Structural aspects of nonlinear optics: optical properties of K2H(IO3)2Cl and related compounds

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Abstract
Linear and nonlinear optical properties of dipotassium hydrogen di-iodate chloride K2H(IO3)2Cl have been measured and are compared with other crystalline systems containing I—O bonds. The nonlinear coefficients d333, d311, d113 and d322 relative to d123 of KH2PO4 are 11.0, 2.1, 2.2 and 0.12, respectively. Microscopic modelling in terms of bonds and lone pairs shows that the major source of the observed nonlinearities (d values) is due to the iodine lone pair and the short iodine-oxygen bond of ∼0.18 nm, rather than to the longer range interactions (∼0.3 nm) between the ions themselves. It is further shown that the 12 nonlinear coefficients from five different crystal systems containing IO– 3 and IO2 F– 2 ions may be geometrically related to only one microscopic polarizability (βijk) with components β∥ and β⊥ which are (15.0 ± 1.5)× 10–40 m4 V–1 and (4.2 ± 0.4)× 10–40 m4 V–1 respectively. Nonlinear coefficients are also predicted for crystalline NH4IO3 and XeO3. The fact that we find a non-negligible β⊥ term is in disagreement with current theoretical models which maintain that β∥≫β⊥.

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