ArticleProceedings of the National Academy of Sciences of the United States of America2009
Zinc chlorins for artificial light-harvesting self-assemble into antiparallel stacks forming a microcrystalline solid-state material.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2009. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 10 papers.
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10 citing papers in PubMed.
- Computational Modeling and Self-Assembly Synthesis of Borazine-Based Free-Standing Molecular-Thin Films.Langmuir : the ACS journal of surfaces and colloids · 2026Article
- Quantum Chemical Simulation of theMolecules (Basel, Switzerland) · 2021Article
- The Assembly of Porphyrin Systems in Well-Defined Nanostructures: An Update.Molecules (Basel, Switzerland) · 2019Review
- Contrasting Modes of Self-Assembly and Hydrogen-Bonding Heterogeneity in Chlorosomes ofThe journal of physical chemistry. C, Nanomaterials and interfaces · 2018Article
- Determination of Controlled Self-Assembly of a Paracrystalline Material by Homology Modelling with Hybrid NMR and TEM.Chemistry (Weinheim an der Bergstrasse, Germany) · 2017Article
- Trefoil factor family 2 expression inhibits gastric cancer cell growth and invasion in vitro via interactions with the transcription factor Sp3.International journal of molecular medicine · 2016Article
- Biosolar cells: global artificial photosynthesis needs responsive matrices with quantum coherent kinetic control for high yield.Interface focus · 2015Review
- Solid-state NMR applied to photosynthetic light-harvesting complexes.Photosynthesis research · 2012Review
- Spectroscopic investigations on the H-type aggregation of coumarin 153 dye molecules: role of Au nanoparticles and γ-cyclodextrin.Journal of fluorescence · 2012Article
- Introduction to theory/modeling methods in photosynthesis.Photosynthesis researchArticle
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8 authors.
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Abstract
We introduce a concept to solve the structure of a microcrystalline material in the solid-state at natural abundance without access to distance constraints, using magic angle spinning (MAS) NMR spectroscopy in conjunction with X-ray powder diffraction and DFT calculations. The method is applied to a novel class of materials that form (semi)conductive 1D wires for supramolecular electronics and artificial light-harvesting. The zinc chlorins 3-devinyl-3(1)-hydroxymethyl-13(2)-demethoxycarbonylpheophorbide a (3',5'-bis-dodecyloxy)benzyl ester zinc complex 1 and 3-devinyl-3(1)-methoxymethyl-13(2)-demethoxycarbonylpheophorbide a (3',5'-bis-dodecyloxy)benzyl ester zinc complex 2, self-assemble into extended excitonically coupled chromophore stacks. (1)H-(13)C heteronuclear dipolar correlation MAS NMR experiments provided the (1)H resonance assignment of the chlorin rings that allowed accurate probing of ring currents related to the stacking of macrocycles. DFT ring-current shift calculations revealed that both chlorins self-assemble in antiparallel pi-stacks in planar layers in the solid-state. Concomitantly, X-ray powder diffraction measurements for chlorin 2 at 80 degrees C revealed a 3D lattice for the mesoscale packing that matches molecular mechanics optimized aggregate models. For chlorin 2 the stacks alternate with a periodicity of 0.68 nm and a 3D unit cell with an approximate volume of 6.28 nm(3) containing 4 molecules, which is consistent with space group P2(1)22(1).
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