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The second-order hyperpolarizability (beta) of pyridinium cations with cutoff (lambdaco) shorter than 400 nm were studied by semiempirical calculation and the hyper-Rayleigh scattering (HRS) technique. The beta value of 4-dimethylaminopyridinium (lambdaco = 390 nm) was evaluated to be about 1.5 times larger than that of p-nitroaniline (lambdaco = 473 nm) in methanolic solution using 1064 nm light as a fundamental beam.
