Abstract
Two-photon absorption (2PA) and subsequent processes may be localized in space with a tightly focused laser beam. This property is used in a wide range of applications, including three dimensional data storage. We report theoretical studies of 5 conjugated chromophores experimentally shown to have large 2PA cross-sections. We use the Time Dependent Density Functional Theory (TD-DFT) to describe the electronic structure. The third order coupled electronic oscillator formalism is applied to calculate frequency-dependent second order hyperpolarizability. Alternatively, the sum over states formalism using state-to-state transition dipoles provided by the a posteriori Tamm-Dancoff approximation is employed. It provides new venues for qualitative interpretation and rational design of 2PA chromophores.
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Tafur, S., Mikhailov, I.A., Belfield, K.D., Masunov, A.E. (2009). Predictions of Two Photon Absorption Profiles Using Time-Dependent Density Functional Theory Combined with SOS and CEO Formalisms. In: Allen, G., Nabrzyski, J., Seidel, E., van Albada, G.D., Dongarra, J., Sloot, P.M.A. (eds) Computational Science – ICCS 2009. ICCS 2009. Lecture Notes in Computer Science, vol 5545. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-01973-9_20
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DOI: https://doi.org/10.1007/978-3-642-01973-9_20
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