Time-resolved four-wave-mixing spectroscopy for inner-valence transitions.
Time-resolved four-wave-mixing spectroscopy for inner-valence transitions.
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DOI：
10.1364/ol.41.000709
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发表时间：
2015-10
期刊：
影响因子：
3.6
通讯作者：
T. Ding;C. Ott;A. Kaldun;A. Blättermann;K. Meyer;V. Stooß;M. Rebholz;P. Birk;M. Hartmann;A. Brown;H. W. van der Hart;T. Pfeifer
中科院分区：
文献类型：
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作者：
T. Ding;C. Ott;A. Kaldun;A. Blättermann;K. Meyer;V. Stooß;M. Rebholz;P. Birk;M. Hartmann;A. Brown;H. W. van der Hart;T. Pfeifer
近红外（NIR）、可见光和紫外频率的非线性四波混频（FWM）技术已被广泛用于绘制振动和电子耦合，特别是在复杂分子中。然而，在极紫外（XUV）光谱范围内，分子不同位点之间的空间定域内价跃迁之间的相关性尚未被观察到。作为实现这一目标的实验步骤，我们使用飞秒近红外和阿秒XUV脉冲进行时间分辨FWM光谱。前两个脉冲（XUV-NIR）在时间上重合，作为相干激励场，而第三个脉冲（NIR）作为探针。作为第一个应用，我们展示了如何使用二维光谱表示来揭示氖的奇偶宇称、内价激发态之间的耦合动力学。实验得到的结果与从头算时相关的r矩阵计算结果一致，提供了多电子相互作用的完整描述，以及低水平的模型模拟。该方法的未来应用还包括分子中电子过程的位点特异性探测。
Noncollinear four-wave-mixing (FWM) techniques at near-infrared (NIR), visible, and ultraviolet frequencies have been widely used to map vibrational and electronic couplings, typically in complex molecules. However, correlations between spatially localized inner-valence transitions among different sites of a molecule in the extreme ultraviolet (XUV) spectral range have not been observed yet. As an experimental step toward this goal, we perform time-resolved FWM spectroscopy with femtosecond NIR and attosecond XUV pulses. The first two pulses (XUV-NIR) coincide in time and act as coherent excitation fields, while the third pulse (NIR) acts as a probe. As a first application, we show how coupling dynamics between odd- and even-parity, inner-valence excited states of neon can be revealed using a two-dimensional spectral representation. Experimentally obtained results are found to be in good agreement with ab initio time-dependent R-matrix calculations providing the full description of multielectron interactions, as well as few-level model simulations. Future applications of this method also include site-specific probing of electronic processes in molecules.