Real-time feedback from iterative electronic structure calculations

TL;DR

This paper presents a mediator-based approach using surrogate potentials to enable real-time feedback in iterative electronic structure calculations, facilitating real-time quantum chemistry applications.

Contribution

It introduces a mediator concept with surrogate potentials that provide reliable, real-time feedback despite unpredictable calculation times in electronic structure methods.

Findings

Surrogate potentials can be updated continuously for reliable feedback.

The approach enables real-time reactivity exploration in quantum chemistry.

Implementation with semi-empirical methods demonstrates practical applicability.

Abstract

Real-time feedback from iterative electronic structure calculations requires to mediate between the inherently unpredictable execution times of the iterative algorithm employed and the necessity to provide data in fixed and short time intervals for real-time rendering. We introduce the concept of a mediator as a component able to deal with infrequent and unpredictable reference data to generate reliable feedback. In the context of real-time quantum chemistry, the mediator takes the form of a surrogate potential that has the same local shape as the first-principles potential and can be evaluated efficiently to deliver atomic forces as real-time feedback. The surrogate potential is updated continuously by electronic structure calculations and guarantees to provide a reliable response to the operator for any molecular structure. To demonstrate the application of iterative electronic structure methods in real-time reactivity exploration, we implement self-consistent semi-empirical methods as the data source and apply the surrogate-potential mediator to deliver reliable real-time feedback.