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A dual-wavelength polarimetric technique at 633 and 661 nm has been used for the characterization of a nonlinear lithium triborate (LiB3O5) nonenantiomorphous biaxial crystal. The mismatch of the crystallographic and optical coordinate systems was taken into account. The optical rotatory power for light propagation along one of the optical axes is ρ = 7.06° mm−1. The gyration tensor component along the bisector between the x and y crystallographic axes has been measured as g12 = 4.31 × 10−5. Computed values based on the crystalline structure and electronic polarizabilities are in good agreement with those obtained experimentally.

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