Mechanistic Regimes of Vibronic Transport in a Heterodimer and the Design Principle of Incoherent Vibronic Transport in Phycobiliproteins
- Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology; Canadian Inst. for Advanced Research, Toronto, ON (Canada). Bio-Inspired Solar Energy Program
- Vrije Univ., Amsterdam (Netherlands). Dept. of Physics and Astronomy; Charles Univ., Prague (Czech Republic). Faculty of Mathematics and Physics; Canadian Inst. for Advanced Research, Toronto, ON (Canada). Bio-Inspired Solar Energy Program
- Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology
- Vrije Univ., Amsterdam (Netherlands). Dept. of Physics and Astronomy; Canadian Inst. for Advanced Research, Toronto, ON (Canada). Bio-Inspired Solar Energy Program
Following the observation of coherent oscillations in nonlinear spectra of photosynthetic pigment protein complexes, in particular, phycobilliproteins such as PC645, coherent vibronic transport has been suggested as a design principle for novel light-harvesting materials. Vibronic transport between energetically remote pigments is coherent when the presence of a vibration resonant with the electronic energy gap supports transient delocalization between the electronic excited states. We establish the mechanism of vibronic transport for a model heterodimer across a wide range of molecular parameter values. The resulting mechanistic map demonstrates that the molecular parameters of phycobiliproteins in fact support incoherent vibronic transport. This result points to an important design principle: Incoherent vibronic transport is more efficient than a coherent mechanism when energetic disorder exceeds the coupling between the donor and vibrationally excited acceptor states. Finally, our results suggest that the role of coherent vibronic transport in pigment protein complexes should be reevaluated.
- Research Organization:
- Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- SC0001088
- OSTI ID:
- 1470509
- Journal Information:
- Journal of Physical Chemistry Letters, Vol. 9, Issue 10; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; ISSN 1948-7185
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
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71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
solar (photovoltaic)
solid state lighting
photosynthesis (natural and artificial)
charge transport
optics
synthesis (novel materials)
synthesis (self-assembly)
synthesis (scalable processing)