Real-time feedback from iterative electronic structure calculations

Real‐time feedback from iterative electronic structure calculations requires to mediate between the inherently unpredictable execution times of the iterative algorithm used 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 semiempirical methods as the data source and apply the surrogate‐potential mediator to deliver reliable real‐time feedback. © 2015 Wiley Periodicals, Inc. Interactive reactivity exploration based on iterative electronic structure methods faces an unavoidable incompatibility of unpredictable execution times of such calculations and of the necessity for feedback to be delivered in fixed and short time intervals. This article proposes a mediator strategy involving surrogate potentials to provide real‐time feedback that allows for an effective and reliable immersion of a user into the exploration process.