Ultrafast delocalization of excitation in synthetic light-harvesting nanorings

Yong, Chaw-Keong; Parkinson, Patrick; Kondratuk, Dmitry V.; Chen, Wei‐Hsin; Stannard, Andrew; Summerfield, Alex; Sprafke, Johannes K.; O’Sullivan, Melanie C.; Beton, Peter H.; Anderson, Harry L.; Herz, Laura M.

doi:10.1039/c4sc02424a

Cited by 103 publications

(157 citation statements)

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%

Using coherence to enhance function in chemical and biophysical systems

Scholes

Fleming

Chen

et al. 2017

Nature

536

550

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Section: Coherent Excitons Are Prevalent and Robustmentioning

confidence: 81%

Using coherence to enhance function in chemical and biophysical systems

Scholes

Fleming

Chen

et al. 2017

Nature

536

550

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“…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%

Controlling supramolecular polymerization through multicomponent self‐assembly

Besenius

2016

J. Polym. Sci. Part A: Polym. Chem.

122

102

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The self-assembly into supramolecular polymers is a process driven by reversible non-covalent interactions between monomers, and gives access to materials applications incorporating mechanical, biological, optical or electronic functionalities. Compared to the achievements in precision polymer synthesis via living and controlled covalent polymerization processes, supramolecular chemists have only just learned how to developed strategies that allow similar control over polymer length, (co)monomer sequence and morphology (random, alternating or blocked ordering). This highlight article discusses the unique opportunities that arise when coassembling multicomponent supramolecular polymers, and focusses on four strategies in order to control the polymer architecture, size, stability and its stimuli-responsive properties: (1) endcapping of supramolecular polymers, (2) biomimetic templated polymerization, (3) controlled selectivity and reactivity in supramolecular copolymerization, and (4) living supramolecular polymerization. In contrast to the traditional focus on equilibrium systems, our emphasis is also on the manipulation of selfassembly kinetics of synthetic supramolecular systems. V C 2016

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“…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%

Time resolved structural dynamics of butadiyne-linked porphyrin dimers

Camargo

Hall

Anderson

et al. 2016

Structural Dynamics

Self Cite

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In this work, the timescales and mechanisms associated with the structural dynamics of butadiyne-linked porphyrin dimers are investigated through time resolved narrowband pump/broadband probe transient absorption spectroscopy. Our results confirm previous findings that the broadening is partly due to a distribution of structures with different (dihedral) angular conformations. Comparison of measurements with excitations on the red and blue sides of the Q-band unravel the ground and excited state conformational re-equilibration timescales. Further comparison to a planarized dimer, through the addition of a ligand, provides conclusive evidence for the twisting motion performed by the porphyrin dimer in solution.

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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.

Cited by 103 publications

References 54 publications

Using coherence to enhance function in chemical and biophysical systems

Using coherence to enhance function in chemical and biophysical systems

Controlling supramolecular polymerization through multicomponent self‐assembly

Time resolved structural dynamics of butadiyne-linked porphyrin dimers

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