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 language | English |
|---|---|
| Journal | Journal of Chemical Theory and Computation |
| DOIs | |
| Publication status | Accepted/In press - Jan 1 2019 |
Fingerprint
ASJC Scopus subject areas
- Computer Science Applications
- Physical and Theoretical Chemistry
Cite this
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 journal › Article
}
TY - JOUR
T1 - Norm-Conserving Pseudopotentials and Basis Sets to Explore Lanthanide Chemistry in Complex Environments
AU - Lu, Jun Bo
AU - Cantu, David C.
AU - Nguyen, Manh Thuong
AU - Li, Jun
AU - Glezakou, Vassiliki Alexandra
AU - Rousseau, Roger
PY - 2019/1/1
Y1 - 2019/1/1
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85073880592&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85073880592&partnerID=8YFLogxK
U2 - 10.1021/acs.jctc.9b00553
DO - 10.1021/acs.jctc.9b00553
M3 - Article
C2 - 31580663
AN - SCOPUS:85073880592
JO - Journal of Chemical Theory and Computation
JF - Journal of Chemical Theory and Computation
SN - 1549-9618
ER -