Evaluation and Optimization Methods for Applicability Domain Methods and Their Hyperparameters, Considering the Prediction Performance of Machine Learning Models

Abstract

In molecular, material, and process design and control, the applicability domain (AD) of a mathematical model y = f(x) between properties, activities, and features x is constructed. As there are multiple AD methods, each with its own set of hyperparameters, it is necessary to select an appropriate AD method and hyperparameters for each data set and mathematical model. However, there is no method for optimizing the AD model. This study proposes a method for evaluating and optimizing the AD model for each data set and a mathematical model. Using the predictions of double cross-validation with all samples, the relationship between coverage and root-mean-squared error (RMSE) was calculated for all combinations of AD methods and their hyperparameters, and the area under the coverage and RMSE curve (AUCR) was calculated. The AD model with the lowest AUCR value was selected as the optimal fit for the mathematical model. The proposed method was validated using eight data sets, including molecules, materials, and spectra, demonstrating that the proposed method could generate optimal AD models for all data sets. The Python code for the proposed method is available at https://github.com/hkaneko1985/dcekit.