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Exploring the dynamic and thermodynamic properties of halides through molecular dynamics simulations
257th American Chemical Society National Meeting, Orlando, 31-01-2019, 31-03-2019 -
Predictive simulations of ionization energies of solvated halide ions with relativistic embedded Equation of Motion Coupled-Cluster Theory
PHYSICAL REVIEW LETTERS, American Physical Society, 28-12-2018, 121, 266001Compte-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 -
Predicting solvent effects on the photoelectron spectra of halide ions with WFT-in-DFT embedding
1res Journées Scientifiques du GDR 2035 SolvATE, Nancy, 16-05-2018, 16-05-2018 -
Electronic states of (ultra) heavy halogen species with four-component based equation of motion coupled cluster methods
MESM2018 Molecular Electronic Structure, Metz, 28-08-2018, 28-08-2018 -
Exploration of excited, electron attachment and detachment states of (ultra)heavy halogen species with relativistic 4-component EOM-CC methods
12th International Conference on Relativistic Effects in Heavy-Element Chemistry and Physics, Marburg, 02-09-2017, 02-09-2017 -
Relativistic Coupled Cluster theory for the Calculation of Ground and Excited State Energies and Molecular Properties
19th DIRAC Working Group Meeting 2016, Odensee, 29-05-2016, 30-05-2016 -
Equation-of-Motion Coupled-Cluster Theory based on the 4-component Dirac-Coulomb(-Gaunt) Hamiltonian. Energies for single electron detachment, attachment and electronically excited states
The Journal of Chemical Physics, American Institute of Physics, 07-11-2018, 149, 174113Compte-rendu et recension critique d'ouvragetexte intégral -
The DIRAC code for relativistic molecular calculations
The Journal of Chemical Physics, American Institute of Physics, 26-05-2020, 152, 204104Compte-rendu et recension critique d'ouvragetexte intégral -
Relativistic EOM-CCSD for core-excited and core-ionized state energies based on the 4-component Dirac-Coulomb(-Gaunt) Hamiltonian
Journal of Chemical Theory and Computation, American Chemical Society, 04-05-2021, 17; 6, 3583-3598Compte-rendu et recension critique d'ouvragetexte intégral