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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Probing Charge-Transfer Excited States in a Qyasi-Nonluminescent Electron-Rich Fe(II)-Acetyiide Complex by Femtosecond Optical Spectroscopy
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Probing Charge-Transfer Excited States in a Qyasi-Nonluminescent Electron-Rich Fe(II)-Acetyiide Complex by Femtosecond Optical Spectroscopy

机译:飞秒光学光谱法测定Qaasi-不发光电子富集Fe(II)-乙酰胺络合物中的电荷转移激发态

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摘要

Molecules with photoswitchable nonlinear optical (NLO) properties on the nanosecond time scale are attracting considerable attention as potential solid-state components of photonic devices, downsizeable at will, for ultrafast information encoding. In this context, we present here the study of an electron-rich Fe(II) 4-nitrophenylaikynyl complex which possesses a high hyperpolarizability in its singlet ground state and a negative (and presumably much decreased) NLO activity in its first excited MLCT state(s). On the basis of an ensemble of spectroscopic and time-resolved measurements we investigate the ultrafast dynamics for deactivation of the initially populated MLCT singlet state(s) of this particular organometallic complex, which are shown todecay into a metastable triplet state. The purported mechanism is rationalized with DFT calculations. We show that this triplet state, which should also exhibit a strongly diminished hyperpolarizability, is fully formed with a very high quantum yield within 15 ps.
机译:纳秒级尺度上具有光开关非线性光学(NLO)特性的分子正引起人们的广泛关注,因为光子器件的潜在固态组件可以随意减小尺寸,以进行超快信息编码。在此背景下,我们在此介绍了富电子的Fe(II)4-硝基苯基烷基炔基络合物的研究,该络合物在其单线基态下具有高超极化性,并且在其第一个激发的MLCT状态下具有负(且可能大大降低)的NLO活性( s)。在光谱学和时间分辨测量的基础上,我们研究了该特定有机金属配合物的最初填充的MLCT单重态失活的超快动力学,这表明其分解为亚稳态三重态。通过DFT计算可以合理化所声称的机制。我们表明,这种三重态也应该表现出极强的超极化性,它在15 ps内以非常高的量子产率完全形成。

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