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Intermolecular conical intersections in molecular aggregates.

Antonietta De Sio1, Ephraim Sommer2, Xuan Trung Nguyen2

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Researchers discovered intermolecular conical intersections (CoIns) in molecular aggregates using ultrafast spectroscopy. These CoIns control energy transfer pathways in photovoltaic materials.

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Area of Science:

  • Photochemistry
  • Molecular Dynamics
  • Materials Science

Background:

  • Conical intersections (CoIns) on potential energy surfaces govern photochemical reaction pathways.
  • Intermolecular CoIns in molecular aggregates are crucial for energy transport but remain largely unexplored.
  • Understanding these dynamics is key for designing efficient optoelectronic materials.

Purpose of the Study:

  • To reveal the existence of intermolecular CoIns in molecular aggregates relevant for photovoltaics.
  • To investigate the role of these CoIns in ultrafast energy transfer processes.
  • To provide insights into the design of functional nanostructures for optoelectronics.

Main Methods:

  • Ultrafast two-dimensional electronic spectroscopy (2DES) with sub-10-fs resolution.
  • Tracking coherent vibrational wave packet motion.
  • Non-adiabatic dynamics simulations.

Main Results:

  • Direct observation of intermolecular CoIns in molecular aggregates.
  • Evidence of ultrafast (40 fs) transition from bright to dark states via CoIns.
  • Identification of intermolecular CoIns as the source of observed non-adiabatic dynamics.

Conclusions:

  • Intermolecular CoIns play a significant role in energy transfer within molecular aggregates.
  • These CoIns can effectively steer energy pathways in nanostructures for optoelectronics.
  • The findings open new avenues for designing advanced photovoltaic and optoelectronic devices.