structure calculations of gas-phase reactivity and thermodynamics of actinide species
Plutonium Futures: The Science 2022, Avignon, 26-09-2022, 26-09-2022 -
Relativistic correlated calculations of the thermodynamic properties of gaseous plutonium oxides
ISTCP IX 2016 Conference, Grand Forks, 17-07-2016, 17-07-2016Autre communication scientifique (congrès sans actes - poster - séminaire...) -
Investigation of the spectroscopic and thermodynamics properties of gaseous plutonium oxides
Workshop Excited States Simulations: Bridging Scales, Marseille, 07-11-2016, 07-11-2016Autre communication scientifique (congrès sans actes - poster - séminaire...)