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Quantum coherence is highly involved in photochemical functioning of complex molecular systems. Co-existence and intermixing of electronic and/or vibrational coherences, while never unambiguously identified experimentally, has been proposed to be responsible for this phenomenon. Analysis of multidimensional spectra of a synthetic belt-shaped molecular six-porphyrin nanoring with an inner template clearly shows a great diversity of separable electronic, vibrational and mixed coherences and their cooperation shaping the optical response. The results yield clear assignment of electronic and vibronic states, estimation of excitation transfer rates, and decoherence times. Theoretical considerations prove that the complexity of excitation dynamics and spectral features of the nanoring excitation spectrum is due to combined effect of cyclic symmetry, small geometrical deformations, and vibronic coupling.
Coherent dynamics of coupled molecules are effectively characterized by the two-dimensional (2D) electronic coherent spectroscopy. Depending on the coupling between electronic and vibrational states, oscillating signals of purely electronic, purely v
The effect of nuclear dynamics and conical intersections on electronic coherences is investigated employing a two-state, two-mode linear vibronic coupling model. Exact quantum dynamical calculations are performed using the multi-configuration time-de
The two-dimensional spectroscopy has recently revealed oscillatory behavior of excitation dynamics in molecular systems. However, in the majority of cases it is strongly debated if excitonic or vibrational wavepackets, or evidences of quantum transpo
Electronic spectra of C$_6$H are measured in the $18,950-21,100$ cm$^{-1}$ domain using cavity ring-down spectroscopy of a supersonically expanding hydrocarbon plasma. In total, 19 (sub)bands of C$_6$H are presented, all probing the vibrational manif
We demonstrate that the coupling of excitonic and vibrational motion in biological complexes can provide mechanisms to explain the long-lived oscillations that have been obtained in non linear spectroscopic signals of different photosynthetic pigment