Details

Autor(en) / Beteiligte

• Sommers, Grace M
• Calegari Andrade, Marcos F
• Zhang, Linfeng
• Wang, Han
• Car, Roberto

Titel

Raman spectrum and polarizability of liquid water from deep neural networks

Ist Teil von

• Physical chemistry chemical physics : PCCP, 2020-05, Vol.22 (19), p.1592-162

Ort / Verlag

England: Royal Society of Chemistry

Erscheinungsjahr

2020

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• We introduce a scheme based on machine learning and deep neural networks to model the environmental dependence of the electronic polarizability in insulating materials. Application to liquid water shows that training the network with a relatively small number of molecular configurations is sufficient to predict the polarizability of arbitrary liquid configurations in close agreement with ab initio density functional theory calculations. In combination with a neural network representation of the interatomic potential energy surface, the scheme allows us to calculate the Raman spectra along 2-nanosecond classical trajectories at different temperatures for H 2 O and D 2 O. The vast gains in efficiency provided by the machine learning approach enable longer trajectories and larger system sizes relative to ab initio methods, reducing the statistical error and improving the resolution of the low-frequency Raman spectra. Decomposing the spectra into intramolecular and intermolecular contributions elucidates the mechanisms behind the temperature dependence of the low-frequency and stretch modes. Using deep neural networks to model the polarizability and potential energy surfaces, we compute the Raman spectrum of liquid water at several temperatures with ab initio molecular dynamics accuracy.