The determination of first hyperpolarizabilities β using hyper-Rayleigh scattering: a caveat
✍ Scribed by Marinus C. Flipse; Roel de Jonge; Richard H. Woudenberg; Albert W. Marsman; Cornelis A. van Walree; Leonardus W. Jenneskens
- Publisher
- Elsevier Science
- Year
- 1995
- Tongue
- English
- Weight
- 427 KB
- Volume
- 245
- Category
- Article
- ISSN
- 0009-2614
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✦ Synopsis
A comparison of first hyperpolarizabilities /3 determined by hyper-Rayleigh scattering (HRS; /3HRS) and electric field-induced second-harmonic generation (EFISH; /3E~aSn) for a series of donor-acceptor substituted ~r-conjugated organic compounds shows a marked discrepancy between /3H~ and /3E~aSH values for NLO-chromophores which fluoresce in the frequency-doubled wavelength region (532 nm). For MONS and DANS it is unequivocally established that two-photon absorption (TPA) at the fundamental wavelength (1064 nm) occurs followed by Stokes and anti-Stokes fluorescence around the second-harmonic wavelength. Hence, hyper-Rayleigh scattering at 1064 nm is not suited to determining the /3 of these fluorescent NLO-chromophores.
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We provide an improved method for measuring the first order hyperpolarizability of organic nonlinear optical materials in solution by the hyper-Rayleigh scattering technique. The method is free from the overestimation which is encountered in the conventional method due to the fluorescence induced by
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