Solution of the Schrodinger equation for quasi-one-dimensional materials using helical waves

TL;DR

This paper introduces a spectral method using helical waves for solving the Schrödinger equation in quasi-one-dimensional materials, enabling accurate and efficient electronic structure calculations without traditional supercell approximations.

Contribution

The authors develop a novel spectral approach with fast transforms and matrix-free diagonalization for quasi-1D materials, implemented in the HelicES package, improving over existing methods.

Findings

Accurate electronic structure calculations for nanotubes, nanoribbons, and nanowires.

Demonstrated convergence, efficiency, and accuracy of the method.

Applicable to various nanostructures without supercell approximations.

Abstract

We formulate and implement a spectral method for solving the Schrodinger equation, as it applies to quasi-one-dimensional materials and structures. This allows for computation of the electronic structure of important technological materials such as nanotubes (of arbitrary chirality), nanowires, nanoribbons, chiral nanoassemblies, nanosprings and nanocoils, in an accurate, efficient and systematic manner. Our work is motivated by the observation that one of the most successful methods for carrying out electronic structure calculations of bulk/crystalline systems -- the plane-wave method -- is a spectral method based on eigenfunction expansion. Our scheme avoids computationally onerous approximations involving periodic supercells often employed in conventional plane-wave calculations of quasi-one-dimensional materials, and also overcomes several limitations of other discretization strategies, e.g., those based on finite differences and atomic orbitals. We describe the setup of fast transforms to carry out discretization of the governing equations using our basis set, and the use of matrix-free iterative diagonalization to obtain the electronic eigenstates. Miscellaneous computational details, including the choice of eigensolvers, use of a preconditioning scheme, evaluation of oscillatory radial integrals and the imposition of a kinetic energy cutoff are discussed. We have implemented these strategies into a computational package called HelicES (Helical Electronic Structure). We demonstrate the utility of our method in carrying out systematic electronic structure calculations of various quasi-one-dimensional materials through numerous examples involving nanotubes, nanoribbons and nanowires. We also explore the convergence, accuracy and efficiency of our method. We anticipate that our method will find numerous applications in computational nanomechanics and materials science.