Abstract

We report on the extremely large nonresonant quadratic optical nonlinearity of the stilbazolium salt trans-4-(dimethylamino)-N-phenyl-4-stilbazolium hexafluorophosphate (DAPSH). The phenyl-pyridinium chromophores in DAPSH crystals grown from acetone solution pack with a highly aligned polar order, resulting in a very large birefringence, Δn=1.17±0.06 at λ=0.83μm and Δn=0.83±0.04 at λ=1.55μm. More importantly, this leads to an extremely large diagonal quadratic susceptibility with the nonlinear optical coefficient for second-harmonic generation reaching up to d111=290±40pmV at 1.907μm fundamental wavelength, which presents a considerable improvement with respect to the presently best material trans-4-(dimethylamino)-N-methyl-4-stilbazolium tosyate (DAST) with d111=210±55pmV at λ=1.907μm. The result is in agreement with the preferential packing of the chromophores and the previous studies demonstrating higher microscopic nonlinearity of the chromophores in DAPSH compared to that of DAST.

© 2008 Optical Society of America

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