Compound-tunable embedding potential method and its application to fersmite crystal

Abstract

Compound-tunable embedding potential (CTEP) method is proposed. A fragment of some chemical compound, "main cluster" in the present paper, is limited by boundary anions such that the nearest environmental atoms are cations. The CTEP method is based on constructing the embedding potential as linear combination of short-range "electron-free" spherical "tunable" pseudopotentials for cations from nearest environment of the main cluster, whereas the long-range CTEP part consists of Coulomb potentials from optimized fractional point charges centered on both environmental cations and anions. A pilot application of the CTEP method to the fersmite crystal, CaNb${}_2$O${}_6$, is performed and a remarkable agreement of the electronic density and interatomic distances within the fragment with those of the original periodic crystal calculation is attained. Characteristics of "atoms-in-compounds" which are of great importance for compound of $f$- and $d$-elements (Nb in fersmite) are considered on examples of chemical shifts of $K_{{\alpha }_{1,2}}$ and $K_{{\beta }_{1,2}}$ lines of X-ray emission spectra in niobium. A very promising potential of this approach in studying variety of properties of point defects containing $f$- and heavy $d$-elements with relativistic effects, extended basis set and broken crystal symmetry considered is discussed.

References in corpus (13)

• Hubbard-corrected density functional perturbation theory with ultrasoft pseudopotentials
• Theoretical study of thorium monoxide for the electron electric dipole moment search, II: Electronic properties of $H^3{\Delta }_1$ in ThO
• Can Density Matrix Embedding Theory with the Complete Activate Space Self-Consistent Field Solver Describe Single and Double Bond Breaking in Molecular Systems?
• Theoretical study of ThF${}^{+}$ in the search for T,P-violation effects: Effective state of a Th atom in ThF${}^{+}$ and ThO compounds
• Concept of effective states of atoms in compounds to describe properties determined by the densities of valence electrons in atomic cores
• Rigorous wave function embedding with dynamical fluctuations
• Cluster size convergence of the density matrix embedding theory and its dynamical cluster formulation: a study with an auxiliary-field quantum Monte Carlo solver
• Many-body renormalisation of forces in f-electron materials
• Actinide and lanthanide molecules to search for strong CP-violation
• Ultrasoft pseudopotentials with kinetic energy density support: implementing the modified Becke-Johnson potential
• Which oxidation state of uranium and thorium as point defects in xenotime is favorable?
• Global and local approaches to population analysis: bonding patterns in superheavy element compounds
• Compound-tunable embedding potential method and its application to ytterbium fluoride crystals YbF${}_2$ and YbF${}_3$

Cited by in corpus (2)

• Compound-tunable embedding potential method to model local electronic excitations on $f$-element ions in solids: Pilot relativistic coupled cluster study of Ce and Th impurities in yttrium orthophosphate, YPO${}_4$
• On the rank-reduced relativistic coupled cluster method