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Probing the Dynamics of Rydberg and Valence States of Molecular Nitrogen with Attosecond Transient Absorption Spectroscopy

机译:用阿秒瞬态吸收光谱研究分子氮的里德堡和价态动力学

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摘要

An attosecond pulse is used to create a wavepacket in molecular nitrogen composed of multiple-bound and autoionizing electronic states of Rydberg and valence character between 12 and 16.7 eV. A time-delayed,, few-femtosecond, near-infrared (NIR) laser pulse is used to couple individual state in the wavepacket to multiple neighboring states, resulting in time-dependent modification of the absorption spectrum and revealing both individual quantum beats of the wavepacket and the energy shifts of the excited states in the presence of the strong NIR field: The broad bandwidth of the attosecond pulse and high energy,resolution of the extreme ultraviolet spectrometer allow the simultaneous Observation of time-dependent dynamics cot many, individual vibrational levels in each electronic state. Quantum beating with periods from. 1.3 to 12 fs and transient line shape changes are observed among vibrational levels of a progression of electronically autoionizing Rydberg states leading to the excited A (IIu)-I-2 N-2(+) ion core. Vibrational levels in the valence b (IIu)-I-1 state exhibit 50 fs oscillation periods, revealing superpositions between individual vibrational levels within this state. Comparisons are, made to previous studies of electronic wavepackets in atoms that highlight similarities to atomic behavior yet illustrate unique contributions of the diatomic molecular structure to the wavepacket, including the influence of different electronic potentials and vibrational-level-specific electronic dynamics.
机译:阿秒脉冲用于在分子氮中创建一个波包,该波包由里德堡的多重结合和电离电子态以及12至16.7 eV之间的价态特征组成。使用延时的,几飞秒的近红外(NIR)激光脉冲将波包中的单个状态耦合到多个相邻状态,从而导致吸收光谱随时间的变化,并揭示了两个单独的量子拍波包和强NIR场存在下激发态的能量转移:阿秒脉冲的宽带宽和高能量,极紫外光谱仪的分辨率允许同时观察随时间变化的动力学,包括许多单独的振动水平在每种电子状态下。量子从周期开始跳动。在电子自动电化的里德堡态的振动水平之间观察到1.3至12 fs和瞬态线形变化,从而导致激发的A(IIu)-I-2 N-2(+)离子核。 b(IIu)-I-1价态的振动能级显示50 fs的振荡周期,揭示了该状态下各个振动能级之间的叠加。与先前对原子中电子波包的研究进行了比较,这些研究突出了与原子行为的相似性,但也说明了双原子分子结构对波包的独特贡献,包括不同电势和特定于振动水平的电子动力学的影响。

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