Publications [#231891] of David N. Beratan

Journal Articles

1. De Mey, K; Clays, K; Therien, MJ; Beratan, DN; Asselberghs, I, Analysis of the unusual wavelength dependence of the first hyperpolarizability of porphyrin derivatives, Proceedings of SPIE - The International Society for Optical Engineering, vol. 7774 (October, 2010), SPIE, ISSN 0277-786X [doi]
   (last updated on 2024/04/24)

   Abstract:
   Successfully predicting the frequency dispersion of electronic hyperpolarizabilities is an unresolved challenge in materials science and electronic structure theory. It has been shown1 that the generalized Thomas-Kuhn sum rules combined with linear absorption data and measured hyperpolarizabilities at one or two frequencies, may be used to predict the entire frequency-dependent electronic hyperpolarizability spectrum. This treatment includes two- and three-level contributions that arise from the lowest two or three excited state manifolds, enabling us to describe the unusual observed frequency dispersion of the dynamic hyperpolarizability in high oscillator strength M-PZn chromophores, where (porphinato)zinc(II) (PZn) and metal(II)polypyridyl (M) units are connected via an ethyne unit that aligns the high oscillator strength transition dipoles of these components in a head-to-tail arrangement. Importantly, this approach provides a quantitative scheme to use linear optical absorption spectra and very few individual hyperpolarizability values to predict the entire frequency-dependent nonlinear optical response. In addition we provide here experimental dynamic hyperpolarizability values determined by hyper-Rayleigh scattering that underscore the validity of our approach. © 2010 SPIE.