The loss of the property of locality of the kernel in high-dimensional Gaussian process regression on the example of the fitting of molecular potential energy surfaces

Kernel-based methods, including Gaussian process regression (GPR) and generally kernel ridge regression, have been finding increasing use in computational chemistry, including the fitting of potential energy surfaces and density functionals in high-dimensional feature spaces. Kernels of the Matern family, such as Gaussian-like kernels (basis functions), are often used which allow imparting to them the meaning of covariance functions and formulating GPR as an estimator of the mean of a Gaussian distribution. The notion of locality of the kernel is critical for this interpretation. It is also critical to the formulation of multi-zeta type basis functions widely used in computational chemistry. We show, on the example of fitting of molecular potential energy surfaces of increasing dimensionality, the practical disappearance of the property of locality of a Gaussian-like kernel in high dimensionality. We also formulate a multi-zeta approach to the kernel and show that it significantly improves the quality of regression in low dimensionality but loses any advantage in high dimensionality, which is attributed to the loss of the property of locality.

Automated summary

Kernel-based methods, such as Gaussian process regression (GPR), are widely used in computational chemistry for fitting potential energy surfaces in high-dimensional spaces. This study shows the disappearance of the locality property of Gaussian-like kernels in high dimensionality, which has a significant impact on the regression quality. Additionally, a multi-zeta approach to the kernel is formulated and found to improve regression in low dimensionality but not in high dimensionality due to the loss of locality property.