Reliable emulation of complex functionals by active learning with error control*

A statistical emulator can be used as a surrogate of complex physics-based calculations to drastically reduce the computational cost. Its successful implementation hinges on an accurate representation of the nonlinear response surface with a high-dimensional input space. Conventional "space-filling'' designs, including random sampling and Latin hypercube sampling, become inefficient as the dimensionality of the input variables increases, and the predictive accuracy of the emulator can degrade substantially for a test input away from the training input set. To address this fundamental challenge, we develop a reliable emulator for predicting complex functionals by active learning with error control (ALEC). The algorithm is applicable to infinite-dimensional mapping with high-fidelity predictions and a controlled predictive error. The computational efficiency has been demonstrated by emulating the classical density functional theory (cDFT) calculations, a statistical-mechanical method widely used in modeling the equilibrium properties of complex molecular systems. We show that ALEC is more accurate than conventional emulators based on the Gaussian processes with "space-filling'' designs and alternative active learning methods. Besides, it is computationally more efficient than direct cDFT calculations. ALEC can be a reliable building block for emulating expensive functionals owing to its minimal computational cost, controllable predictive error, and fully automatic features.