Novel approach to nonlinear susceptibility in semiconductors

We here propose a new procedure to derive a general expression of the third-order susceptibility valid for any semiconductor Hamiltonian. It relies on our theory for composite exciton many-body effects which is quite appropriate to this problem since all optical nonlinearities in semiconductors come from exchange scatterings with the virtual excitons coupled to photons. Our expression of chi((3)) is sample volume free, as physically expected. It also contains a Pauli term (exchange without Coulomb) which is missed by all bosonized exciton approaches. This term, dominant at large detuning, is a direct manifestation of the exciton composite nature.