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Register a new userUsing Gaussian Process Regression to Simulate the Vibrational Raman Spectra of Molecular Crystals
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Added by
Nathaniel Raimbault
Publication date
2019
fields
Physics
and research's language is
English
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Vibrational properties of molecular crystals are constantly used as structural fingerprints, in order to identify both the chemical nature and the structural arrangement of molecules. The simulation of these properties is typically very costly, especially when dealing with response properties of materials to e.g. electric fields, which require a good description of the perturbed electronic density. In this work, we use Gaussian process regression (GPR) to predict the static polarizability and dielectric susceptibility of molecules and molecular crystals. We combine this framework with ab initio molecular dynamics to predict their anharmonic vibrational Raman spectra. We stress the importance of data representation, symmetry, and locality, by comparing the performance of different flavors of GPR. In particular, we show the advantages of using a recently developed symmetry-adapted version of GPR. As an examplary application, we choose Paracetamol as an isolated molecule and in different crystal forms. We obtain accurate vibrational Raman spectra in all cases with less than 1000 training points, and obtain improvements when using a GPR trained on the molecular monomer as a baseline for the crystal GPR models. Finally, we show that our methodology is transferable across polymorphic forms: we can train the model on data for one structure, and still be able to accurately predict the spectrum for a second polymorph. This procedure provides an independent route to access electronic structure properties when performing force-evaluations on empirical force-fields or machine-learned potential energy surfaces.
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Folding uncertainty in theoretical models into Bayesian parameter estimation is necessary in order to make reliable inferences. A general means of achieving this is by marginalizing over model uncertainty using a prior distribution constructed using Gaussian process regression (GPR). As an example, we apply this technique to the measurement of chirp mass using (simulated) gravitational-wave signals from binary black holes that could be observed using advanced-era gravitational-wave detectors. Unless properly accounted for, uncertainty in the gravitational-wave templates could be the dominant source of error in studies of these systems. We explain our approach in detail and provide proofs of various features of the method, including the limiting behavior for high signal-to-noise, where systematic model uncertainties dominate over noise errors. We find that the marginalized likelihood constructed via GPR offers a significant improvement in parameter estimation over the standard, uncorrected likelihood both in our simple one-dimensional study, and theoretically in general. We also examine the dependence of the method on the size of training set used in the GPR; on the form of covariance function adopted for the GPR, and on changes to the detector noise power spectral density.
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