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首页> 外文期刊>Chemistry: A European journal >Spectral Signatures of Ultrafast Spin Crossover in Single Crystal [Fe-II(bpy)(3)](PF6)(2)
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Spectral Signatures of Ultrafast Spin Crossover in Single Crystal [Fe-II(bpy)(3)](PF6)(2)

机译：单晶[Fe-II（bpy）（3）]（PF6）（2）中超快自旋交叉的光谱特征

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摘要

Solvated iron(II)-tris(bipyridine) ([Fe-II(bpy)(3)](2+)) has been extensively studied with regard to the spin crossover (SCO) phenomenon. Herein, the ultrafast spin transition dynamics of single crystal [Fe-II(bpy)(3)](PF6)(2) was characterized for the first time using femtosecond transient absorption (TA) spectroscopy. The single crystal environment is of interest for experiments that probe the nuclear motions involved in the SCO transition, such as femtosecond X-ray and electron diffraction. We found that the TA at early times is very similar to what has been reported in solvated [Fe-II(bpy)(3)](2+), whereas the later dynamics are perturbed in the crystal environment. The lifetime of the high-spin state is found to be much shorter (100ps) than in solution due to chemical pressure exerted by the lattice. Oscillatory behavior was observed on both time scales. Our results show that single crystal [Fe-II(bpy)(3)](PF6)(2) serves as an excellent model system for localized molecular spin transitions.
机译：溶剂化铁（II）-三（联吡啶）（[Fe-II（bpy）（3）]（2+））已就自旋交叉（SCO）现象进行了广泛研究。本文中，首次使用飞秒瞬态吸收（TA）光谱表征了单晶[Fe-II（bpy）（3）]（PF6）（2）的超快速自旋跃迁动力学。单晶环境对于探测参与SCO跃迁的核运动（例如飞秒X射线和电子衍射）的实验很有意义。我们发现，早期的TA与溶剂化的[Fe-II（bpy）（3）]（2+）中的报道非常相似，而后来的动力学在晶体环境中受到干扰。由于晶格施加的化学压力，发现高自旋状态的寿命比溶液中的寿命短得多（100ps）。在两个时间尺度上均观察到振荡行为。我们的结果表明，单晶[Fe-II（bpy）（3）]（PF6）（2）可作为用于局部分子自旋跃迁的出色模型系统。

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