Choosing tight-binding models for accurate optoelectronic responses

Tight-binding models provide great insight and are a low-cost alternative to ab initio methods for the calculation of a material’s electronic structure. These models are used to calculate optical responses, including nonlinear optical effects such as the shift current bulk photovoltaic effect. The validity of tight-binding models is often evaluated by comparing their band structures to those calculated with density functional theory. However, we find that band structure agreement is a necessary but not sufficient condition for accurate optical response calculations. We compute the shift current response and dielectric tensor using a variety of tight-binding models of MoS2, including both Slater-Koster and Wannier tight-binding models that treat the Mo 4d orbitals and/or S 3p orbitals. We also truncate hoppings in the Wannier function models to next-nearest-neighbor, as is common in tight-binding methods, in order to gauge the effect on optical response. By examining discrepancies in ene..., , # Data from: Choosing tight-binding models for accurate optoelectronic responses

Dataset DOI: [10.5061/dryad.3r2280gwt](https://doi.org/10.5061/dryad.3r2280gwt)

## Description of the data and file structure

This data was collected using the following techniques. For more information, consult the paper.

1. Quantum Espresso - used for electronic structure calculations
2. Wannier90 - used for Wannierization
3. PythTB - used to generate tight-binding models

The data shown here is the final data that is plotted/shown in figures in the paper. All data should be viewable by a text editor, except for the Brillouin Zone data, which are .npy files.

### Files and variables

#### File: Dryad_Data.zip

**Description:** Attached is the data for the article *Choosing tight-binding models for accurate optoelectronic responses* ([https://journals.aps.org/prb/abstract/10.1103/PhysRevB.111.125203](https://journals.aps.org/prb/abstract/10.1103/PhysRevB.111.125203)) in PRB. These data were used to gen...,