Path-integral calculation of the third dielectric virial coefficient of noble gases

We present a rigorous framework for fully quantum calculation of the third dielectric virial coefficient C_ɛ(T) of noble gases, including exchange effects. The quantum effects are taken into account with the path-integral Monte Carlo method. Calculations employing state-of-the-art pair and three-body potentials and pair polarizabilities yield results generally consistent with the few scattered experimental data available for helium, neon, and argon, but rigorous calculations with well-described uncertainties will require the development of surfaces for the three-body nonadditive polarizability and the three-body dipole moment. The framework, developed here for the first time, will enable new approaches to primary temperature and pressure metrology based on first-principles calculations of gas properties.