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Characterization of light-induced potentials in the strong-field dissociation ofO2+
Physical Review A ( IF 2.6 ) Pub Date : 2020-11-24 , DOI: 10.1103/physreva.102.053114 P. M. Abanador , U. Thumm
Physical Review A ( IF 2.6 ) Pub Date : 2020-11-24 , DOI: 10.1103/physreva.102.053114 P. M. Abanador , U. Thumm
We investigate theoretically the imprints of light-induced potentials (LIPs) on the dissociation dynamics of molecular ions, as observable in angle-resolved fragment kinetic-energy-release (KER) spectra. Following the vibrational and rotational dynamics of the initial pump-laser-excited cationic nuclear wave packet, while accounting for the dipole coupling between the and electronic states in 800-nm 40-fs probe-laser pulses with peak intensities between and , we calculate angle-resolved KER spectra which reveal characteristic energy- and angle-dependent fringe structures. These fringes shift downward in energy as the molecular alignment angle relative to the probe-pulse polarization direction increases from 0 to . The angle-dependent shifts in the KER fringes increase for larger probe-pulse peak intensities and follow the angle and light-wave-intensity dependence of the vibrational spectrum in the associated Floquet bond-hardening well, which is a manifestation of transient nuclear-probability trapping in the LIP during dissociation. By examining the rovibrational dynamics of the dissociating molecular cation near the light-induced conical intersection (LICI) in the cationic LIP surface at , we identify related angle-dependent structures in the KER spectra, suggesting a means for assessing the significance of LICIs in molecular dissociation pathways.
中文翻译:
O2 +强场解离中光诱导势的表征
我们在理论上研究光致电势(LIPs)的解离动力学的烙印 角分辨片段动能释放(KER)光谱中可以观察到的分子离子 遵循初始泵激激光激发的阳离子核波包的振动和旋转动力学,同时考虑了两者之间的偶极耦合 和 800-nm 40-fs探测激光脉冲中的电子态,其峰值强度在 和 ,我们计算了角度分辨的KER光谱,揭示了特征性的依赖于能量和角度的条纹结构。这些条纹的能量随着分子排列角向下移动 相对于探测脉冲的极化方向从0增加到 。对于较大的探测脉冲峰值强度,KER条纹中与角度相关的位移会增加,并且在相关的Floquet键硬化井中遵循振动光谱的角度和光波强度相关性,这是瞬态的一种表现。解离过程中LIP中的核概率陷阱。通过检查阳离子LIP表面上光诱导圆锥形交叉点(LICI)附近解离的分子阳离子的旋转动力学,我们确定了KER光谱中相关的角度依赖性结构,这表明了一种评估LICIs在分子解离途径中的意义的方法。
更新日期:2020-11-25
中文翻译:
O2 +强场解离中光诱导势的表征
我们在理论上研究光致电势(LIPs)的解离动力学的烙印 角分辨片段动能释放(KER)光谱中可以观察到的分子离子 遵循初始泵激激光激发的阳离子核波包的振动和旋转动力学,同时考虑了两者之间的偶极耦合 和 800-nm 40-fs探测激光脉冲中的电子态,其峰值强度在 和 ,我们计算了角度分辨的KER光谱,揭示了特征性的依赖于能量和角度的条纹结构。这些条纹的能量随着分子排列角向下移动 相对于探测脉冲的极化方向从0增加到 。对于较大的探测脉冲峰值强度,KER条纹中与角度相关的位移会增加,并且在相关的Floquet键硬化井中遵循振动光谱的角度和光波强度相关性,这是瞬态的一种表现。解离过程中LIP中的核概率陷阱。通过检查阳离子LIP表面上光诱导圆锥形交叉点(LICI)附近解离的分子阳离子的旋转动力学,我们确定了KER光谱中相关的角度依赖性结构,这表明了一种评估LICIs在分子解离途径中的意义的方法。