Quantum Coherence and Energy Landscapes in Photosynthetic Systems Investigated with Two-Dimensional Electronic Spectroscopy
Abstract
Two-dimensional (2D) electronic spectroscopy has recently emerged as a powerful technique for the study of complex photodynamics in a variety of condensed phase systems. The application of this technique to both photosynthetic pigment-protein complexes and chromophore solutions has provided insight into their intricate excitation energy transfer mechanisms and landscapes. Analysis of beating peak amplitudes in 2D spectra of the Fenna-Matthews-Olson bacteriochlorophyll complex combined with changing lineshapes has revealed signals consistent with excitonic coherence. In addition, the long lifetime of the coherence indicates a reversible, wavelike motion of energy through the complex as opposed to the classical hopping picture. This quantum-mechanical behavior may explain the near unity quantum efficiency of excitation energy transfer observed in networks of photosynthetic complexes. The inclusion of a noncollinear optical parametric amplifier producing broad bandwidth pulses enables the exploration of excitonic coherence in Light Harvesting Complex II, the most abundant antenna complex in higher plants. Long-lived quantum coherence is again observed suggesting this to be a universal phenomenon in natural photosynthetic systems. To expand upon these findings, a coherence power spectrum is produced. This novel technique allows the first direct experimental determination of the excitonic energy levels. In another set of experiments, the building an adaptive, pulse-shaping…
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