Mr. Kurt De Mey Profile

Kurt De Mey

at KU Leuven

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Proceedings Article | 20 September 2011 Paper

Modeling the hyperpolarizability dispersion with the Thomas-Kuhn sum rules

Kurt De Mey, Javier Perez-Moreno, Koen Clays

Proceedings Volume 8113, 81130V (2011) https://doi.org/10.1117/12.893482

KEYWORDS: Absorption, Nonlinear optics, Chromophores, Molecules, Data modeling, Hyper Rayleigh scattering, Dispersion, Chemistry, Near infrared, Precision calibration

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The continued interest in molecules that possess large quadratic nonlinear optical (NLO) properties has motivated considerable interplay between molecular synthesis and theory. The screening of viable candidates for NLO applications has been a tedious work, much helped by the advent of the hyper-Rayleigh scattering (HRS) technique. The downside of this technique is the low efficiency, which usually means that measurements have to be performed at wavelengths that are close to the molecular resonances, in the visible area. This means generally that one has to extrapolate the results from HRS characterization to the longer wavelengths that are useful for applications. Such extrapolation is far from trivial and the classic 2-level model can only be used for the most straightforward single charge-transfer chromophores. An alternative is the TKSSOS technique, which uses a few input-hyperpolarizabilities and UV-Vis absorption data to calculate the entire hyperpolarizability spectrum. We have applied this TKS-SOS technique on a set of porphyrines to calculate the hyperpolarizability dispersion. We have also built a tunable HRS set up, capable of determining hyperpolarizabilities in the near infrared (up to 1600 nm). This has allowed us to directly confirm the results predicted in the application region. Due to the very sharp transitions in the hyperpolarizability dispersion, the calculation is subjected to a very precise calibration with respect to the input-hyperpolarizabilities, resulting in very accurate predictions for long wavelength hyperpolarizabilities. Our results not only underscribe the aforementioned technique, but also confirm the use of porphyrines as powerful moieties in NLO applications.

Proceedings Article | 18 August 2010 Paper

Analysis of the unusual wavelength dependence of the first hyperpolarizability of porphyrin derivatives

K. De Mey, K. Clays, Michael Therien, David Beratan, Inge Asselberghs

Proceedings Volume 7774, 777403 (2010) https://doi.org/10.1117/12.859819

KEYWORDS: Absorption, Chromophores, Transition metals, Oscillators, Chemical elements, Nonlinear optics, Hyper Rayleigh scattering, Molecules, Supramolecular assemblies, Chemistry

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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 threelevel 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.

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