Efficient and accurate calculation of band gaps of halide perovskites with the Tran-Blaha modified Becke-Johnson potential

Abstract

We report on a reoptimization of the Tran-Blaha modified Becke-Johnson (TB-mBJ) potential dedicated to the prediction of the band gaps of 3-dimensional (3D) and layered hybrid organicinorganic perovskites (HOP) within pseudopotential-based density functional theory methods. These materials hold promise for future photovoltaic and optoelectronic applications. We begin by determining a set of parameters for 3D HOP optimized over a large range of materials. Then we consider the case of layered HOP. We design an empirical relationship that facilitates the prediction of band gaps of layered HOP with arbitrary interlayer molecular spacers with a computational cost considerably lower than more advanced methods like hybrid functionals or GW. Our study also shows that substituting interlayer molecular chains of layered HOP with Cs atoms is an appealing and cost-effective route to band gap calculations. Finally, we discuss on the pitfalls and limitations of TB-mBJ for HOP, notably its tendency to overestimate the effective masses due to the narrowing of the band dispersions. We expect our results to extend the use of TB-mBJ for other low-dimensional materials. 2 B. Traore et coll. Phys. Rev.

Cation Engineering in Two-Dimensional Ruddlesden–Popper Lead Iodide Perovskites with Mixed Large A-Site Cations in the Cages

“…70 We used optimized pseudopotential TB-mBJ (ppTB-mBJ) parameters α = A c c e p t e d m a n u s c r i p t 0.65 and β = 1.023 for hybrid perovskites within pseudopotential implementation of DFT as detailed elsewhere. 51 All the calculations take SOC into account.…”

Local Modified Becke-Johnson Exchange-Correlation Potential for Interfaces, Surfaces, and Two-Dimensional Materials

“…We chose the latter parameters for this work, as they predict band gaps of semiconductors very close to their experimental values. Other parameters were also obtained recently for more specialized material sets [18,19]. In spite of its many virtues, analyzed in detail in Ref.…”

Spectroscopic properties of few-layer tin chalcogenides

“…Vibrational properties are also checked for higher k-point grid (up to 16×16×16) and we have a convergence on phonon mode eigenvalues of 0.1 cm −1 . Electron band structures are also calculated using the TB-mBJ meta-GGA functional [44,45,65]. α=−0.012 and β=1.023 Bohr 1/2 are the parameters that are used in our calculation.…”

“…Electronic band structures are also calculated for bulk and few-layer materials using the Tran-Blaha modified Becke-Johnson (TB-mBJ) meta-GGA functional [44,45] using the relaxed lattice parameters reported above. In general, the band gap predicted by the TB-mBJ functional is comparable to more computationally demanding techniques such as GW or hybrid functionals [46].…”