揭示在铂供体-受体-供体系统中调制电子转移的量子相干效应。

IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Juanjuan Li, Yuqing Shi, Can Cui, Yefan Li, Chenluwei Ruan, Tao Cheng
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引用次数: 0

摘要

量子相干效应(QCEs)是由类波振幅的干涉引起的,在控制分子系统的电子传递函数中起着至关重要的作用。在这里,我们报道了一种与电荷分离(CS)相关的相干现象,在一系列Pt (II)顺式乙酰基酯供体-受体-供体(D-A-D)体系中,光生成的Pt (III)中心充当连接两个(R)吩噻嗪(R = H或tBu)供体的受体。飞秒瞬态吸收光谱显示,具有双CS路径的D-A- d系统的CS速率比具有单路径的供体-受体(D-A)系统加快了4-8倍。在CS路径之间的干扰情况下,推导出电子耦合的增强因子为2-3,提供了qce的清晰特征。CS过程中的这种魅力与捐赠者之间的耦合强度密切相关。本研究强调了量子电子束对分子系统光物理性质的重要影响,并为自然和人工系统中的电荷和能量传输机制提供了见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Unveiling Quantum Coherence Effects in Modulating Electron Transfer in Platinum (II) Donor-Acceptor-Donor Systems

Unveiling Quantum Coherence Effects in Modulating Electron Transfer in Platinum (II) Donor-Acceptor-Donor Systems

Unveiling Quantum Coherence Effects in Modulating Electron Transfer in Platinum (II) Donor-Acceptor-Donor Systems

Unveiling Quantum Coherence Effects in Modulating Electron Transfer in Platinum (II) Donor-Acceptor-Donor Systems

Quantum coherence effects (QCEs), arising from the interference of wave-like amplitudes, are crucial in controlling the electron transfer function of molecular systems. Here, we report a coherence phenomenon associated with charge separation (CS) in a range of Pt (II) cis-acetylide donor-acceptor-donor (D-A-D) systems, where the photogenerated Pt (III) center acts as an acceptor connecting two (R)phenothiazine (R = H or tBu) donors. Femtosecond transient absorption spectroscopy revealed that CS rates in D-A-D systems with double CS paths were accelerated by 4–8 times compared to their donor-acceptor (D-A) counterparts with a single path. An enhancement factor of 2–3 in electronic coupling, within the context of interference between CS paths, is derived, providing a clear signature of QCEs. This enhancementin CS processes closely correlates with the strength of coupling between donors. This study highlights the significant impact of QCEs on the photophysical properties of molecular systems and offers insights into charge and energy transport mechanisms in both natural and artificial systems.

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来源期刊
Chemistry - A European Journal
Chemistry - A European Journal 化学-化学综合
CiteScore
7.90
自引率
4.70%
发文量
1808
审稿时长
1.8 months
期刊介绍: Chemistry—A European Journal is a truly international journal with top quality contributions (2018 ISI Impact Factor: 5.16). It publishes a wide range of outstanding Reviews, Minireviews, Concepts, Full Papers, and Communications from all areas of chemistry and related fields. Based in Europe Chemistry—A European Journal provides an excellent platform for increasing the visibility of European chemistry as well as for featuring the best research from authors from around the world. All manuscripts are peer-reviewed, and electronic processing ensures accurate reproduction of text and data, plus short publication times. The Concepts section provides nonspecialist readers with a useful conceptual guide to unfamiliar areas and experts with new angles on familiar problems. Chemistry—A European Journal is published on behalf of ChemPubSoc Europe, a group of 16 national chemical societies from within Europe, and supported by the Asian Chemical Editorial Societies. The ChemPubSoc Europe family comprises: Angewandte Chemie, Chemistry—A European Journal, European Journal of Organic Chemistry, European Journal of Inorganic Chemistry, ChemPhysChem, ChemBioChem, ChemMedChem, ChemCatChem, ChemSusChem, ChemPlusChem, ChemElectroChem, and ChemistryOpen.
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