Molecule-specific Uncertainty Quantification in Quantum Chemical Studies

TL;DR

This paper emphasizes the importance of system-specific uncertainty quantification in electronic structure calculations to improve the reliability of quantum chemical predictions across various chemical phenomena.

Contribution

It introduces the concept that meaningful quantum predictions require uncertainty estimates for each calculation, highlighting a shift towards more reliable, system-specific assessments in electronic structure modeling.

Findings

Electronic structure models are central to chemical research.

Uncertainty quantification enhances confidence in quantum predictions.

Future developments should focus on system-specific uncertainty information.

Abstract

Solving the electronic Schr\"odinger equation for changing nuclear coordinates provides access to the Born-Oppenheimer potential energy surface. This surface is the key starting point for almost all theoretical studies of chemical processes in electronic ground and excited states (including molecular structure prediction, reaction mechanism elucidation, molecular property calculations, quantum and molecular dynamics). Electronic structure models aim at a sufficiently accurate approaximation of this surface. They have therefore become a cornerstone of theoretical and computational chemistry, molecular physics, and materials science. In this work, we elaborate on general features of approximate electronic structure models such as accuracy, transferability, and general applicability in order to arrive at a perspective for future developments, of which a vanguard has already arrived. Our quintessential proposition is that meaningful quantum mechanical predictions for chemical phenomena require system-specific uncertainty information for each and every electronic structure calculation, if objective conclusions shall be drawn with confidence.