A two-beam second-harmonic generation technique is developed to calibrate the magnitude of the second-order nonlinear optical susceptibility components of surface and bulk (multipolar origin) of isotropic materials. The values obtained for fused silica calibrated against ChiXXX of crystalline quartz are chi parallel parallel perpendicular = 7.9(4), chi perpendicular parallel parallel (+)gamma = 3.8(4), parallel perpendicular perpendicular perpendicular(+)gamma = 59(4), and delta' = 7.8(4) in units of 10(-22) m(2)/V. Similar values are obtained for BK7 glass. An alternative way of calibration against ChiXYZ of quartz is demonstrated. The technique could also be extended to characterize the susceptibility tensor of crystals as a convenient alternative to the Maker-fringe technique.
We use two-beam second-harmonic generation to perform a quantitative tensor analysis of the effective dipolar surface nonlinearity and the separable multipolar bulk nonlinearity for BK7 glass. The most straightforward, self-consistent interpretation of the results is obtained when the effective surface response is assumed to have approximate Kleinman symmetry and the bulk contribution is dominated by magnetic, rather than quadrupole, effects.
We show that nonlinear optical signals generated by non-phase-matched interactions are strongly suppressed when the interaction volume is finite and localized deep inside the bulk of a homogeneous material, as opposed to the case where the interaction volume extends across a boundary of the material. The suppression in the bulk originates from destructive interference between the signals generated in the two regions where the interaction is gradually turned on and off and depends on the ratio of the coherence length to the characteristic length of the interaction volume.
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