Alkali-helium exciplex formation on the surface of helium nanodroplets. II. A time-resolved study

Alkali-helium exciplex formation on the surface of helium nanodroplets. II. A time-resolved study
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氦纳米滴表面上碱-氦激基复合物的形成。

DOI:
10.1063/1.1321034
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发表时间:
2000
影响因子:
4.4
通讯作者:
G. Scoles
G. Scoles
中科院分区:
化学2区
文献类型:
--
作者:
J. Reho;J. Higgins;K. Lehmann;G. Scoles

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利用反向时间相关单光子计数技术,对氦纳米液滴表面形成的K*He复合物荧光的时间演化进行了监测。通过对现有数据和我们之前关于Na*He的工作进行建模,我们发现部分自旋-轨道耦合以及氦原子从液滴中提取能量有助于观察到K*He和Na*He形成的动力学,在K(n=4)和Na(n=3)的D1(n 2P1/2←n 2S1/2)或D2(n 2P3/2←n 2S1/2)激发后,两者的动力学差异很大。我们对Na*He地层动力学的定量预测,加上K*He地层动力学的初步数据和建模,允许外推到Rb*He的情况。自旋轨道考虑结合氦原子从矩阵中提取的简单模型揭示了以下预测趋势:随着碱客体原子的选择在元素周期表中下移,碱原子- he -激络合物沿1 2Π3/2表面的形成速度更快,而…
We have monitored the time evolution of the fluorescence of K*He exciplexes formed on the surface of helium nanodroplets using reversed time-correlated single photon counting. In modeling the present data and that from our previous work on Na*He, we find that partial spin–orbit coupling as well as the extraction energy of helium atoms from the droplet contribute to the observed dynamics of both K*He and Na*He formation, which differ considerably after either D1(n 2P1/2←n 2S1/2) or D2(n 2P3/2←n 2S1/2) excitation for both K(n=4) and Na(n=3). Our quantitative prediction of the Na*He formation dynamics coupled with preliminary data on and modeling of the formation dynamics of K*He allow for extrapolation to the case of Rb*He. Spin–orbit considerations combined with a simple model of helium atom extraction from the matrix reveal the following predicted trend: as the choice of the alkali guest atom is moved down the periodic table, alkali atom–He exciplex formation along the 1 2Π3/2 surface occurs faster while ...