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Enhanced energy transport in genetically engineered excitonic networks

Nature Materials volume 15, pages 211–216 (2016)Cite this article

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Abstract

One of the challenges for achieving efficient exciton transport in solar energy conversion systems is precise structural control of the light-harvesting building blocks. Here, we create a tunable material consisting of a connected chromophore network on an ordered biological virus template. Using genetic engineering, we establish a link between the inter-chromophoric distances and emerging transport properties. The combination of spectroscopy measurements and dynamic modelling enables us to elucidate quantum coherent and classical incoherent energy transport at room temperature. Through genetic modifications, we obtain a significant enhancement of exciton diffusion length of about 68% in an intermediate quantum-classical regime.

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Figure 1: Molecular models of the genetically engineered M13 viruses.
Figure 2: Steady-state spectra and fluorescence quenching at room temperature.
Figure 3: Steady-state fluorescence data at room temperature showing exciton harvesting.
Figure 4: Transient-absorption spectra at room temperature.
Figure 5: Comparison of numerical simulations of classical and quantum transport theories for M13SF to the experiment.

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Acknowledgements

This work was supported from Eni, S.p.A. (Italy) through the MIT Energy Initiative Program. H.P. thanks Kwanjeong Educational Foundation for its financial support, and G. W. Hwang for allowing us to use a fluorometer. F.C. has been supported by EU FP7 Marie-Curie Programme (Career Integration Grant) and by MIUR-FIRB grant (Project No. RBFR10M3SB).

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Author notes

  1. Heechul Park and Nimrod Heldman: These authors contributed equally to this work.

Authors and Affiliations

  1. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA

    Heechul Park, Nimrod Heldman & Angela M. Belcher

  2. The David H. Koch Institute for Integrative Cancer Research, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA

    Heechul Park, Nimrod Heldman & Angela M. Belcher

  3. Department of Biological Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA

    Nimrod Heldman, Hannah C. Johnsen & Angela M. Belcher

  4. Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA

    Patrick Rebentrost, Masoud Mohseni & Seth Lloyd

  5. Research Center for Non-Conventional Energy, Istituto eni Donegani, eni S.p.A., Novara 28100, Italy

    Luigi Abbondanza, Andrea Alessi, Mario Salvalaggio, Roberto Fusco & Petra F. Scudo

  6. European Laboratory for Non-linear Spectroscopy, University of Florence, Sesto Fiorentino 50019, Italy

    Alessandro Iagatti, Barbara Patrizi, Laura Bussotti, Filippo Caruso & Paolo Foggi

  7. INO CNR, Sesto Fiorentino 50019, Italy

    Alessandro Iagatti & Paolo Foggi

  8. QSTAR and Department of Physics and Astronomy, University of Florence, Florence 50125, Italy

    Filippo Caruso

  9. Department of Chemistry, University of Perugia, Perugia 06123, Italy

    Paolo Foggi

  10. Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA

    Seth Lloyd

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  1. Heechul Park
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Contributions

H.P., N.H., P.F.S., M.M., R.F., S.L. and A.M.B. conceived the work. P.F.S., P.F., S.L. and A.M.B. supervised the overall work. H.P. and N.H. designed the experiments including protocols. H.P. prepared all the samples, performed the spectroscopic measurements, analysed the data, and interpreted the data with classical Förster theory. H.P. wrote a first version of the manuscript, based on which H.P., P.R. and N.H. developed the final version of the manuscript. H.P. and N.H. reconstructed the virus structure models, and performed the virus cloning. P.F.S. and R.F. made collaborations between MIT and Italy. P.R., P.F.S., L.A., M.M., R.F. and S.L. designed the theoretical work. P.R. and S.L. developed the fluorescence theory, and P.R. and H.P. applied it to the data. P.R. and S.L. developed the quantum transport theory, and P.R. and L.A. performed the quantum mechanical simulations. A.I., B.P., L.B. and P.F. performed the TA measurements and analysed the TA data. P.F., A.I. and H.P. interpreted the TA data. M.S. and R.F. helped H.P., N.H. and A.A. perform the QY measurements, and H.P. and A.A. analysed the QY data. F.C. collaborated in developing the computation model. H.C.J. helped H.P. with the virus preparations. H.P., N.H., P.R., P.F.S., S.L. and A.M.B. made major edits on the manuscript. All the authors gave helpful comments on the manuscript.

Corresponding authors

Correspondence to Petra F. Scudo, Seth Lloyd or Angela M. Belcher.

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The authors declare no competing financial interests.

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Park, H., Heldman, N., Rebentrost, P. et al. Enhanced energy transport in genetically engineered excitonic networks. Nature Mater 15, 211–216 (2016). https://doi.org/10.1038/nmat4448

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