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Abstract
Single-crystalline vanadyl phthalocyanine film has been grown by the molecular-beam epitaxy technique. The χ(3) components, χ111 and χ1111, have been determined by third-harmonic generation using a fundamental Nd:YAG laser source. The relation, χ1221∼0.8χ1111, reveals that the nondiagonal component significantly contributes to the nonlinear optical response, which originates in two-dimensional π-electron system of this molecule.
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