Abstract
Squaraines have attracted much research interest because of their large, nonresonant third-order optical susceptibilities γijkl(−ω4; ω1, ω2, ω3).1,2 Evidence has accumulated that a two-level model for γijkl(−ω4; ω1, ω2, ω3). is not adequate even for molecules with negative γijkl(−ω4; ω1, ω2, ω3).. Earlier we discussed the experimental observation of high-lying two-photon states that are critical to the negative γijkl(−ω4; ω1, ω2, ω3). in squaraines, achieved by using femtosecond pump-probe techniques.3 We report here results from our recent full third-harmonic dispersion measurements on squaraine dyes using a tunable picosecond laser source based on optical parametric generation and amplification in KTP crystals pumped by a picosecond Nd:YAG laser.4
© 1995 Optical Society of America
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