High-fidelity electronic structure and properties of InSb: $G_0{W}_0$ and Bayesian-optimized hybrid functionals and DFT+$U$ approaches

Abstract

This study presents a refined approach to computing the electronic structure of indium antimonide (InSb) using advanced \textit{ab initio} techniques with the In and Sb $4d^{10}$ semicore electrons included in the valence states. These states are modeled using fully relativistic projector augmented waves (PAW) and optimized norm-conserving Vanderbilt (ONCV) pseudopotentials. However, standard Kohn-Sham density-functional theory (DFT) calculations with these pseudopotentials often produce non-physical band inversions and incorrect band gaps at the $\Gamma$-point due to $5p$-$4d$ repulsion and self-interaction errors (SIE). To resolve these issues, we apply a combination of hybrid Heyd-Scuseria-Ernzerhof (HSE) exchange-correlation (XC) functionals, many-body perturbation theory (MBPT) via quasiparticle $G_0{W}_0$, and DFT+$U$, significantly improving the accuracy of the band structure over previous studies. A Bayesian optimization framework is used to refine key parameters, including the inverse screening length ($\mu$) and Hartree-Fock (HF) exchange fraction ($\alpha$) in HSE-based XC functionals, as well as the Hubbard $U$ parameters in DFT+$U$, leading to significantly improved band structure predictions. This approach yields highly precise band gaps, bulk moduli, effective masses, Luttinger parameters, valence bandwidth, and $4d$ band positions, achieving unprecedented agreement with experimental data. The resulting model resolves the long-standing incomplete description of InSb's electronic band structure and provides a transferable computational framework for accurate electronic structure predictions across diverse material systems, offering valuable insights for future electronic, optoelectronic, energy, and quantum applications.

arXiv commentAccepted in Physical Review B (APS). 16 pages, 3 figures. Supplemental Material included in the source folder

References in corpus (15)

• Advanced capabilities for materials modelling with Quantum ESPRESSO
• A linear response approach to the calculation of the effective interaction parameters in the LDA+U method
• Optimized norm-conserving Vanderbilt pseudopotentials
• The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table
• Wannier90 as a community code: new features and applications
• Localization and delocalization errors in density functional theory and implications for band-gap prediction
• Optimization Algorithm for the Generation of ONCV Pseudopotentials
• Gaussian Process Optimization in the Bandit Setting: No Regret and Experimental Design
• 103-Compound Band Structure Benchmark of Post-SCF Spin-Orbit Coupling Treatments in Density-Functional Theory
• The derivative discontinuity of the exchange-correlation functional
• In-plane selective area InSb-Al nanowire quantum networks
• Strain tuning of topological band order in cubic semiconductors
• An Optimally-Tuned Starting Point for Single-Shot $GW$ Calculations of Solids
• Fully relativistic $GW$/Bethe-Salpeter calculations in BerkeleyGW: implementation, symmetries, benchmarking, and performance
• Strong and tunable spin-orbit interaction in a single crystalline InSb nanosheet