Machine learning exciton dynamics
View/ Open
Author
Pyzer-Knapp, Edward
Note: Order does not necessarily reflect citation order of authors.
Published Version
https://doi.org/10.1039/c5sc04786bMetadata
Show full item recordCitation
Häse, Florian, Stéphanie Valleau, Edward Pyzer-Knapp, and Alán Aspuru-Guzik. 2016. “Machine Learning Exciton Dynamics.” Chem. Sci. 7 (8): 5139–5147. doi:10.1039/c5sc04786b.Abstract
Obtaining the exciton dynamics of large photosynthetic complexes by using mixed quantum mechanics/molecular mechanics (QM/MM) is computationally demanding. We propose a machine learning technique, multi-layer perceptrons, as a tool to reduce the time required to compute excited state energies. With this approach we predict time-dependent density functional theory (TDDFT) excited state energies of bacteriochlorophylls in the Fenna-Matthews-Olson (FMO) complex. Additionally we compute spectral densities and exciton populations from the predictions. Different methods to determine multi-layer perceptron training sets are introduced, leading to several initial data selections. In addition, we compute spectral densities and exciton populations. Once multi-layer perceptrons are trained, predicting excited state energies was found to be significantly faster than the corresponding QM/MM calculations. We showed that multi-layer perceptrons can successfully reproduce the energies of QM/MM calculations to a high degree of accuracy with prediction errors contained within 0.01 eV (0.5%). Spectral densities and exciton dynamics are also in agreement with the TDDFT results. The acceleration and accurate prediction of dynamics strongly encourage the combination of machine learning techniques with ab-initio methods.Other Sources
http://arxiv.org/abs/1511.07883Terms of Use
This article is made available under the terms and conditions applicable to Other Posted Material, as set forth at http://nrs.harvard.edu/urn-3:HUL.InstRepos:dash.current.terms-of-use#LAACitable link to this page
http://nrs.harvard.edu/urn-3:HUL.InstRepos:33439112
Collections
- FAS Scholarly Articles [18295]
Contact administrator regarding this item (to report mistakes or request changes)