Journal
NATURE NANOTECHNOLOGY
Volume 16, Issue 1, Pages 63-68Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41565-020-00791-2
Keywords
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Funding
- Deutsche Forschungsgemeinschaft [SPP1839, SPP1840, GRK1885, SFB1372, SINOXI FR2833/60-1, RTG-2247]
- Korea Foundation for International Cooperation of Science and Technology (Global Research Laboratory project) [K20815000003]
- German-Israeli Foundation [1256]
- Los Alamos National Laboratory (LANL) Directed Research and Development funds
- ANPCyT [PICT-2018-02360]
- CONICET [PICT-2018-02360)]
- UNQ [PICT-2018-02360)]
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The study reveals the presence of intermolecular conical intersections in molecular aggregates relevant for photovoltaics using ultrafast two-dimensional electronic spectroscopy. The coherent motion of a vibrational wave packet between different states can be observed in a very short timescale.
Conical intersections (CoIns) of multidimensional potential energy surfaces are ubiquitous in nature and control pathways and yields of many photo-initiated intramolecular processes. Such topologies can be potentially involved in the energy transport in aggregated molecules or polymers but are yet to be uncovered. Here, using ultrafast two-dimensional electronic spectroscopy (2DES), we reveal the existence of intermolecular CoIns in molecular aggregates relevant for photovoltaics. Ultrafast, sub-10-fs 2DES tracks the coherent motion of a vibrational wave packet on an optically bright state and its abrupt transition into a dark state via a CoIn after only 40 fs. Non-adiabatic dynamics simulations identify an intermolecular CoIn as the source of these unusual dynamics. Our results indicate that intermolecular CoIns may effectively steer energy pathways in functional nanostructures for optoelectronics. Two-dimensional electronic spectroscopy reveals the existence of intermolecular conical intersections in molecular aggregates relevant for photovoltaics.
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