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Anisotropic Organization and Microscopic Manipulation of Self-Assembling Synthetic Porphyrin Microrods That Mimic Chlorosomes: Bacterial Light-Harvesting Systems

Chappaz-Gillot, Cyril and Marek, Peter L. and Blaive, Bruno J. and Canard, Gabriel and Bürck, Jochen and Garab, Győző and Hahn, Horst and Jávorfi, Tamás and Kelemen, Loránd and Krupke, Ralph and Mössinger, Dennis and Ormos, Pál and Reddy, Chilla Malla and Roussel, Christian and Steinbach, Gábor and Szabó, Milán and Ulrich, Anne S. and Vanthuyne, Nicolas and Vijayaraghavan, Aravind and Zupcanova, Anita and Balaban, Teodor Silviu (2012):
Anisotropic Organization and Microscopic Manipulation of Self-Assembling Synthetic Porphyrin Microrods That Mimic Chlorosomes: Bacterial Light-Harvesting Systems.
134, In: Journal of the American Chemical Society, (2), pp. 944-954, ISSN 0002-7863, [Online-Edition: http://dx.doi.org/10.1021/ja203838p],
[Article]

Abstract

Being able to control in time and space the positioning, orientation, movement, and sense of rotation of nano- to microscale objects is currently an active research area in nanoscience, having diverse nanotechnological applications. In this paper, we demonstrate unprecedented control and maneuvering of rod-shaped or tubular nanostructures with high aspect ratios which are formed by self-assembling synthetic porphyrins. The self-assembly algorithm, encoded by appended chemical-recognition groups on the periphery of these porphyrins, is the same as the one operating for chlorosomal bacteriochlorophylls (BChl's). Chlorosomes, rod-shaped organelles with relatively long-range molecular order, are the most efficient naturally occurring light-harvesting systems.(1, 2) They are used by green photosynthetic bacteria to trap visible and infrared light of minute intensities even at great depths, e.g., 100 m below water surface or in volcanic vents in the absence of solar radiation. In contrast to most other natural light-harvesting systems, the chlorosomal antennae are devoid of a protein scaffold to orient the BChl's; thus, they are an attractive goal for mimicry by synthetic chemists, who are able to engineer more robust chromophores to self-assemble. Functional devices with environmentally friendly chromophores—which should be able to act as photosensitizers within hybrid solar cells, leading to high photon-to-current conversion efficiencies even under low illumination conditions—have yet to be fabricated. The orderly manner in which the BChl's and their synthetic counterparts self-assemble imparts strong diamagnetic and optical anisotropies and flow/shear characteristics to their nanostructured assemblies, allowing them to be manipulated by electrical, magnetic, or tribomechanical forces.

Item Type: Article
Erschienen: 2012
Creators: Chappaz-Gillot, Cyril and Marek, Peter L. and Blaive, Bruno J. and Canard, Gabriel and Bürck, Jochen and Garab, Győző and Hahn, Horst and Jávorfi, Tamás and Kelemen, Loránd and Krupke, Ralph and Mössinger, Dennis and Ormos, Pál and Reddy, Chilla Malla and Roussel, Christian and Steinbach, Gábor and Szabó, Milán and Ulrich, Anne S. and Vanthuyne, Nicolas and Vijayaraghavan, Aravind and Zupcanova, Anita and Balaban, Teodor Silviu
Title: Anisotropic Organization and Microscopic Manipulation of Self-Assembling Synthetic Porphyrin Microrods That Mimic Chlorosomes: Bacterial Light-Harvesting Systems
Language: English
Abstract:

Being able to control in time and space the positioning, orientation, movement, and sense of rotation of nano- to microscale objects is currently an active research area in nanoscience, having diverse nanotechnological applications. In this paper, we demonstrate unprecedented control and maneuvering of rod-shaped or tubular nanostructures with high aspect ratios which are formed by self-assembling synthetic porphyrins. The self-assembly algorithm, encoded by appended chemical-recognition groups on the periphery of these porphyrins, is the same as the one operating for chlorosomal bacteriochlorophylls (BChl's). Chlorosomes, rod-shaped organelles with relatively long-range molecular order, are the most efficient naturally occurring light-harvesting systems.(1, 2) They are used by green photosynthetic bacteria to trap visible and infrared light of minute intensities even at great depths, e.g., 100 m below water surface or in volcanic vents in the absence of solar radiation. In contrast to most other natural light-harvesting systems, the chlorosomal antennae are devoid of a protein scaffold to orient the BChl's; thus, they are an attractive goal for mimicry by synthetic chemists, who are able to engineer more robust chromophores to self-assemble. Functional devices with environmentally friendly chromophores—which should be able to act as photosensitizers within hybrid solar cells, leading to high photon-to-current conversion efficiencies even under low illumination conditions—have yet to be fabricated. The orderly manner in which the BChl's and their synthetic counterparts self-assemble imparts strong diamagnetic and optical anisotropies and flow/shear characteristics to their nanostructured assemblies, allowing them to be manipulated by electrical, magnetic, or tribomechanical forces.

Journal or Publication Title: Journal of the American Chemical Society
Volume: 134
Number: 2
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Fachgebiet Molekulare Nanostrukturen
11 Department of Materials and Earth Sciences > Material Science > Joint Research Laboratory Nanomaterials
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences
Date Deposited: 27 Aug 2012 09:28
Official URL: http://dx.doi.org/10.1021/ja203838p
Identification Number: doi:10.1021/ja203838p
Funders: Partial financial support was granted by the Deutsche Forschungsgemeinschaft through the Center for Functional Nanostructures at the Universität Karlsruhe (Projects C3.5 and C3.5b to S.T.B., E1.2 to A.S.U.). , The collaborative work between Marseille and Karlsruhe was facilitated by the CNRS through PICS No. 3777 allocated to C.R., Funding from the Initiative and Networking Fund of the Helmholtz-Gemeinschaft Deutscher Forschungszentren (VH- NG-126) is acknowledged by R.K. and A.V., This work was in part supported by the Hungarian Scientific Research Fund (OTKA/ NKTH CNK 80345 to G.G., GOP-1.1.2-07/1-2008-0007 to G.S. who thanks Biofotonika R&D Ltd. for additional funding).
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