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首页> 外文期刊>Physical chemistry chemical physics: PCCP >Mapping CTTS dynamics of Na- in tetrahydrofurane with ultrafast multichannel pump-probe spectroscopy
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Mapping CTTS dynamics of Na- in tetrahydrofurane with ultrafast multichannel pump-probe spectroscopy

机译：超快速多通道泵浦-探针光谱法绘制四氢呋喃中Na-的CTTS动力学图

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摘要

Using multichannel femtosecond spectroscopy we have followed Na- charge transfer to solvent (CTTS) dynamics in THF solution. Absorption of the primary photoproducts in the visible, resolved here for the first time, consists of an asymmetric triplet centered at 595 nm, which we assign to a metastable incompletely solvated neutral atomic sodium species. Decay of this feature within similar to 1 ps to a broad and structureless solvated neutral is accompanied by broadening and loss of spectral detail. Kinetic analysis shows that both the spectral structure and the decay of this band are independent of the excitation photon frequency in the range 400-800 nm. With different pump-probe polarizations the anisotropy in transient transmission has been charted and its variation with excitation wavelength surveyed. The anisotropies are assigned to the reactant bleach, indicating that due to solvent-induced symmetry breaking, the CTTS absorption band of Na- is made up of discreet orthogonally polarized sub bands. None of the anisotropy in transient absorption could be associated with the photoproduct triplet band even at the earliest measurable time delays. Along with the documented differences in the spatial distribution of ejected electrons across the tested excitation wavelength range, these results lead us to conclude that photoejection is extremely rapid, and that loss of correlations between the departing electron and its neutral core is faster than our time resolution of similar to 60 fs.
机译：使用多通道飞秒光谱仪，我们追踪了THF溶液中Na电荷转移至溶剂（CTTS）的动力学。在这里首次解析的可见光中主要光产物的吸收是由以595 nm为中心的不对称三重态组成，我们将其分配给亚稳的不完全溶剂化的中性原子钠物质。此特征在大约1 ps内衰减为宽广且无结构的溶剂化中性峰，同时伴随着光谱细节的扩大和损失。动力学分析表明，该谱带的光谱结构和衰减均与400-800 nm范围内的激发光子频率无关。用不同的泵浦极化极化，可以绘制瞬态传输的各向异性，并测量其随激发波长的变化。各向异性被分配给反应物漂白剂，表明由于溶剂诱导的对称性破坏，Na-的CTTS吸收带由离散的正交极化子带组成。即使在最早可测量的时间延迟下，瞬态吸收中的各向异性也不会与光产物三重态带相关。连同已记录的在测试的激发波长范围内射出的电子的空间分布的差异，这些结果使我们得出结论：光射出非常快，并且离去的电子与其中性核之间的相关性损失快于我们的时间分辨率。类似于60 fs。

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