On the Predictive Power of Chemical Concepts

TL;DR

This paper evaluates the predictive capabilities of fundamental chemical concepts derived from quantum theories, aiming to enhance autonomous reaction exploration through first-principles heuristics.

Contribution

It systematically analyzes the predictive power of key chemical reactivity concepts for guiding autonomous reaction exploration.

Findings

Chemical concepts have potential for predictive modeling.

Theoretical basis enables systematic definition of concepts.

Insights could improve autonomous reaction protocols.

Abstract

Many chemical concepts can be well defined in the context of quantum chemical theories. Examples are the electronegativity scale of Mulliken and Jaffe and the hard and soft acids and bases concept of Pearson. The sound theoretical basis allows for a systematic definition of such concepts. However, while they are often used to describe and compare chemical processes in terms of reactivity, their predictive power remains unclear. In this work, we elaborate on the predictive potential of chemical reactivity concepts, which can be crucial for autonomous reaction exploration protocols to guide them by first-principles heuristics that expoit these concepts.