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Spin Parameter Optimization for Spin-polarized Extended Tight-binding Methods by Moradi, Siyavash; Tomann, Rebecca; Hendrix, Josie; Head-Gordon, Martin; Stein, Christopher J. is a scholarly article available to read on EtoBox.

What is Spin Parameter Optimization for Spin-polarized Extended Tight-binding Methods about?

We present an optimization strategy for atom-specific spin-polarization constants within the spin-polarized GFN2-xTB framework, aiming to enhance the accuracy of molecular simulations. We compare a sequential and global optimization of spin parameters for hydrogen, carbon, nitrogen, oxygen, and fluorine. Sensitivity analysis using Sobol indices guides the identification of the most influential parameters for a given reference dataset, allowing for a nuanced understanding of their impact on diverse molecular properties. In the case of the W4-11 dataset, substantial error reduction was achieved, demonstrating the potential of the optimization. Transferability of the optimized spin-polarization constants over different properties, however, is limited, as we demonstrate by applying the optimized parameters on a set of singlet-triplet gaps in carbenes. Further studies on ionization potentials and electron affinities highlight some inherent limitations of current extended tight-binding methods that can not be resolved by simple parameter optimization. We conclude that the significantly improved accuracy strongly encourages the present re-optimization of the spin-polarization constants, w

Author

Moradi, Siyavash; Tomann, Rebecca; Hendrix, Josie; Head-Gordon, Martin; Stein, Christopher J.

Published

2024

Language

EN