Abstract
Long-lived oscillations in 2D spectra of chlorophylls are at the heart of an ongoing debate. Their physical origin is either a multipigment effect, such as excitonic coherence, or localized vibrations. We show how relative phase differences of diagonal- and cross-peak oscillations can distinguish between electronic and vibrational (vibronic) effects. While direct discrimination between the two scenarios is obscured when peaks overlap, their sensitivity to temperature provides a stronger argument. We show that vibrational (vibronic) oscillations change relative phase with temperature, while electronic oscillations are only weakly dependent. This highlights that studies of relative phase difference as a function of temperature provide a clear and easily accessible method to distinguish between vibrational and electronic coherences.
Highlights
We show that vibrational oscillations change relative phase with temperature, while electronic oscillations are only weakly dependent
I n the early stage of photosynthesis, excitation is created by absorption of a photon, followed by exciton migration from the peripheral antenna complexes to the reaction center with remarkably high efficiency.[1]
The original argument triggered a critical discussion[5−14] as it quickly became understood that the outof-phase oscillatory pattern of diagonal and cross peaks cannot serve as a strong criterion for the identification of electronic coherence
Summary
I n the early stage of photosynthesis, excitation is created by absorption of a photon, followed by exciton migration from the peripheral antenna complexes to the reaction center with remarkably high efficiency.[1]. We show how relative phase differences of diagonal- and cross-peak oscillations can distinguish between electronic and vibrational (vibronic) effects. We show that vibrational (vibronic) oscillations change relative phase with temperature, while electronic oscillations are only weakly dependent.
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