Electronic coupling and spin–orbit charge transfer intersystem crossing (SOCT-ISC) in compact BDP–carbazole dyads with different mutual orientations of the electron donor and acceptor

系统间交叉 化学 激发态 三重态 超快激光光谱学 接受者 光化学 光子上转换 光谱学 单重态 分子物理学 原子物理学 离子 物理 量子力学 有机化学 凝聚态物理
作者
Yuqi Hou,Ivan V. Kurganskii,Ayhan Elmalı,Huimin Zhang,Yuting Gao,Lingling Lv,Jianzhang Zhao,Ahmet Karatay,Liang Luo,Matvey V. Fedin
出处
期刊:Journal of Chemical Physics [American Institute of Physics]
卷期号:152 (11) 被引量:55
标识
DOI:10.1063/1.5145052
摘要

In order to study the spin-orbit charge transfer induced intersystem crossing (SOCT-ISC), Bodipy (BDP)-carbazole (Cz) compact electron donor/acceptor dyads were prepared. Charge transfer (CT) emission bands were observed for dyads showing strong electronic coupling between the donor and the acceptor (coupling matrix elements VDA, 0.06 eV-0.18 eV). Depending on the coupling magnitude, the CT state of the dyads can be either dark or emissive. Equilibrium between the 1LE (locally excited) state and the 1CT state was confirmed by temperature-dependent fluorescence studies. Efficient ISC was observed for the dyads with Cz connected at the meso-position of the BDP. Interestingly, the dyad with non-orthogonal geometry shows the highest ISC efficiency (ΦΔ = 58%), which is different from the previous conclusion. The photo-induced charge separation (CS, time constant: 0.7 ps) and charge recombination (CR, ∼3.9 ns) were studied by femtosecond transient absorption spectroscopy. Nanosecond transient absorption spectroscopy indicated that the BDP-localized triplet state was exceptionally long-lived (602 µs). Using pulsed laser excited time-resolved electron paramagnetic resonance spectroscopy, the SOCT-ISC mechanism was confirmed, and we show that the electron spin polarization of the triplet state is highly dependent on the mutual orientation of the donor and acceptor. The dyads were used as triplet photosensitizers for triplet-triplet-annihilation (TTA) upconversion, and the quantum yield is up to 6.7%. TTA-based delayed fluorescence was observed for the dyads (τDF = 41.5 µs). The dyads were also used as potent photodynamic therapy reagents (light toxicity of IC50 = 0.1 µM and dark toxicity of IC50 = 70.8 µM).
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