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Title: Solid Oganesson via a Many-Body Interaction Expansion Based on Relativistic Coupled-Cluster Theory and from Plane-Wave Relativistic Density Functional Theory

Abstract

In this work, many-body potentials up to fourth order in the expansion are constructed using non-relativistic, scalar-relativistic and relativistic coupled-cluster theory to accurately describe the interaction between superheavy oganesson atoms. The obtained distance dependent energy values were fitted to extended two-body Lennard-Jones and three-body Axilrod-Teller-Muto potentials, with the fourth-order term treated through a classical long-range Drude dipole interaction model. From these interac tion potentials, spectroscopic constants for the oganesson dimer and solid state properties were obtained. Furthermore, these high-level results are compared to scalar relativistic and two-component plane-wave DFT calculations based on a tailor-made projector augmented-wave pseudopotential (PAW-PP) and newly derived parameters for Grimme’s dispersion correction. It is shown that the functionals PBE-D3(BJ), PBEsol and in particular SCAN provide excellent agreement with the many-body ref erence for solid Og. Finally, the results for Og are compared and related to the lighter rare gas elements and periodic trends are discussed.

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [3]; ORCiD logo [2]
  1. Max-Planck-Inst. für Kohlenforschung (KOFO), Mülheim an der Ruhr (Germany)
  2. Massey Univ. Auckland (New Zealand)
  3. Washington State Univ., Pullman, WA (United States)
Publication Date:
Research Org.:
Washington State Univ., Pullman, WA (United States)
Sponsoring Org.:
Royal Society of New Zealand Te Apārangi; Alexander-von-Humboldt Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1611062
Grant/Contract Number:  
SC0008501; 17-MAU-021; FG02-12ER16329
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 123; Journal Issue: 19; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Physics; Elements; Energy; Chemical calculations; Lattices

Citation Formats

Jerabek, Paul, Smits, Odile R., Mewes, Jan-Michael, Peterson, Kirk A., and Schwerdtfeger, Peter. Solid Oganesson via a Many-Body Interaction Expansion Based on Relativistic Coupled-Cluster Theory and from Plane-Wave Relativistic Density Functional Theory. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.jpca.9b01947.
Jerabek, Paul, Smits, Odile R., Mewes, Jan-Michael, Peterson, Kirk A., & Schwerdtfeger, Peter. Solid Oganesson via a Many-Body Interaction Expansion Based on Relativistic Coupled-Cluster Theory and from Plane-Wave Relativistic Density Functional Theory. United States. https://doi.org/10.1021/acs.jpca.9b01947
Jerabek, Paul, Smits, Odile R., Mewes, Jan-Michael, Peterson, Kirk A., and Schwerdtfeger, Peter. Wed . "Solid Oganesson via a Many-Body Interaction Expansion Based on Relativistic Coupled-Cluster Theory and from Plane-Wave Relativistic Density Functional Theory". United States. https://doi.org/10.1021/acs.jpca.9b01947. https://www.osti.gov/servlets/purl/1611062.
@article{osti_1611062,
title = {Solid Oganesson via a Many-Body Interaction Expansion Based on Relativistic Coupled-Cluster Theory and from Plane-Wave Relativistic Density Functional Theory},
author = {Jerabek, Paul and Smits, Odile R. and Mewes, Jan-Michael and Peterson, Kirk A. and Schwerdtfeger, Peter},
abstractNote = {In this work, many-body potentials up to fourth order in the expansion are constructed using non-relativistic, scalar-relativistic and relativistic coupled-cluster theory to accurately describe the interaction between superheavy oganesson atoms. The obtained distance dependent energy values were fitted to extended two-body Lennard-Jones and three-body Axilrod-Teller-Muto potentials, with the fourth-order term treated through a classical long-range Drude dipole interaction model. From these interac tion potentials, spectroscopic constants for the oganesson dimer and solid state properties were obtained. Furthermore, these high-level results are compared to scalar relativistic and two-component plane-wave DFT calculations based on a tailor-made projector augmented-wave pseudopotential (PAW-PP) and newly derived parameters for Grimme’s dispersion correction. It is shown that the functionals PBE-D3(BJ), PBEsol and in particular SCAN provide excellent agreement with the many-body ref erence for solid Og. Finally, the results for Og are compared and related to the lighter rare gas elements and periodic trends are discussed.},
doi = {10.1021/acs.jpca.9b01947},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 19,
volume = 123,
place = {United States},
year = {2019},
month = {4}
}

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    Works referencing / citing this record:

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