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271.
S(0), S(1), and T(1) states of various orthogonal 8,8' and 8,2'-bis-boradiaza-s-indacene (BODIPY) dyes, recently (Angew. Chem., Int. Ed.2011, 50, 11937) proposed as heavy atom free photosensitizers for O(2)((1)Δ(g)) generation, were studied by multireference quantum chemical approaches. S(0)→S(1) excitation characteristics of certain bis-BODIPYs are shown to be drastically different than the parent BODIPY chromophore. Whereas a simple HOMO→LUMO-type single substitution perfectly accounts for the BODIPY core, S(1) states of certain orthogonal bis-BODIPYs are described as linear combinations of doubly substituted (DS) configurations which overall yield four electrons in four singly occupied orbitals. Computed DS character of S(1), strongly correlated with facile (1)O(2) production, was presumed to occur via S(1)→T(1) intersystem crossing (ISC) of the sensitizer. Further confirmation of this relation was provided by newly synthesized BODIPY derivatives and comparison of spectroscopic properties of their dimers and monomers. Near-IR absorption, desired for potential photodynamic therapy applications, was not pursuable for bis-chromophores by the standard strategy of π-extension, as DS singlet states are destabilized. Decreased exchange coupling in π-extended cases appears to be responsible for this destabilization. Comparisons with iodine incorporated bis-BODIPYs suggest that the dynamics of (1)O(2) generation via DS S(1) states are qualitatively different from that via ISC originating from heavy atom spin-orbit coupling. Although red-shifting the absorption wavelength to enter the therapeutic window does not seem attainable for orthogonal bis-BODIPYs with DS S(1) states, modifications in the chromophore cores are shown to be promising in fine-tuning the excitation characteristics. 相似文献
272.
Daniela Lürding Yavuz Ba
ar Ulrike Hansktter 《International Journal of Solids and Structures》2001,38(52)
The contribution deals with an extension of a classical Neo–Hookean model for compressible isotropic materials to transverse isotropy. With this enhancement for one preferred material direction there is a possibility to simulate large strains in volume changes of the isotropic basic continuum and supplementary in fiber direction. The integrity basis of polynomial invariants in case of transversely isotropic hyperelasticity consists of three principal invariants of the isotropic basic continuum and additionally of two principal invariants for the preferred material direction. The proposed stored energy function for transverse isotropy contains the classical theory near to the natural state and fulfills the restriction on polyconvexity and coerciveness.By numerical enforcement of the material model into shell kinematics without rotational variables a four-node isoparametric finite element is developed using special concepts to avoid locking. The capability of the algorithms proposed is demonstrated by a numerical example involving large strains as well as finite rotations. 相似文献
273.