Quantum control of energy flow in light harvesting.
Coherent light sources have been widely used in control schemes that exploit quantum interference effects to direct the outcome of photochemical processes. The adaptive shaping of laser pulses is a particularly powerful tool in this context: experimental output as feedback in an iterative learning loop refines the applied laser field to render it best suited to constraints set by the experimenter. This approach has been experimentally implemented to control a variety of processes, but the extent to which coherent excitation can also be used to direct the dynamics of complex molecular systems in a condensed-phase environment remains unclear. Here we report feedback-optimized coherent control over the energy-flow pathways in the light-harvesting antenna complex LH2 from Rhodopseudomonas acidophila, a photosynthetic purple bacterium. We show that phases imprinted by the light field mediate the branching ratio of energy transfer between intra- and intermolecular channels in the complex's donor acceptor system. This result illustrates that molecular complexity need not prevent coherent control, which can thus be extended to probe and affect biological functions.
Herek
Jennifer L
JL
Chemical Physics, Lund University, 22100 Lund, Sweden.
Wohlleben
Wendel
W
Cogdell
Richard J
RJ
Zeidler
Dirk
D
Motzkus
Marcus
M
D004735:Energy Transfer; D007700:Kinetics; D008027:Light; D008958:Models, Molecular; D045322:Photosynthetic Reaction Center Complex Proteins / Q000737:chemistry / Q000378:metabolism*; D020836:Protein Structure, Quaternary; D012241:Rhodopseudomonas / Q000737:chemistry / Q000378:metabolism*
D045322:Photosynthetic Reaction Center Complex Proteins