Biosupramolecular Nanowires from Chlorophyll Dyes with Exceptional Charge‐Transport Properties

Sengupta, Sanchita; Ebeling, Daniel; Patwardhan, Sameer; Zhang, Xin; Berlepsch, Hans von; Böttcher, Christoph; Stepanenko, Vladimir; Uemura, Shinobu; Hentschel, Carsten; Fuchs, Harald; Grozema, Ferdinand C.; Siebbeles, Laurens D. A.; Holzwarth, Alfred R.; Chi, Lifeng; Würthner, Frank

doi:10.1002/anie.201201961

Cited by 92 publications

(88 citation statements)

References 38 publications

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“…These features of chlorosomes have led to an enormous interest in their structure-function relationships, because these aggregates might serve as templates for artificial light harvesting. [171][172][173] Previous research has led to various models for the supramolecular structure, proposing tubular, lamellae and rolled lamellae "onion-type" arrangements. [174][175][176][177][178][179][180][181] This diversity reflects the large degree of structural heterogeneity observed for chlorosomes.…”

Section: Green-sulphur Bacteriamentioning

confidence: 99%

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Brixner

Hildner

Köhler

et al. 2017

Advanced Energy Materials

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The transport of excitation energy in molecular aggregates is of crucial importance for the function of organic optoelectronic devices and next‐generation solar cells. First, this review summarizes the theoretical background of the nature of the electronically excited states of molecular aggregates. For these systems, the electronic interaction between the monomers leads to the formation of exciton states. This goes along with a shift of the excitation energies and a redistribution of the oscillator strength with respect to the monomers. Next, a brief overview is provided over experimental techniques that allow to study the properties of excitons in molecular aggregates. This includes single‐molecule spectroscopy, coherent two‐dimensional (2D) spectroscopy, and single‐molecule coherent spectroscopy. Finally, examples of molecular aggregates spanning the range from natural systems that act in photosynthesis as light‐harvesting antennas to artificial aggregates built from synthetic chromophores are illustrated.

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Section: Green-sulphur Bacteriamentioning

confidence: 99%

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Brixner

Hildner

Köhler

et al. 2017

Advanced Energy Materials

Self Cite

302

301

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“…It was already established that the interaction of the hydroxy group and the Zn ion induces the self‐assembly of Chl‐1 and Chl‐2 into π‐stacked aggregates in solution‐based systems . This self‐assembled π‐stacking aggregation processes highly orientated and organized structures in the solid state that have an excellent inherent ability for light‐harvesting and energy transfer . The difference between the Chl‐1 and Chl‐2 molecular structures lies in the esterifying substituents, namely, Chl‐1 features two dodecyl groups, whereas Chl‐2 features a single methyl group .…”

Section: Resultsmentioning

confidence: 99%

“…[41,42] This self-assembled p-stacking aggregation processes highly orientated and organized structures in the solids tate that have an excellent inherent ability for light-harvesting and energy transfer. [43,44] The differenceb etween the Chl-1 and Chl-2 molecular structures lies in the esterifying substituents, namely,C hl-1f eatures two dodecylg roups, whereas Chl-2 features as ingle methyl group. [41] Such as mall variation causes differencesn ot only in the solubility in nonpolar solvents but also on the thin film organization of the moleculest hat form their self-assemblies.…”

Section: Resultsmentioning

confidence: 99%

Dopant‐Free Zinc Chlorophyll Aggregates as an Efficient Biocompatible Hole Transporter for Perovskite Solar Cells

Sasaki

et al. 2016

ChemSusChem

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Chlorophylls (Chls) are abundant, naturally occurring pigments that play key roles in light-harvesting and electron/energy transfer in natural photosynthetic apparatus. To demonstrate the idea that Chls are suitable hole transporters, we employed two Chl derivatives, Chl-1 and Chl-2, which self-assembled readily into π-stacking aggregates through a simple spincasting process, in perovskite solar cells (PSCs). The Chl aggregate films exhibit an ultra-smooth film surface, high hole mobility, appropriate energy levels, and efficient hole injection efficiencies that are all key characteristics for efficient hole transporters in PSCs. CH NH PbI Cl -based PSCs with these Chls as hole transporters were fabricated and compared with P3HT as a standard hole transporter. PSCs based on Chl-1 and Chl-2 without the use of typical additives, such as 4-tert-butylpyridine and lithium bis(trifluoromethanesulfinyl)imide, gave power conversion efficiencies of 11.44 and 8.06 %, respectively. This research provides a unique way to incorporate low-cost and environmentally friendly natural photosynthetic materials in the development of highly efficient photovoltaic devices.

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“…Metal–ligand coordination and host–guest complexation are particularly useful in constructing supramolecular systems. 8−10 Metal–ligand interactions offer various coordination geometries, strong yet tunable binding abilities, 11,12 and unique electronic or magnetic properties. 13−15 For example, strands of DNA can be self-assembled in the presence of copper ions, and controlling the spacing between the ions can impart ferromagnetism to the materials.…”

Section: Introductionmentioning

confidence: 99%

Altering the Peptide Binding Selectivity of Polymeric Reverse Micelle Assemblies via Metal Ion Loading

et al. 2017

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Supramolecular reverse micelle assemblies, formed by amphiphilic copolymers, can selectively encapsulate molecules in their interiors depending on the functional groups present in the polymers. Altering the binding selectivity of these materials typically requires the synthesis of alternate functional groups. Here, we demonstrate that the addition of Zr(IV) ions to the interiors of reverse micelles having phosphonate functional groups transforms the supramolecular materials from ones that selectively bind positively charged peptides into materials that selectively bind phosphorylated peptides. We also show that the binding selectivity of these reverse micelle assemblies can be further tuned by varying the fractions of phosphonate groups in the copolymer structure. The optimized reverse micelle materials can selectively transfer and bind phosphorylated peptides from aqueous solutions over a wide range of pH conditions and can selectively enrich phosphorylated peptides even in complicated mixtures.

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Biosupramolecular Nanowires from Chlorophyll Dyes with Exceptional Charge‐Transport Properties

Cited by 92 publications

References 38 publications

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Dopant‐Free Zinc Chlorophyll Aggregates as an Efficient Biocompatible Hole Transporter for Perovskite Solar Cells

Altering the Peptide Binding Selectivity of Polymeric Reverse Micelle Assemblies via Metal Ion Loading

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