We present two enhancements to our methods for calculating vibrational-rotational free energies by Feynman path integrals, namely, a sequential sectioning scheme for efficiently generating random free-particle paths and a stratified sampling scheme that uses the energy of the path centroids. These improved methods are used with three interaction potentials to calculate equilibrium constants for the fractionation behavior of Cl- hydration in the presence of a gas-phase mixture of H2O, D2O, and HDO. Ion cyclotron resonance experiments indicate that the equilibrium constant, K-eq, for the reaction Cl(H2O)(-) + D2O reversible arrow Cl(D2O)(-) + H2O is 0.76, whereas the three theoretical predictions are 0.946, 0.979, and 1.20. Similarly, the experimental K-eq for the Cl(H2O)(-) + HDO reversible arrow Cl(HDO)(-) + H2O reaction is 0.64 as compared to theoretical values of 0.972, 0.998, and 1.10. Although Cl(H2O)(-) has a large degree of anharmonicity, K-eq values calculated with the harmonic oscillator rigid rotator (HORR) approximation agree with the accurate treatment to within better than 2% in all cases. Results of a variety of electronic structure calculations, including coupled cluster and multireference configuration interaction calculations, with either the HORR approximation or with anharmonicity estimated via second-order vibrational perturbation theory, all agree well with the equilibrium constants obtained from the analytical surfaces.