First-principles melting of krypton and xenon based on many-body relativistic coupled-cluster interaction potentials

O. R. Smits, P. Jerabek, E. Pahl, and P. Schwerdtfeger
Phys. Rev. B 101, 104103 – Published 24 March 2020

Abstract

The solid-to-liquid phase transition for krypton and xenon is studied by means of parallel-tempering Monte Carlo simulations based on an accurate description of the atomic interactions within a many-body ansatz using relativistic coupled-cluster theory. These high-level data were subsequently fitted to computationally efficient extended Lennard-Jones and extended Axilrod-Teller-Muto types of interaction potentials. Solid-state calculations demonstrate that the many-body decomposition of the interaction energy converges well for the heavier rare gas solids, leading to solid-state properties in good agreement with experiment. The results show that it suffices to include two- and three-body interactions only for the melting simulation. The melting of the bulk is simulated for cells with cubic periodic boundary conditions, as well as within a finite cluster approach. For the latter, melting of spherical magic number clusters with increasing cluster size is studied, and the melting temperatures are obtained from extrapolation to the bulk. The calculated melting temperatures for the cluster extrapolation (the periodic approach values corrected for superheating are set in parentheses) are Tm=113.7 K (110.9 K) and Tm=160.8 K (156.1 K) for krypton and xenon, respectively. Both are in very good agreement with corresponding experimental values of 115.75 and 161.40 K.

  • Figure
  • Figure
  • Figure
  • Figure
  • Figure
  • Figure
  • Received 2 December 2019
  • Revised 24 February 2020
  • Accepted 4 March 2020

DOI:https://doi.org/10.1103/PhysRevB.101.104103

©2020 American Physical Society

Physics Subject Headings (PhySH)

Statistical Physics & ThermodynamicsCondensed Matter, Materials & Applied PhysicsGeneral Physics

Authors & Affiliations

O. R. Smits1,*, P. Jerabek2,†, E. Pahl3,1,‡, and P. Schwerdtfeger1,§

  • 1Centre for Theoretical Chemistry and Physics, The New Zealand Institute for Advanced Study, Massey University Auckland, Private Bag 102904, 0632 Auckland, New Zealand
  • 2Nanotechnology Department, Helmholtz-Zentrum Geesthacht, Max-Planck-Straße 1, 21502 Geesthacht, Germany
  • 3The MacDiarmid Institute for Advanced Materials and Nanotechnology, Department of Physics, University of Auckland, New Zealand

  • *smits.odile.rosette@gmail.com
  • paul.jerabek@gmail.com
  • elke.pahl@auckland.ac.nz
  • §peter.schwerdtfeger@gmail.com; http://ctcp.massey.ac.nz/

Article Text (Subscription Required)

Click to Expand

References (Subscription Required)

Click to Expand
Issue

Vol. 101, Iss. 10 — 1 March 2020

Reuse & Permissions
Access Options
Author publication services for translation and copyediting assistance advertisement

Authorization Required


×
×

Images

×

Sign up to receive regular email alerts from Physical Review B

Log In

Cancel
×

Search


Article Lookup

Paste a citation or DOI

Enter a citation
×