Abstract
One approach to the experimental determination of the molecular second-order nonlinear polarizability, or the first hyperpolarizability, of fluorescent species by hyper-Rayleigh scattering is based on high-frequency demodulation of the time-delayed fluorescence contribution to the immediate scattering signal [Rev. Sci. Instrum. 69, 2233 (1998)]. For typical fluorescence lifetimes of less than a nanosecond a detection bandwidth of more than 1 GHz is necessary. This bandwidth has not yet been realized. Measurements at successively higher modulation frequencies are performed instead. A fitting of the apparent hyperpolarizability as a function of the modulation frequency then reveals the inherent hyperpolarizability without the fluorescence contribution. An improved fitting function has been derived, resulting in the elimination of a small systematic error and in the reduction of the larger statistical uncertainty in the deduced value. Possible implications of the improved accuracy and precision are discussed.
© 2000 Optical Society of America
Full Article | PDF ArticleMore Like This
Koen Clays, Kurt Wostyn, Geert Olbrechts, André Persoons, Akira Watanabe, Kyoko Nogi, Xuan-Ming Duan, Shuji Okada, Hidetoshi Oikawa, Hachiro Nakanishi, Henryk Vogel, David Beljonne, and Jean-Luc Brédas
J. Opt. Soc. Am. B 17(2) 256-265 (2000)
Geert Olbrechts, Kurt Wostyn, Koen Clays, and André Persoons
Opt. Lett. 24(6) 403-405 (1999)
V. Ostroverkhov, R. G. Petschek, K. D. Singer, L. Sukhomlinova, R. J. Twieg, S.-X. Wang, and L. C. Chien
J. Opt. Soc. Am. B 17(9) 1531-1542 (2000)