Band unfolding with a general transformation matrix: From code implementation to interpretation of photoemission spectra ?

Unfolding of a supercell band structure into a primitive Brillouin zone is important for understanding implications of structural distortions, disorder, defects, and solid solutions on materials electronic structure. The necessity of band unfolding is also recognized in the interpretation of angle-resolved photoemission spectroscopy (ARPES) measurements. We describe an extension of the fold2Bloch package by implementing an arbitrary transformation matrix used to establish a relation between the primitive cell and supercell. This development allows us to overcome limitations of supercells constructed exclusively by scaling of primitive cell lattice vectors. It becomes possible to transform between primitive and conventional cells as well as include rotations. The fold2Bloch is publicly available from a GitHub repository as a FORTRAN code. It interfaces with the all-electron full-potential WIEN2k and the pseudopotential VASP density functional theory packages. The fold2Bloch is supplemented by additional pre-and post-processing utilities that aid in generating k points in the supercell (such that they later fall onto a desired path in the primitive Brillouin zone after unfolding) and plotting the unfolded band structure. We selected Sr2IrO4 as an illustrative example and, for the first time, present its properly unfolded band structure in direct comparison with ARPES measurements. In addition, critical importance of the band unfolding for interpretation of SrIrO3 ARPES data is illustrated and discussed as a perspective.& COPY; 2023 Elsevier B.V. All rights reserved.