Long-range molecular order as an efficient strategy for light harvesting in photosynthesis

Fetisova, Z. G.; Freiberg, Arvi; Timpmann, K. E.

doi:10.1038/334633a0

Cited by 112 publications

(58 citation statements)

References 16 publications

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“…43 This contribution provides a guideline of how exciton motion in supramolecular systems can be studied, despite the limits currently set for connecting experimental and theoretical state- of-the-art methodologies. Though we report on an artificial light harvester that self-assembles in aqueous solution, it is inspiring to think about likely functional analogies to tubular complexes occurring in nature, 6,44 which, similarly, do not require any structural templates. A forthcoming work that compares experimental results from single-as well as double-quantum 2D electronic spectroscopy 45,46 against refined calculations is in progress.…”

Section: Discussionmentioning

confidence: 99%

Excitons and Disorder in Molecular Nanotubes: A 2D Electronic Spectroscopy Study and First Comparison to a Microscopic Model

et al. 2010

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The efficiency of natural light-harvesting complexes relies on delocalization and directed transfer of excitation energy on spatially well-defined arrangements of molecular absorbers. Coherent excitation delocalization and long-range molecular order are also central prerequisites for engineering energy flows in bioinspired devices. Double-wall cylindrical aggregates have emerged as excellent candidates that meet these criteria. So far, the experimental signatures of exciton relaxation in these tubular supramolecules could not be linked to models encompassing their entire spatial structure. On the basis of the power of two-dimensional electronic spectroscopy, we characterize the motion of excitons in the three-fold band structure of the bitubular aggregate C8S3 through temporal, energetic, and spatial attributes. Accounting for intra-as well as interwall electronic interactions in the framework of a Frenkel exciton basis, we employ numerical computations using inhomogeneous and homogeneous microscopic models. The calculations on large but finite structures identify disorder-induced effects, which become increasingly relevant for higher energy states and give insight into the topology of the excited state manifold. Calculations in the infinite homogeneous limit capture the phenomena evidenced in the experimental two-dimensional patterns. Our results provide a basis for understanding recently reported correlated fluctuations of excitonic absorption bands and interband coherences in tubular aggregates.

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Section: Discussionmentioning

confidence: 99%

Excitons and Disorder in Molecular Nanotubes: A 2D Electronic Spectroscopy Study and First Comparison to a Microscopic Model

et al. 2010

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“…the exciton level structure with intensive higher levels [7][8][9] and polarization of all levels parallel to the long axis of the chlorosome [6,13] (Fig. 1).…”

Section: Resultsmentioning

confidence: 99%

“…the number of rod layers. That is why the published values of BChl c fluorescence decay in whole cells exhibit lifetimes in a rather wide range, from 12 ps to ,~ 40 ps ( [6,15,16]; this work).…”

Section: Z Fetisova Et Al/febs Letters 383 (1996)mentioning

confidence: 96%

“…Spectrally resolved fluorescence measurements for intact cells of C aurantiacus were made with a picosecond spectrochronograph [6]. The pulse source was a mode-locked CW rhodamine 590 dye laser (pulse duration, 3 ps), synchronously pumped at 76 MHz by a NdYag laser (Ontares, 'Coherent').…”

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confidence: 99%

“…Micrographs of the ultrathin sections were used for morphometric measurements (magnification 50 000 × 10) to obtain histograms of chlorosomes heights and calculate the number of layers of rod elements in the chlorosome, assuming that the diameter of the rod equals 5.5 nm [4,5].Absorption spectra of intact cells were recorded with a Hitachi-557 spectrophotometer (Japan).Spectrally resolved fluorescence measurements for intact cells of C aurantiacus were made with a picosecond spectrochronograph [6]. The pulse source was a mode-locked CW rhodamine 590 dye laser (pulse duration, 3 ps), synchronously pumped at 76 MHz by a NdYag laser (Ontares, 'Coherent').…”

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confidence: 99%

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Antenna size dependent exciton dynamics in the chlorosomal antenna of the green bacterium Chloroflexus aurantiacus

Fetisova¹,

Freiberg²,

Novoderezhkin³

et al. 1996

FEBS Letters

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aldehyde, postfixed with OsO4, embedded in Epon-812, and ultrathinsectioned by standard method [4]. Micrographs of the ultrathin sections were used for morphometric measurements (magnification 50 000 × 10) to obtain histograms of chlorosomes heights and calculate the number of layers of rod elements in the chlorosome, assuming that the diameter of the rod equals 5.5 nm [4,5].Absorption spectra of intact cells were recorded with a Hitachi-557 spectrophotometer (Japan).Spectrally resolved fluorescence measurements for intact cells of C aurantiacus were made with a picosecond spectrochronograph [6]. The pulse source was a mode-locked CW rhodamine 590 dye laser (pulse duration, 3 ps), synchronously pumped at 76 MHz by a NdYag laser (Ontares, 'Coherent'). Emission, viewed at an angle of 90 ° to the exciting beam, was registered with a home-made synchroscan streak camera. The time resolution of the measuring system was 10 ps.

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Light‐Harvesting Nanotubes Formed by Supramolecular Assembly of Aromatic Oligophosphates

2016

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A 2,7‐disubstituted phosphodiester‐linked phenanthrene trimer forms tubular structures in aqueous media. Chromophores are arranged in H‐aggregates. Incorporation of small quantities of pyrene results in the development of light‐harvesting nanotubes in which phenanthrenes act as antenna chromophores and pyrenes as energy acceptors. Energy collection is most efficient after excitation at the phenanthrene H‐band. Fluorescence quantum yields up to 23 % are reached in pyrene doped, supramolecular nanotubes.

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Long-range molecular order as an efficient strategy for light harvesting in photosynthesis

Cited by 112 publications

References 16 publications

Excitons and Disorder in Molecular Nanotubes: A 2D Electronic Spectroscopy Study and First Comparison to a Microscopic Model

Excitons and Disorder in Molecular Nanotubes: A 2D Electronic Spectroscopy Study and First Comparison to a Microscopic Model

Antenna size dependent exciton dynamics in the chlorosomal antenna of the green bacterium Chloroflexus aurantiacus

Light‐Harvesting Nanotubes Formed by Supramolecular Assembly of Aromatic Oligophosphates

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