Photosynthesis provides the energy source for essentially all living
things on Earth, and its functionality has been one of the most
fascinating mysteries of life. Photosynthetic conversion of the energy
of sunlight into its chemical form suitable for cellular processes
involves a variety of physicochemical mechanisms. The conversion starts
with the absorption of a photon of sunlight by one of the
light-harvesting pigments, followed by transfer of electronic excitation
energy to the reaction center, where charge separation is initiated. At
low light intensities, surprisingly, the quantum efficiency of the
transfer is near unity. A longstanding question in photosynthesis has
been the following: How does light harvesting deliver such high
efficiency in the presence of disordered and fluctuating dissipative
environments? Why does not energy get lost? The precise molecular
mechanisms of these initial steps of photosynthesis are not yet fully
elucidated from the standpoint of atomic, molecular, and optical science.
Recently, the technique of two-dimensional electronic spectroscopy has
been applied to explore photosynthetic light harvesting complexes. The
observations of long-lived electronic quantum coherence in the complexes
(1, 2, 3) stimulated a huge burst of activity among experimentalists and
theorists. Much of the interest arose because the finding of electronic
quantum coherence in a “warm, wet, and noisy” biological system was
considered very surprising. The observation has led to the suggestion
that quantum coherence might play a significant role in achieving the
remarkable efficiency of photosynthetic light harvesting. At the same
time, the observation has raised questions regarding the role of the
surrounding protein in protecting the quantum coherence. In order to
elucidate the origin of the long-lived electronic quantum coherence and
its interplay with the protein environment, we tackled the development
of an appropriate theoretical framework and concept (4, 5). As a result,
we succeeded in predicting several times longer-lived quantum coherence
between electronic excited states of pigments than the conventional
theories which are widely used in the literature of photosynthetic light
harvesting, does. Furthermore, our results explain the experimental data
at 77K and 300K (5, 6).
In this talk, we would like to discuss the present state of
understanding of electronic quantum coherence in photosynthetic light
harvesting with the aim of shedding light on the physical mechanisms
underlying the long-lived coherence and the potential functions such
coherence could facilitate (7).
References
(1) G. S. Engel, T. R. Calhoun, et al. Nature 446, 782 (2007).
(2) E. Collini, C. Y. Wong, et al. Nature 463, 644 (2010).
(3) G. Panitchayangkoon, D. Hayes, et al. Proc. Natl. Acad. Sci. USA 107, 12766 (2010).
(4) A. Ishizaki and G. R. Fleming, J. Chem. Phys. 130, 234111 (2009).
(5) A. Ishizaki and G. R. Fleming, Proc. Natl. Acad. Sci. USA 106, 17255-17260 (2009).
(6) G. S. Schlau-Cohen, A. Ishizaki, Nat. Chem. 4, 389 (2012).
(7) A. Ishizaki and G. R. Fleming, Annu. Rev. Condens. Matter Phys. 3, 333(2012). |