A sum rule for nonlinear optical susceptibilities

摘要

It is explicitly shown, for optical processes arbitrarily comprising two-, three- or four-photon interactions, that the sum over all matter states of any optical susceptibility is exactly ero. The result remains true even in frequency regions where damping is prominent. Using a quantum electrodynamical framework to render the photonic nature of the fundamental interactions, the result emerges in the form of a traceless operator in Hilbert space. The generality of the sum rule and its significance as a thermodynamic limit are discussed, and the applicability to real systems is assessed.