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We report two-dimensional electronic spectroscopy (2DES) experiments on thebacterial reaction center (BRC) from purple bacteria, revealing hiddenexcitonic and vibronic structure. Through analysis of the coherent dynamics ofthe BRC we resolve specific coherent signatures that allow us to definitivelyassign the upper exciton energy of the "special pair." This assignment issupported by simulations of coherent dynamics of a reduced excitonic model ofthe BRC. The simulations also identify nonsecular vibronic coherence transferprocesses neglected in standard models of photosynthetic energy transfer andcharge separation. In addition, the coherent dynamics reveal multiplequasi-resonances between key intramolecular pigment vibrations and excitedstate energy gaps in the BRC. The functional significance of suchelectronic-vibrational resonances for photosynthetic energy transfer and chargeseparation remains an open question.

Hidden Vibronic and Excitonic Structure and Vibronic Coherence Transfer in the Bacterial Reaction Center