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Journal Article

Light-induced charge separation in densely packed donor acceptor coordination cages

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Ahrens,  J.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Schwarzer,  D.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Citation

Frank, M., Ahrens, J., Bejenke, I., Krick, M., Schwarzer, D., & Clever, G. H. (2016). Light-induced charge separation in densely packed donor acceptor coordination cages. Journal of the American Chemical Society, 138(26), 8279-8287. doi:10.1021/jacs.6b04609.


Cite as: http://hdl.handle.net/11858/00-001M-0000-002B-192A-7
Abstract
Photon-powered charge separation is achieved in a supramolecular architecture based on the dense packing of functional building blocks. Therefore, self-assembled dimers of interpenetrated coordination cages consisting of redoxactive chromophors were synthesized in a single assembly step starting from easily accessible ligands and Pd(II) cations. Two backbones consisting of electron rich phenothiazine (PTZ) and electron deficient anthraquinone (ANQ) were used to assemble either homo-octameric or mixed-ligand double cages. The electrochemical and spectroscopic properties of the pure cages, mixtures of donor and acceptor cages and the mixed-ligand cages were compared by steady-state UV-vis and transient absorption spectroscopy, supported by cyclic voltammetry and spectroelectrochemistry. Only the mixed-ligand cages, allowing close intra-assembly communication between the donors and acceptors, showed the characteristic PTZ radical cation and ANQ radical anion features upon excitation in the transient spectra. In contrast, excitation of the mixtures of the homo-octameric donor and acceptor cages in solution did not lead to any signs of electron transfer. Densely packed photo- and redox-functional self-assemblies promise molecular-level control over the morphology of the charge separation layer in future photovoltaic applications.