Instantaneous mapping of coherently coupled electronic transitions and energy transfers in a photosynthetic complex using angle-resolved coherent optical wave-mixing.
Understanding the role of coherent electronic motion is expected to resolve general questions of importance in macromolecular energy transfer. We demonstrate a novel nonlinear optical method, angle-resolved coherent wave mixing, that separates out coherently coupled electronic transitions and energy transfers in an instantaneous two-dimensional mapping. Angular resolution of the signal is achieved by using millimeter laser beam waists at the sample and by signal relay to the far field; for this we use a high energy, ultrabroadband hollow fiber laser source. We reveal quantum electronic beating with a time-ordered selection of transition energies in a photosynthetic complex.
Mercer
Ian P
IP
School of Physics, Centre for Synthesis and Chemical Biology, University College Dublin, Dublin 4, Ireland.
El-Taha
Yasin C
YC
Kajumba
Nathaniel
N
Marangos
Jonathan P
JP
Tisch
John W G
JW
Gabrielsen
Mads
M
Cogdell
Richard J
RJ
Springate
Emma
E
Turcu
Edmund
E
D001426:Bacterial Proteins / Q000737:chemistry*; D045342:Light-Harvesting Protein Complexes / Q000737:chemistry*; D017711:Nonlinear Dynamics; D055095:Optics and Photonics / Q000295:instrumentation / Q000379:methods*; D010788:Photosynthesis; D011789:Quantum Theory
C081521:B800-850 light-harvesting complex, bacteria; D001426:Bacterial Proteins; D045342:Light-Harvesting Protein Complexes