Skip to Main content Skip to Navigation
Journal articles

Unveiling the Role of Hot Charge-Transfer States in Molecular Aggregates via Nonadiabatic Dynamics

Abstract : Exciton dynamics governs energy transfer and charge generation in organic functional materials. We investigate high-energy nonadiabatic excited-state dynamics for a bithiophene dimer to describe time-dependent excitonic effects in molecular aggregates. We show that the lowest excited states are populated on the subpicosecond time scale. These states are localized and unproductive in terms of charge separation. Productive high-energy charge-transfer (CT) states are populated within 50 fs during exciton deactivation, but they are short-lived (∼100 fs) and quickly transfer their population to lower states. Our simulations offer molecular-level insights into ultrafast photoinduced charge separation potentially triggered by hot CT states in solid-state organic materials. Design rules are suggested to increase hot exciton lifetimes, favoring the population of CT states as gateways for direct charge generation. These rules may boost the CT quantum yield by depleting unproductive recombination channels.
Document type :
Journal articles
Complete list of metadatas

https://hal-amu.archives-ouvertes.fr/hal-02288606
Contributor : Mario Barbatti <>
Submitted on : Sunday, September 15, 2019 - 10:07:56 AM
Last modification on : Thursday, July 16, 2020 - 4:11:39 PM
Long-term archiving on: : Saturday, February 8, 2020 - 12:09:20 PM

File

p110_fazzi_excition_jacs_2016....
Files produced by the author(s)

Identifiers

Collections

Citation

Daniele Fazzi, Mario Barbatti, Walter Thiel. Unveiling the Role of Hot Charge-Transfer States in Molecular Aggregates via Nonadiabatic Dynamics. Journal of the American Chemical Society, American Chemical Society, 2016, 138 (13), pp.4502-4511. ⟨10.1021/jacs.5b13210⟩. ⟨hal-02288606⟩

Share

Metrics

Record views

75

Files downloads

144