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Research Article

Robust excitons inhabit soft supramolecular nanotubes

Dörthe M. Eisele, Dylan H. Arias, Xiaofeng Fu, Erik A. Bloemsma, Colby P. Steiner, Russell A. Jensen, Patrick Rebentrost, Holger Eisele, Andrei Tokmakoff, Seth Lloyd, Keith A. Nelson, Daniela Nicastro, Jasper Knoester, and Moungi G. Bawendi
  1. aCenter for Excitonics and Department of Chemistry and
  2. dDepartment of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139;
  3. bBiology Department, Rosenstiel Basic Medical Science Research Center, Brandeis University, Waltham, MA 02454;
  4. cInstitute for Theoretical Physics and Zernike Institute for Advanced Materials, University of Groningen, NL-9747 AG, Groningen, The Netherlands;
  5. eInstitut für Festkörperphysik, Technische Universität Berlin, 103623 Berlin, Germany; and
  6. fDepartment of Chemistry, University of Chicago, Chicago, IL 60637

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PNAS August 19, 2014 111 (33) E3367-E3375; first published August 4, 2014; https://doi.org/10.1073/pnas.1408342111
Dörthe M. Eisele
aCenter for Excitonics and Department of Chemistry and
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  • For correspondence: Eisele@ccny.cuny.edu Nicastro@brandeis.edu J.Knoester@rug.nl MGB@mit.edu
Dylan H. Arias
aCenter for Excitonics and Department of Chemistry and
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Xiaofeng Fu
bBiology Department, Rosenstiel Basic Medical Science Research Center, Brandeis University, Waltham, MA 02454;
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Erik A. Bloemsma
cInstitute for Theoretical Physics and Zernike Institute for Advanced Materials, University of Groningen, NL-9747 AG, Groningen, The Netherlands;
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Colby P. Steiner
aCenter for Excitonics and Department of Chemistry and
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Russell A. Jensen
aCenter for Excitonics and Department of Chemistry and
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Patrick Rebentrost
dDepartment of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139;
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Holger Eisele
eInstitut für Festkörperphysik, Technische Universität Berlin, 103623 Berlin, Germany; and
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Andrei Tokmakoff
fDepartment of Chemistry, University of Chicago, Chicago, IL 60637
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Seth Lloyd
dDepartment of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139;
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Keith A. Nelson
aCenter for Excitonics and Department of Chemistry and
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Daniela Nicastro
bBiology Department, Rosenstiel Basic Medical Science Research Center, Brandeis University, Waltham, MA 02454;
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  • For correspondence: Eisele@ccny.cuny.edu Nicastro@brandeis.edu J.Knoester@rug.nl MGB@mit.edu
Jasper Knoester
cInstitute for Theoretical Physics and Zernike Institute for Advanced Materials, University of Groningen, NL-9747 AG, Groningen, The Netherlands;
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  • For correspondence: Eisele@ccny.cuny.edu Nicastro@brandeis.edu J.Knoester@rug.nl MGB@mit.edu
Moungi G. Bawendi
aCenter for Excitonics and Department of Chemistry and
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  • For correspondence: Eisele@ccny.cuny.edu Nicastro@brandeis.edu J.Knoester@rug.nl MGB@mit.edu
  1. Contributed by Moungi G. Bawendi, May 30, 2014 (sent for review December 2, 2013)

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Significance

The scientific community has been broadly inspired by tiny deep-sea bacteria, the green sulfur bacteria, that are able to harvest minute amounts of incoming sunlight with exquisite efficiency. Nature’s masterpiece consists of soft, cylindrical-shaped, supramolecular structures that are densely packed in superstructures. Only little is known about the fundamental processes that govern nature’s efficiency. Here we unravel, for the first time to our knowledge, the impact of structural complexity through the use of a model system akin to that found in nature, focusing on the properties that are prerequisite for nature’s efficient light harvesting. Our work suggests that the cylindrical geometry presents a rational design that may be key for protecting the system’s quantum properties upon dense packing.

Abstract

Nature's highly efficient light-harvesting antennae, such as those found in green sulfur bacteria, consist of supramolecular building blocks that self-assemble into a hierarchy of close-packed structures. In an effort to mimic the fundamental processes that govern nature’s efficient systems, it is important to elucidate the role of each level of hierarchy: from molecule, to supramolecular building block, to close-packed building blocks. Here, we study the impact of hierarchical structure. We present a model system that mirrors nature’s complexity: cylinders self-assembled from cyanine-dye molecules. Our work reveals that even though close-packing may alter the cylinders’ soft mesoscopic structure, robust delocalized excitons are retained: Internal order and strong excitation-transfer interactions—prerequisites for efficient energy transport—are both maintained. Our results suggest that the cylindrical geometry strongly favors robust excitons; it presents a rational design that is potentially key to nature’s high efficiency, allowing construction of efficient light-harvesting devices even from soft, supramolecular materials.

  • supramolecular assembly
  • self-assembled excitonic nanoscale systems
  • photosynthesis
  • exciton theory
  • light-harvesting antennae systems

Footnotes

  • ↵1To whom correspondence may be addressed. Email: Eisele{at}ccny.cuny.edu, Nicastro{at}brandeis.edu, J.Knoester{at}rug.nl, or MGB{at}mit.edu.
  • Author contributions: D.M.E. and M.G.B. developed and guided the project; D.M.E. prepared shock-frozen samples for cryo-EM/ET, prepared samples for nonlinear spectroscopy, and performed linear spectroscopy experiments; D.H.A. performed linear dichroism and nonlinear spectroscopy experiments and data analysis with input and support from D.M.E. and C.P.S. and guidance from A.T. and K.A.N.; X.F. recorded and processed cryo-EM/ET data; D.M.E., X.F., and D.N. analyzed cryo-EM/ET data; E.A.B. performed spectral simulations in collaboration with D.M.E. supervised by J.K.; R.A.J. built the fast-acquisition absorption spectrometer and performed flash-dilution measurements with D.M.E.; P.R. performed exciton dynamic simulations in collaboration with D.M.E and S.L.; H.E. provided fundamental contributions to the discussion on the structure analysis and simulated illustrations for the bundle structure; all authors provided fruitful discussions and interpretations of the data and analyses; J.K. provided essential interpretation of optical data, particularly in the context of exciton theory; and D.M.E., S.L., J.K., and M.G.B. wrote the paper, with input from all authors.

  • The authors declare no conflict of interest.

  • This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.1073/pnas.1408342111/-/DCSupplemental.

Freely available online through the PNAS open access option.

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Robust excitons inhabit soft supramolecular tubes
Dörthe M. Eisele, Dylan H. Arias, Xiaofeng Fu, Erik A. Bloemsma, Colby P. Steiner, Russell A. Jensen, Patrick Rebentrost, Holger Eisele, Andrei Tokmakoff, Seth Lloyd, Keith A. Nelson, Daniela Nicastro, Jasper Knoester, Moungi G. Bawendi
Proceedings of the National Academy of Sciences Aug 2014, 111 (33) E3367-E3375; DOI: 10.1073/pnas.1408342111

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Robust excitons inhabit soft supramolecular tubes
Dörthe M. Eisele, Dylan H. Arias, Xiaofeng Fu, Erik A. Bloemsma, Colby P. Steiner, Russell A. Jensen, Patrick Rebentrost, Holger Eisele, Andrei Tokmakoff, Seth Lloyd, Keith A. Nelson, Daniela Nicastro, Jasper Knoester, Moungi G. Bawendi
Proceedings of the National Academy of Sciences Aug 2014, 111 (33) E3367-E3375; DOI: 10.1073/pnas.1408342111
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