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Enhanced energy transport in genetically engineered excitonic networks

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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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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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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