Sum-frequency generation at interfaces: A Fresnel story. III. Origin of pseudo-resonant processes in centrosymmetric bulks.

Abstract

The properties of bulk contribution to sum-frequency generation reflected and transmitted by a finite layer in a multilayer system are described. The leading term is essentially due to the processes emitting in the transmission geometry, in particular for macroscopic layers. For such transmission processes, phase mismatch leads to the production of interference fringes when the layer thickness or a wavelength is tuned, which may be mistaken for resonant processes inside or at the surface of the material. Experimental evidence of such fringes measured from centrosymmetric bulks is provided for a diamond window in the far infrared and suggested for other materials in previously published data. The existence of a stationary point in the phase mismatch, related to the group velocity mismatch, is shown to be the source of another pseudo-resonant process in centrosymmetric calcium and barium fluorides, for which theoretical predictions reproduce the experimental observations.