  The molecular polarizability describes the tendency of a molecule to deform
or polarize in response to an applied electric field. As such, this quantity
governs key intra- and inter-molecular interactions such as induction and
dispersion, plays a key role in determining the spectroscopic signatures of
molecules, and is an essential ingredient in polarizable force fields and other
empirical models for collective interactions. Compared to other ground-state
properties, an accurate and reliable prediction of the molecular polarizability
is considerably more difficult as this response quantity is quite sensitive to
the description of the underlying molecular electronic structure. In this work,
we present state-of-the-art quantum mechanical calculations of the static
dipole polarizability tensors of 7,211 small organic molecules computed using
linear-response coupled-cluster singles and doubles theory (LR-CCSD). Using a
symmetry-adapted machine-learning based approach, we demonstrate that it is
possible to predict the molecular polarizability with LR-CCSD accuracy at a
negligible computational cost. The employed model is quite robust and
transferable, yielding molecular polarizabilities for a diverse set of 52
larger molecules (which includes challenging conjugated systems, carbohydrates,
small drugs, amino acids, nucleobases, and hydrocarbon isomers) at an accuracy
that exceeds that of hybrid density functional theory (DFT). The atom-centered
decomposition implicit in our machine-learning approach offers some insight
into the shortcomings of DFT in the prediction of this fundamental quantity of
interest.
