Ultrafast Dynamical Study of Pyrene-N,N-dimethylaniline (PyDMA) as an Organic Molecular Diode in Solid State

Femtosecond optical pump–probe spectroscopy has been employed for studying the directly linked electron donor–acceptor system pyrene-N,N-dimethylaniline (PyDMA) in solid state. This DMA-pyrene derivative discussed is being applied as a molecular diode system switching on an ultrafast time scale. Our...

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Bibliographic Details
Published in:The journal of physical chemistry. B 2014-03, Vol.118 (12), p.3291-3297
Main Authors: Thekku Veedu, Sreevidya, Raiser, Dirk, Kia, Reza, Scholz, Mirko, Techert, Simone
Format: Article
Language:English
Subjects:
Aniline Compounds - chemistry
Diodes
Dynamical systems
Electron Transport
Femtosecond
Ion pairs
Models, Molecular
Molecular orbitals
Optical Devices
Optical transition
Photochemistry
Pyrenes - chemistry
Radicals
Solid state
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Summary:Femtosecond optical pump–probe spectroscopy has been employed for studying the directly linked electron donor–acceptor system pyrene-N,N-dimethylaniline (PyDMA) in solid state. This DMA-pyrene derivative discussed is being applied as a molecular diode system switching on an ultrafast time scale. Our ultrafast solid-state studies reveal a complex photochemistry of this molecular crystal system. Strong couplings of the optically induced charge-transfer state with the radical ion pair state allow a femtosecond transition of the latter. One could see on the highest occupied molecular orbital–lowest unoccupied molecular orbital (HOMO–LUMO) description that a pure optical transition switches the system from a conducting to a blocked system because the molecular orbitals (MOs) of DMA moiety lie in a node plane of the LUMO. Within 800 fs the system relaxes back to the ground state and/or forms a radical ion pair, which is the surprising result of our study; when the system was probed further, the system underwent vibrational cooling and enhanced population inversion of the radical ion pair.
ISSN:1520-6106
1520-5207
DOI:10.1021/jp4121222