Linear and nonlinear optical susceptibilities and hyperpolarizability of borate LiNaB4O7 single crystals: Theory and experiment J. Appl. Phys. 112, 053526 (2012) Effect of Lorentz local field for optical second order nonlinear susceptibility in ZnO nanorod J. Appl. Phys. 111, 103112 (2012) Size dependent optical properties of the CdSe-CdS core-shell quantum dots in the strong confinement regime J. Appl. Phys. 111, 074312 (2012) Methyl groups at dielectric and metal surfaces studied by sum-frequency generation in co-and counterpropagating configurations J. Chem. Phys. 135, 044704 (2011) The third-order nonlinear optical coefficients of Si, Ge, and Si1−xGex in the midwave and longwave infrared J. Appl. Phys. 110, 011301 (2011) Additional information on J. Appl. Phys. The structural origin of the nonlinear optical susceptibility (/v (3) /) of lead-niobium-germanate film glasses with large Nb 2 O 5 contents has been investigated. /v (3) / shows a strong enhancement with the Nb content in the films with /v (3) / values close to 2 Â 10 À11 esu at 800 nm for a Nb content as high as 0.71. Boling-Glass-Owyoung and Lines' semiempirical models predict accurately the values of /v (3) / for transparent bulk glasses but not for film glasses. This discrepancy is related to the remarkable structural differences between them. Raman spectroscopy suggests the formation of a three-dimensional (3D) structure of [NbO 6 ] octahedra in the case of film glasses having large Nb contents, while X-ray photoelectron spectroscopy shows that a significant fraction of these units contain Nb 4þ ions. The combination of a 3D structure of [NbO 6 ] with the presence of Nb 4þ polarons and their migration through electron intervalence transfer is proposed as the origin of the observed enhancement of /v (3) / in the film glasses.