Work

Making excited state MD faster: Extrapolation of transition densities for TD-DFT calculations

Year: 2026

Type: article

Abstract: Excited state molecular dynamics simulations are a powerful computational tool for the study of photoinduced phenomena. These are often used in conjunction with linear response TD-DFT to get the excited state energy and its gradients. At each step of molecular dynamics simulation, the new molecular geometry is relatively close to the previous ones, suggesting that some extrapolation strategy can be applied, such that the results of the previous calculations, which are available for free, can be used to predict the result of the upcoming calculation. The prediction can then be used as a guess for the iterative solver to lower the number of iterations and thus the cost. In this contribution, we present an extension of the Grassmann extrapolation scheme to linear response TD-DFT, in which the knowledge about the manifold structure to which the solutions belong is used to make the extrapolation more accurate. The new extrapolation strategy is then tested on four systems, showing a significant acceleration of the excited state molecular dynamics.

Source: The Journal of Chemical Physics

DOI: 10.1063/5.0323068

Authors: Michele Nottoli, Damiano Castrignano', Patrizia Mazzeo, Lorenzo Cupellini, Benjamin Stamm

Institutions: University of Stuttgart, University of Pisa

Language: English

Topic: Advanced Chemical Physics Studies

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: green

Funder: Deutsche Forschungsgemeinschaft

Award: G1486546336