2015
DOI: 10.1039/c4sc02424a
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Ultrafast delocalization of excitation in synthetic light-harvesting nanorings

Abstract: When light is absorbed by a nanoring consisting of 6–24 porphyrin units, the excitation delocalizes over the whole molecule within 200 fs. Highly symmetric nanorings exhibit thermally enhanced super-radiance.

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Cited by 103 publications
(157 citation statements)
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References 54 publications
(120 reference statements)
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“…Energetic disorder disrupts these perfect wavelike properties underpinning exciton states, thereby diminishing their delocalization through space 12,58 . Delocalization competing with localization is seen in experimental data and is well illustrated by recent studies of various supramolecular systems [59][60][61] as well as in natural ring-shaped light-harvesting complexes from purple bacteria 62 . Superradiance is the collective fluorescence emission from two or more interacting chromophores, which lead to shorter radiative rates (analogously to coherent backscattering).…”
Section: Coherent Excitons Are Prevalent and Robustmentioning
confidence: 81%
“…Energetic disorder disrupts these perfect wavelike properties underpinning exciton states, thereby diminishing their delocalization through space 12,58 . Delocalization competing with localization is seen in experimental data and is well illustrated by recent studies of various supramolecular systems [59][60][61] as well as in natural ring-shaped light-harvesting complexes from purple bacteria 62 . Superradiance is the collective fluorescence emission from two or more interacting chromophores, which lead to shorter radiative rates (analogously to coherent backscattering).…”
Section: Coherent Excitons Are Prevalent and Robustmentioning
confidence: 81%
“…208 These synthetic p-conjugated nanorings were further shown to mimic the ultrafast energy transfer and delocalization observed in natural light-harvesting systems. 209,210 Single-stranded DNA (ssDNA) can be used as a template to control the self-assembly of synthetic amphiphiles into onedimensional supramolecular polymers and nanofibers. 211,212 Hydrogen-bonding of amphiphilic building blocks to the DNA strand thereby produces uniform hierarchical structures, which has been a powerful approach to self-assemble p-conjugated amphiphiles.…”
Section: Biomimetic Templated Polymerizationmentioning
confidence: 99%
“…Indeed, great progress has been made towards synthesizing conjugated porphyrin multi-chromophore structures tailored specifically for energy materials related applications 5 . However, extended chromophoric structures inevitably present conformational heterogeneity that can act as an energy or charge sink.…”
Section: Introductionmentioning
confidence: 99%