Norm-Conserving Pseudopotentials and Basis Sets to Explore Lanthanide Chemistry in Complex Environments

Jun Bo Lu, David C. Cantu, Manh Thuong Nguyen, Jun Li, Vassiliki Alexandra Glezakou, Roger Rousseau

Research output: Contribution to journalArticle

Abstract

A complete set of pseudopotentials and accompanying basis sets for all lanthanide elements are presented based on the relativistic, norm-conserving, separable, dual-space Gaussian-type pseudopotential protocol of Goedecker, Teter, and Hutter (GTH) within the generalized gradient approximation (GGA) and the exchange-correlation functional of Perdew, Burke, and Ernzerhof (PBE). The corresponding basis sets have been molecularly optimized (MOLOPT) using a contracted form with a single set of Gaussian exponents for the s, p, and d states. The f states are uncontracted explicitly with Gaussian exponents. Moreover, the Hubbard U values for each lanthanide element, for DFT+U calculations, are also tabulated, allowing for the proper treatment of the strong on-site Coulomb interactions of localized 4f electrons. The accuracy and reliability of our GTH pseudopotentials and companion basis sets optimized for lanthanides is illustrated by a series of test calculations on lanthanide-centered molecules, and solid-state systems, with the most common oxidation states. We anticipate that these pseudopotentials and basis sets will enable larger-scale density functional theory calculations and ab initio molecular dynamics simulations of lanthanide molecules in either gas or condensed phases, as well as of solid state lanthanide-containing materials, allowing further exploration of the chemical and physical properties of lanthanide systems.

Original languageEnglish
JournalJournal of Chemical Theory and Computation
DOIs
Publication statusAccepted/In press - Jan 1 2019

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Lanthanoid Series Elements
Rare earth elements
norms
pseudopotentials
chemistry
exponents
solid state
chemical properties
molecules
physical properties
vapor phases
Molecules
molecular dynamics
density functional theory
gradients
oxidation
Coulomb interactions
Discrete Fourier transforms
Chemical properties
Density functional theory

ASJC Scopus subject areas

  • Computer Science Applications
  • Physical and Theoretical Chemistry

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Norm-Conserving Pseudopotentials and Basis Sets to Explore Lanthanide Chemistry in Complex Environments. / Lu, Jun Bo; Cantu, David C.; Nguyen, Manh Thuong; Li, Jun; Glezakou, Vassiliki Alexandra; Rousseau, Roger.

In: Journal of Chemical Theory and Computation, 01.01.2019.

Research output: Contribution to journalArticle

Lu, Jun Bo ; Cantu, David C. ; Nguyen, Manh Thuong ; Li, Jun ; Glezakou, Vassiliki Alexandra ; Rousseau, Roger. / Norm-Conserving Pseudopotentials and Basis Sets to Explore Lanthanide Chemistry in Complex Environments. In: Journal of Chemical Theory and Computation. 2019.
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