Top Curr Chem (Z) (2018) 376:10
1 3
These oscillations have been attributed to electronic, vibrational, and vibronic
origins in various systems. Gradually, the consensus has been reached that the long
lasting oscillations and their frequencies must be explained by mixing of electronic
and vibrational coherences [72–74]. In particular, vibrational modes with frequencies resonant with electronic energy gaps were suggested to be important for both
spectroscopic signals and energy-transfer dynamics [75].
The following example (Fig. 14) shows a recent experimental and theoretical
verification of coherent electronic–vibrational (vibronic) coupling as the origin of
long-lasting coherence, measured in a model system for artificial light harvesting,
a molecular J-aggregate [76]. In this tubular system (Fig. 14a, b), a polarizationcontrolled 2DES approach offered a great tool to distinguish the specific optical responses, leading to fewer region of the 2DES map, which show oscillatory
Fig. 13 Examples of 2DES studies where coherent oscillations have been observed in photosynthetic
complexes, specifically in: a the FMO complex. Reprinted from Copyright 2010 National Academy of
Sciences [68]; b LHCII complex. Reprinted with permission from Copyright 2009 American Chemical
Society [69]; c–d reaction center RC of PSII. Reprinted by permission from Macmillan Publishers Ltd:
Nature Chemistry [70], copyright 2014. Reprinted by permission from Macmillan Publishers Ltd: Nature
Physics [71], copyright 2014
46
Reprinted from the journal
1 3
These oscillations have been attributed to electronic, vibrational, and vibronic
origins in various systems. Gradually, the consensus has been reached that the long
lasting oscillations and their frequencies must be explained by mixing of electronic
and vibrational coherences [72–74]. In particular, vibrational modes with frequencies resonant with electronic energy gaps were suggested to be important for both
spectroscopic signals and energy-transfer dynamics [75].
The following example (Fig. 14) shows a recent experimental and theoretical
verification of coherent electronic–vibrational (vibronic) coupling as the origin of
long-lasting coherence, measured in a model system for artificial light harvesting,
a molecular J-aggregate [76]. In this tubular system (Fig. 14a, b), a polarizationcontrolled 2DES approach offered a great tool to distinguish the specific optical responses, leading to fewer region of the 2DES map, which show oscillatory
Fig. 13 Examples of 2DES studies where coherent oscillations have been observed in photosynthetic
complexes, specifically in: a the FMO complex. Reprinted from Copyright 2010 National Academy of
Sciences [68]; b LHCII complex. Reprinted with permission from Copyright 2009 American Chemical
Society [69]; c–d reaction center RC of PSII. Reprinted by permission from Macmillan Publishers Ltd:
Nature Chemistry [70], copyright 2014. Reprinted by permission from Macmillan Publishers Ltd: Nature
Physics [71], copyright 2014
46
Reprinted from the journal