Abstract
The linear and nonlinear optical properties of six pyridinium-betaines of squaric acid were characterized by means of electro-optical absorption measurements (EOAM) in dioxane solution. All chromophores studied exhibit intense absorption bands in the visible region within 372–441 nm, accompanied with decrease in dipole moment upon excitation. The static hyperpolarizabilities of the NLO-phores studied depend strongly on the substituent in the pyridinium ring and increase significantly going from donor to acceptor substituent. Specifically, the noncentrosymmetrically crystallizing 4-benzoyl compound showed the highest static hyperpolarizability. These empirical trends were supported and verified by quantum-chemical calculations (DFT and ab initio RHF). Bulk crystal properties such as decomposition points within the high temperature range 480–665 K and improved thermal stability in melt demonstrate the advantage of these materials for nonlinear optical applications.
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