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Adapting the Förster Theory of Energy Transfer for Modeling Dynamics in Aggregated Molecular Assemblies
Abstract
The remarkable efficiencies of solar energy conversion attained by photosynthetic organisms derive partly from the designs of the light-harvesting apparatuses. The strategy employed by nature is to capture sunlight over a wide spectral and spatial cross section in chromophore arrays, then funnel the energy to a trap (reaction center). Nature's blueprint has inspired the conception of a diversity of artificial light-harvesting antenna systems for applications in solar energy conversion or photonics. Despite numerous, wide-ranging studies, truly quantitative predictions for such multichromophoric assemblies are scarce because Förster theory in its standard form often seems to fail. We report here a new framework within which energy transfer in molecular assemblies can be modeled quantitatively using a generalization of Förster's theory. Our results show that the principles involved in optimization of energy transfer in confined molecular assemblies are not revealed in a simple way by the absorption and emission spectra because such spectra are insensitive to length scales on the order of molecular dimensions.
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Citations
Cited by
Lessons from nature about solar light harvesting
Scholes, G. D., Fleming, G. R., Olaya-Castro, A., & van Grondelle, R. (2011) · Nature Chemistry · doi:10.1038/nchem.1145 · Cited by 1,915
Self-citationScholes, G. D., & Rumbles, G. (2006) · Nature Materials · doi:10.1038/nmat1710 · Cited by 1,286
Self-citationBeyond Förster Resonance Energy Transfer in Biological and Nanoscale Systems
Beljonne, D., Curutchet, C., Scholes, G. D., & Silbey, R. J. (2009) · The Journal of Physical Chemistry B · doi:10.1021/jp900708f · Cited by 451
Self-citationInterchain vs. intrachain energy transfer in acceptor-capped conjugated polymers
Beljonne, D., Pourtois, G., Silva, C., Hennebicq, E., Herz, L. M., Friend, R. H., Scholes, G. D., Setayesh, S., Müllen, K., & Brédas, J. L. (2002) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.172390999 · Cited by 377
Self-citationElectronic Energy Transfer in Condensed Phase Studied by a Polarizable QM/MM Model
Curutchet, C., Muñoz-Losa, A., Monti, S., Kongsted, J., Scholes, G. D., & Mennucci, B. (2009) · Journal of Chemical Theory and Computation · doi:10.1021/ct9001366 · Cited by 298
Self-citationQuantum Coherence in Photosynthetic Light Harvesting
Ishizaki, A., & Fleming, G. R. (2012) · Annual Review of Condensed Matter Physics · doi:10.1146/annurev-conmatphys-020911-125126 · Cited by 285
Self-citationBioinspiration in light harvesting and catalysis
Proppe, A. H., Li, Y. C., Aspuru-Guzik, A., Berlinguette, C. P., Chang, C. J., Cogdell, R., Doyle, A. G., Flick, J., Gabor, N. M., van Grondelle, R., et al. (2020) · Nature Reviews Materials · doi:10.1038/s41578-020-0222-0 · Cited by 257
Self-citationPathways of Energy Flow in LHCII from Two-Dimensional Electronic Spectroscopy
Schlau-Cohen, G. S., Calhoun, T. R., Ginsberg, N. S., Read, E. L., Ballottari, M., Bassi, R., van Grondelle, R., & Fleming, G. R. (2009) · The Journal of Physical Chemistry B · doi:10.1021/jp9066586 · Cited by 203
Self-citationKolli, A., Nazir, A., & Olaya-Castro, A. (2011) · The Journal of Chemical Physics · doi:10.1063/1.3652227 · Cited by 124
The feasibility of coherent energy transfer in microtubules.
Craddock, T. J. A., Friesen, D., Mane, J., Hameroff, S., & Tuszynski, J. A. (2014) · Journal of The Royal Society Interface · doi:10.1098/rsif.2014.0677 · Cited by 111
Energy-scales convergence for optimal and robust quantum transport in photosynthetic complexes
Mohseni, M., Shabani, A., Lloyd, S., & Rabitz, H. (2014) · The Journal of Chemical Physics · doi:10.1063/1.4856795 · Cited by 55
Quantum effects in photosynthesis
van Grondelle, R., & Novoderezhkin, V. I. (2011) · Procedia Chemistry · doi:10.1016/j.proche.2011.08.027 · Cited by 22
Metadata
- Authors
- Scholes, G. D., Jordanides, X. J., & Fleming, G. R.
- Venue
- The Journal of Physical Chemistry B
- Publisher
- American Chemical Society (ACS)
- Published
- 2001-02-02
- Volume
- 105
- Issue
- 8
- Pages
- 1640-1651
- ISSN
- 1520-5207 (ISSN-L)
- 1520-6106
- OpenAlex
- W1981517702
- Cited by
- 238
- References
- 0
- FWCI
- 7.31
- Type
- journal article
- Language
- en
- Open access
- closed
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