ABSTRACT

Essentially all living things on earth use the sun as their energy

source which is harvested by photosynthesis. Photosynthetic con-

version of physical energy of sunlight into a chemical form useful

for cellular processes involves many steps [1, 2]. Photosynthesis

starts with the absorption of a photon by a light-harvesting pigment

or chromophore forming an exciton, followed by the transfer of

the exciton to the reaction center, where charge separation is

initiated leading subsequently to chemical storage of the energy.

In this chapter, our focus lies on the transfer dynamics which

surprisingly exhibits a quantum efficiency near unity under low

light conditions. Not only plants but also several bacteria make use

of photosynthesis. In green sulfur bacteria such as Chlorobaculum

tepidum light harvesting is done by an antennae complex, the chlorosome, which is a large conglomerate. The connection to the

reaction center is exclusively through the small Fenna-Matthews-

Olson (FMO) complex, a trimerwhosemonomers each contain seven

chromophores [3-6]. Recently, an eighth pigment was resolved

[7] which is, however, very weakly coupled to the other seven

pigments and thus is of little relevance for our studies. The purpose

of the FMO complex is purely to conduct the excitonic energy

from the antennae to the reaction center. Typical transfer times

through the FMO are on the order of picoseconds, whereas the

decay of an excited chromophore (with subsequent reemission of

a photon) takes on the order of nanoseconds. In addition, typically,

the absorption cross section for photons is small, meaning that

in general only a single exciton is present in an FMO complex.

This allows to restrict later the theoretical consideration to the

single excitation subspace. Furthermore, these timescales reflect the

extraordinary quantum efficiency of the excitonic energy transfer

in photosynthesis. However, it is still unclear why transport is so

much faster than direct decay of excitons. An understanding of this

question, which must lie in the design principle of photosynthetic

complexes, would allow to exploit the near-unity efficiency of energy

transfer within artificial light-harvesting complexes. Organic solar

cells suffer from very high exciton losses during transport and thus

could greatly benefit from biomimetic design principles.