Time-resolved relaxation dynamics of Hgn- (11 <or = n <or = 16,n = 18) clusters following intraband excitation at 1.5 eV.
Time-resolved relaxation dynamics of Hgn- (11 <or = n <or = 16,n = 18) clusters following intraband excitation at 1.5 eV.
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Hgn- (11 <or = n <or = 16,n = 18) 簇在 1.5 eV 的带内激励后的时间分辨弛豫动力学。
DOI：
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发表时间：
2004
影响因子：
4.4
通讯作者：
D. Neumark
中科院分区：
文献类型：
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作者：
J. Verlet;A. Bragg;A. Kammrath;O. Cheshnovsky;D. Neumark
利用时间分辨光电子成像技术研究了Hg(n)⁻（11≤n≤16，n = 18）中的电子 - 核弛豫动力学。阴离子中的过剩电子独特地占据p能带，并被1.53 eV的泵浦光子在带内激发；随后的动力学通过3.06 eV的光剥离以及作为泵浦 - 探测延迟函数的光电子图像测量来监测。最初的激发态在大约10 ps的时间尺度上衰减，随后的弛豫动力学显示光电子能谱在50 - 100 ps内朝着更低的电子动能平滑演化。定性地说，弛豫过程可由一个简单的动力学模型描述，该模型假设在密集的电子态流形内存在一系列无辐射跃迁。除了Hg(11)⁻之外，所有研究的团簇都显示出相似的动力学，在Hg(11)⁻中，最初制备的态不像其他态那样快速衰减。
Electron-nuclear relaxation dynamics are studied in Hg(n) (-) (11 <or= n <or= 16,n = 18) using time-resolved photoelectron imaging. The excess electron in the anion uniquely occupies the p band and is excited intraband by 1.53 eV pump photons; the subsequent dynamics are monitored by photodetachment at 3.06 eV and measurement of the photoelectron images as a function of pump-probe delay. The initially excited state decays on a time scale of approximately 10 ps, and subsequent relaxation dynamics reveal a smooth evolution of the photoelectron spectra towards lower electron kinetic energy over 50-100 ps. Qualitatively, the relaxation process is captured by a simple kinetic model assuming a series of radiationless transitions within a dense manifold of electronic states. All the clusters studied show similar dynamics with the exception of Hg(11) (-) in which the initially prepared state does not decay as quickly as the others.