A Mixed Basis Density Functional Approach for One-Dimensional Systems with B-splines

TL;DR

This paper introduces a mixed basis density functional method using B-splines and plane waves for efficient and accurate electronic structure calculations of one-dimensional systems, avoiding supercell artifacts.

Contribution

The paper develops a novel mixed basis approach combining B-splines and plane waves for 1D systems, improving computational efficiency and accuracy in geometry optimization and total energy calculations.

Findings

Efficient calculation of electronic structures for 1D systems.

Avoidance of supercell artifacts and spurious Coulomb interactions.

Successful application to carbon-based 1D nanostructures.

Abstract

A mixed basis approach based on density functional theory is extended to one-dimensional(1D) systems. The basis functions here are taken to be the localized B-splines for the two finite non-periodic dimensions and the plane waves for the third periodic direction. This approach will significantly reduce the number of the basis and therefore is computationally efficient for the diagonalization of the Kohn-Sham Hamiltonian. For 1D systems, B-spline polynomials are particularly useful and efficient in two-dimensional spatial integrations involved in the calculations because of their absolute localization. Moreover, B-splines are not associated with atomic positions when the geometry structure is optimized, making the geometry optimization easy to implement. With such a basis set we can directly calculate the total energy of the isolated system instead of using the conventional supercell model with artificial vacuum regions among the replicas along the two non-periodic directions. The spurious Coulomb interaction between the charged defect and its repeated images by the supercell approach for charged systems can also be avoided. A rigorous formalism for the long-range Coulomb potential of both neutral and charged 1D systems under the mixed basis scheme will be derived. To test the present method, we apply it to study the infinite carbon-dimmer chain, graphene nanoribbon, carbon nanotube and positively-charged carbon-dimmer chain. The resulting electronic structures are presented and discussed in details.