Abstract
The recent observations of second harmonic generation (SHG) of the infrared (IR) light in doped silica glass fibers,1,2 planar waveguides,3,4 and poled silica glass5 have attracted a great deal of attention in understanding the mechanism and origin of nonlinear optical (NLO) processes in a-SiO2. A number of possible mechanisms have been proposed6,7 to explain the experimental observations. However, in so far as these phenomenological models describe the observed SHG in fibers and waveguides, they do not address the microscopic mechanism of optical nonlinearity in silica glass. An understanding of the atomic-scale mechanism of NLO properties in a-SiO2 is important, not only for increasing our fundamental knowledge, but also for modeling new materials with yet enhanced optical susceptibility and faster response time for device applications. Here we present the results of first-ever ab initio studies of microscopic structure-NLO property relationships in systems containing free spin electrons, such as a-SiO2.
© 1995 Optical Society of America
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