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Inside Cover: Photoinduced Processes of Supramolecular Nanoarrays Composed of Porphyrin and Benzo[ghi]perylenetriimide Units through Triple Hydrogen Bonds with One‐Dimensional Columnar Phases (Chem. Asian J. 4/2016)
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Dr. Hayato Sakai Prof. Kei Ohkubo Prof. Shunichi Fukuzumi Prof. Taku Hasobe 《化学:亚洲杂志》2016,11(4):420-420
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Sabrina V. Kirner Danny Arteaga Christian Henkel Johannes T. Margraf Nuria Alegret Kei Ohkubo Braulio Insuasty Alejandro Ortiz Nazario Martín Luis Echegoyen Shunichi Fukuzumi Timothy Clark Dirk M. Guldi 《Chemical science》2015,6(10):5994-6007
The design, synthesis, and electronic properties of a new series of D–π–A conjugates consisting of free base (H2P) and zinc porphyrins (ZnP) as electron donors and a fullerene (C60) as electron acceptor, in which the two electroactive entities are covalently linked through pyridine-vinylene spacers of different lengths, are described. Electronic interactions in the ground state were characterized by electrochemical and absorption measurements, which were further supported with theoretical calculations. Most importantly, charge-transfer bands were observed in the absorption spectra, indicating a strong push–pull behavior. In the excited states, electronic interactions were detected by selective photoexcitation under steady-state conditions, by time-resolved fluorescence investigations, and by pump probe experiments on the femto-, pico-, and nanosecond time scales. Porphyrin fluorescence is quenched for the different D–π–A conjugates, from which we conclude that the deactivation mechanisms of the excited singlet states are based on photoinduced energy- and/or electron transfer processes between H2P/ZnP and C60, mediated through the molecular spacers. The fluorescence intensity decreases and the fluorescence lifetimes shorten as the spacer length decreases and as the spacer substitution changes. With the help of transient absorption spectroscopy, the formation of charge-separated states involving oxidized H2P/ZnP and reduced C60 was confirmed. Lifetimes of the corresponding charge-separated states, which ranged from ∼400 picoseconds to 165 nanoseconds, depend on the spacer length, the spacer substitution, and the solvent polarity. Interestingly, D–π–A conjugates containing the longest linkers did not necessarily exhibit the longest charge-separated state lifetimes. The distances between the electron donors and the acceptors were calculated by molecular modelling. The longest charge-separated state lifetime corresponded to the D–π–A conjugate with the longest electron donor–acceptor distance. Likewise, EPR measurements in frozen media revealed charge separated states in all the D–π–A conjugates investigated. A sharp peak with g values ∼2.000 was assigned to reduced C60, while a broader, less intense signal (g ∼ 2.003) was assigned to oxidized H2P/ZnP. On–off switching of the formation and decay of the charge-separated states was detected by EPR at 77 K by repeatedly turning the irradiation source on and off. 相似文献
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Dr. Hirofumi Nobukuni Prof. Dr. Yuichi Shimazaki Prof. Dr. Hidemitsu Uno Prof. Dr. Yoshinori Naruta Prof. Dr. Kei Ohkubo Prof. Dr. Takahiko Kojima Prof. Dr. Shunichi Fukuzumi Prof. Dr. Shu Seki Dr. Hayato Sakai Prof. Dr. Taku Hasobe Prof. Dr. Fumito Tani 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(38):11611-11623
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