Abstract

Linear and quadratic nonlinear-optical (NLO) properties of a new organic–inorganic crystal, 2-amino-5-nitro-pyridinium-dihydrogen phosphate (2A5NPDP), are reported. 2A5NPDP was designed to display high NLO efficiency by incorporating highly polarizable organic molecules arranged in a polar order between phosphate polyanion sheets. The material is transparent in the visible and the near-IR (from 0.42 to 2 μm) with favorable phase-matching (PM) conditions for second-harmonic generation in the 1-μm region. Crystal nonlinear coefficients responsible for PM were determined by the Maker fringe method, leading at 1.06 μm to d15 ≅ 7.2 pm/V and d24 ≅ 1.3 pm/V. The measured crystal coefficients significantly depart from oriented gas model calculations based on molecular hyperpolarizability values measured in an aprotic solution, thus suggesting important crystal-field effects and protonation contributions. Thermal sensitivity of the PM angle at 1.34 μm is found to be 155″/°C, which is considerably larger than typical values of inorganic NLO crystals and opens the way to efficient thermal tuning of phase-matched processes.

© 1992 Optical Society of America

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