论文标题
表征具有高谐波边带光谱的粒子状电荷迁移动力学
Characterizing Particle-Like Charge Migration Dynamics with High-Harmonic Sideband Spectroscopy
论文作者
论文摘要
我们引入了高谐波侧带光谱（HHSS），并表明它可以是卤代电荷迁移（CM）的强大探针。我们使用从头开始的时间依赖性密度功能理论模拟CM和谐波生成（HHG）动力学。我们发现，沿分子主链启动的CM动力学会在HHG光谱中诱导侧带，该光谱由延迟的激光脉冲驱动，该激光脉冲延迟垂直于分子轴。监视频谱作为HHG激光频率或扫描相对延迟，可以提取有关CM过程的时域特征的详细信息。
We introduce high-harmonic sideband spectroscopy (HHSS) and show that it can be a robust probe of attosecond charge migration (CM) in a halogenated carbon-chain molecule. We simulate both the CM and harmonic-generation (HHG) dynamics using ab initio time-dependent density-functional theory. We find that CM dynamics initiated along the molecular backbone induces sidebands in the HHG spectrum driven by a delayed laser pulse that is polarized perpendicular to the molecular axis. Monitoring the spectrum as either the HHG laser frequency or the relative delay is scanned allows for the extraction of detailed information about the time-domain characteristics of the CM process.
