Abstract
The advances made in the design and synthesis of suitable structures with large nonlinear optical coefficients have been, in large part, due to continued development in understanding of the microscopic origins of these phenomena by means of theoretical studies.1-5 These studies have established that the large nonlinearities observed in conjugated organic structures originate from virtual excitations of π-electron states whose properties are determined primarily by the correlated motions of the π-electrons resulting front repulsive Coulomb interactions. The development of the theoretical methodology has led to the calculation of the nonlinear optical properties of numerous organic structures, usually in good agreement with experimental data. We report here theoretical calculations of the second-order optical susceptibilities of two dipolar quinoid molecules having an alternating single and double bond structure and compare them with the results from second harmonic generation (SHG) measurements.
© 1997 Optical Society of America
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