Direct Signatures of Light-Induced Conical Intersections on the Field-Dressed Spectrum of Na2.
Direct Signatures of Light-Induced Conical Intersections on the Field-Dressed Spectrum of Na2.
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DOI：
10.1021/acs.jpclett.8b01102
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发表时间：
2018-04
期刊：
影响因子：
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通讯作者：
Tamás Szidarovszky;G. Halász;A. Császár;L. Cederbaum;Á. Vibók
中科院分区：
文献类型：
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作者：
Tamás Szidarovszky;G. Halász;A. Császár;L. Cederbaum;Á. Vibók
研究了现场处理的同核双原子 Na2 分子的 Rovibronic 光谱，以识别光谱上光致圆锥相交 (LICI) 的直接特征。所制定的理论框架允许计算（1）由中等强度连续波激光引起的场修饰的振动电子态以及（2）这些场修饰状态之间相对于附加弱探测脉冲的跃迁幅度。场处理光谱具有类似于无场光谱的吸收峰以及与无场情况下不可见的跃迁相对应的受激发射峰。通过研究全维和降维模拟中场修整光谱对修整场波长的依赖性，可以识别 LICI 的直接特征。这些特征包括（1）新峰的出现以及吸收和受激发射的峰分裂，以及（2）现场处理光谱中强度借用效应的表现。
Rovibronic spectra of the field-dressed homonuclear diatomic Na2 molecule are investigated to identify direct signatures of the light-induced conical intersection (LICI) on the spectrum. The theoretical framework formulated allows the computation of the (1) field-dressed rovibronic states induced by a medium-intensity continuous-wave laser light and the (2) transition amplitudes between these field-dressed states with respect to an additional weak probe pulse. The field-dressed spectrum features absorption peaks resembling the field-free spectrum as well as stimulated emission peaks corresponding to transitions not visible in the field-free case. By investigating the dependence of the field-dressed spectra on the dressing-field wavelength, in both full- and reduced-dimensional simulations, direct signatures of the LICI can be identified. These signatures include (1) the appearance of new peaks and the splitting of peaks for both absorption and stimulated emission and (2) the manifestation of an intensity-borrowing effect in the field-dressed spectrum.