High-order nonlinear susceptibilities of helium

With the goal of providing critically evaluated atomic data for modeling high harmonic generation processes in noble gases, we present calculations of frequency-dependent nonlinear susceptibilities of the ground state of helium, within the framework of Rayleigh-Schrödinger perturbation theory at lowest applicable order. The nonrelativistic, infinite-nuclear-mass, atomic Hamiltonian is decomposed in terms of Hylleraas coordinates and spherical harmonics, and the hierarchy of inhomogeneous equations of perturbation theory is solved iteratively. The mixed Hylleraas and Frankowski basis functions are employed to represent accurately the ground-state and perturbed wave functions. We believe our results for nonlinear susceptibilities of helium are the most accurate (and in many cases, the only) available to date, and they are offered as benchmark data for design of future multiphoton experiments.