Charge-Delocalized State and Coherent Vibrational Dynamics in Rigid PBI H-Aggregates,Journal of the American Chemical Society

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Charge-Delocalized State and Coherent Vibrational Dynamics in Rigid PBI H-Aggregates
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-06-24 , DOI: 10.1021/jacs.1c03276
Seongsoo Kang ₁ , Taeyeon Kim ₁ , Yongseok Hong ₁ , Frank Würthner ₂ , Dongho Kim ₁

Affiliation

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.

中文翻译：

刚性 PBI H 聚集体中的电荷离域状态和相干振动动力学

在此，两个苝双酰亚胺（PBI）H-聚集体的超快光致动力学和振动相干性分别展示了激发态下准分子态和离域自由基阴离子态的形成。使用飞秒瞬态吸收 (fs-TA) 和时间分辨脉冲受激拉曼散射 (TR-ISRS) 测量，我们从两个方面揭示了 PBI H 聚集体的激发态动力学：（1）H 中 PBI 单元之间的分子间相互作用-聚集体诱导新激发态、准分子和离域自由基阴离子态的形成，并且 (2) 沿聚集体轴和 PBI 核心 C=C 拉伸拉曼模式的分子间平面外可以是理解H-聚集体中的相干激子动力学。尤其，这些激发态拉曼模式在激发态动力学过程中显示出稳定的峰值位置。TR-ISRS 分析提供了对激发态振动相干性的洞察，这些振动相干性与每个聚合系统中准分子和电荷离域态的形成有关。

更新日期：2021-07-07

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