Enhancing the accuracy of density functional tight binding models through ChIMES many-body interaction potentials

• Published in: The Journal of chemical physics 2023-04, Vol.158 (14), p.144112-144112
• Main Authors: Goldman, Nir, Fried, Laurence E., Lindsey, Rebecca K., Pham, C. Huy, Dettori, R.
• Format: Article
• Language: English
• Subjects: Accuracy; Binding; Chebyshev approximation; Chebyshev functions; Chemical properties; Computational efficiency; computer simulation; Density; density-functional tight-binding; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Interaction models; machine learning; Many body problem; Neural networks; Organic chemistry; quantum mechanical calculations; quantum mechanical systems and processes; Simulation
• ISSN: 0021-9606; 1089-7690
• DOI: 10.1063/5.0141616

Semi-empirical quantum models such as Density Functional Tight Binding (DFTB) are attractive methods for obtaining quantum simulation data at longer time and length scales than possible with standard approaches. However, application of these models can require lengthy effort due to the lack of a systematic approach for their development. In this work, we discuss the use of the Chebyshev Interaction Model for Efficient Simulation (ChIMES) to create rapidly parameterized DFTB models, which exhibit strong transferability due to the inclusion of many-body interactions that might otherwise be inaccurate. We apply our modeling approach to silicon polymorphs and review previous work on titanium hydride. We also review the creation of a general purpose DFTB/ChIMES model for organic molecules and compounds that approaches hybrid functional and coupled cluster accuracy with two orders of magnitude fewer parameters than similar neural network approaches. In all cases, DFTB/ChIMES yields similar accuracy to the underlying quantum method with orders of magnitude improvement in computational cost. Our developments provide a way to create computationally efficient and highly accurate simulations over varying extreme thermodynamic conditions, where physical and chemical properties can be difficult to interrogate directly, and there is historically a significant reliance on theoretical approaches for interpretation and validation of experimental results.