We describe an approach to constructing an analytic Cartesian representation of the molecular dipole polarizability tensor surface in terms of polynomials in interatomic distances with a training set of ab initio data points obtained from a molecular dynamics (MD) simulation or by any other available means. The proposed formulation is based on a perturbation treatment of the unmodified point dipole polarizability model of Applequist [J. Am. Chem. Soc.1972942952] and is shown here to be, by construction (i) free of short-range or other singularities or discontinuities, (ii) symmetric and translationally invariant, and (iii) nonreliant on a body-fixed coordinate system. Permutational invariance of like nuclei is demonstrated to be readily applicable, making this approach useful for highly fluxional and reactive systems. Derivation of the method is described in detail, adding brief didactic numerical examples of H2 and H2O and concluding with an MD simulation of the Raman spectrum of H5O2 + at 300 K with the polarizability tensor fitted to CCSD­(T)/aug-cc-pVTZ data obtained using the HBB-4B potential [044308J. Chem. Phys.2005122].