Updates Add Documentation after each parameter file The Parameterization code for Density functional Tight-binding Theory (DFTB) What does it include? 1. ParameterSets The ParameterSets folder includes parameter sets `PRIOR`, `PTBP`, and `QN+Rep`, as introduced in the article PTBP Although these parameter files were not specifically optimized for compounds, they still demonstrate relatively reliable performance, as shown in Part 3.2 of the article, which benchmarks binary systems (hydrides, nitrides, oxides, and fluorides). Furthermore, the code for processing the parameterization can be found at PTBP_LAB We are pleased to share the SKF files for free use and hope they provide convenience to those exploring the DFTB method. 2. Highly recommend For downloading the parameter files by elements, please access to MBOOK/SKF File Download 3. Acknowledgement The authors gratefully acknowledge Noam Bernstein for providing the initial geometries of the homoelemental crystals and Maxime Van den Bossche for support with the hotcent package. Furthermore, we respectfully thank the works from Thomas Heine's group that initially inspired our work, and the developers of DFTB+ who made our DFTB calculations conveniently possible. [1] https://doi.org/10.1021/acs.jctc.4c00228[2] https://gitlab.com/mncui/ptbp_lab.git