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中国物理学会期刊

拉伸到大核间距的分子离子谐波辐射谱上复杂干涉结构的物理起源

CSTR: 32037.14.aps.72.20222410

Physical origins of complex interference structures in harmonic emission from molecular ions stretched to large internuclear distances

CSTR: 32037.14.aps.72.20222410
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  • 通过数值和解析的方法研究了拉伸到大核间距的分子离子的高次谐波辐射, 重点研究了与短轨道贡献相关的谐波辐射谱的精细结构. 研究结果表明, 大核间距分子离子的短轨道谐波辐射谱呈现了复杂的干涉结构. 通过利用一个考虑了电荷共振效应的强场近似模型, 可以分辨这些复杂的干涉结构的物理起源: 谐波辐射谱上一些干涉最小来源于电离过程中的两中心干涉效应, 而另外一些干涉最小来源于再结合过程中的两中心干涉效应, 电离干涉最小与再结合干涉最小交替出现. 与电离过程不同, 再结合过程中, 库仑加速会显著改变再结合电子的德布罗意波长, 从而改变干涉最小的位置.

     

    High-order harmonic generation (HHG) from the molecular ions stretched to large internuclear distances is studied numerically and analytically in this work. We focus on the fine structure of the HHG spectrum related to the contribution of short electron trajectory. In our numerically solving the time-dependent Schrodinger equation (TDSE), we use a trajectory-dependent filtering procedure to separate the short-trajectory contribution from other contributions of long trajectory and multiple returns. Our TDSE results reveal that the short-trajectory HHG spectra of molecular ion with larger internuclear distance show some complex interference structures characterized by some remarkable dips, and that the position of the dip is sensitive to the laser parameters. With a developed model arising from strong-field approximation (SFA), we are able to identify the physical origins of the complex interference structures. In this model considered is the charge-resonance effect which induces the strong coupling between the ground state and the first excited state of the molecular ion at large internuclear distance. In this model, the well-known effect of two-center interference occurs in the form of the canonical momentum instead of the momentum related to the instantaneous velocity of the electron in the general SFA. It is shown that some dips in TDSE results arise from two-center interference of the electronic wave between these two atomic cores of the molecule in the ionization process, while others come from that in the recombination process. These ionization and recombination dips alternately appear in the HHG spectra from the formed complex interference structures. The main differences between the interference effects in the ionization process and the recombination process are twofold. Firstly, in the ionization process, the destructive two-center interference strongly suppresses the forming of the continuum wavepacket, while in the recombination process, the recombination of the rescattering electron with other bound eigenstates with small weights can also contribute to HHG bedsides the recombination of the ground state with the first excited state with large weights. As a result, in TDSE results, the ionization dips are deeper and more remarkable than the recombination ones. Secondly, in the recombination process, the Coulomb acceleration remarkably changes the de Broglie wavelength of the rescattering electron and therefore changes the position of the interference-induced dip. While in the ionization process, the Coulomb potential plays a small role in the interference effect. As a result, the interference dips in the ionization process and the recombination process differ from each other.

     

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