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Charge-Delocalized State and Coherent Vibrational Dynamics in Rigid PBI H‑Aggregates

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journal contribution
posted on 24.06.2021, 20:30 by Seongsoo Kang, Taeyeon Kim, Yongseok Hong, Frank Würthner, Dongho Kim
Herein, the ultrafast photoinduced dynamics and vibrational coherences for two perylenebisimide (PBI) H-aggregates showcase the formation of the excimer state and the delocalized radical anion state in the excited state, respectively. Using femtosecond transient absorption (fs-TA) and time-resolved impulsive stimulated Raman scattering (TR-ISRS) measurements, we unveiled excited-state dynamics of PBI H-aggregates in two aspects: (1) the intermolecular interactions between PBI units in H-aggregates induce the formation of new excited states, excimer and delocalized radical anion states, and (2) the intermolecular out-of-plane along the aggregate axis and the PBI core CC stretch Raman modes can be a crucial indicator to understand the coherent exciton dynamics in H-aggregates. Notably, those excited-state Raman modes showed stationary peak positions during the excited-state dynamics. TR-ISRS analysis provides insights into the excited-state vibrational coherences concerning the formation of the excimer and charge-delocalized state in each aggregate system.