论文标题
时间分辨的THZ鲜明光谱
Time-resolved THz Stark spectroscopy
论文作者
论文摘要
我们通过使用强烈的单周terahertz脉冲作为电场源来引入THZ Stark光谱，并监测各向同性分子集合的诱导光谱响应，并具有一致的flestsecond Supercontinuum脉冲。 THZ Stark光谱法具有比传统的鲜明光谱法具有多个优点，并开放了以前无法访问的观点。最重要的是，THZ脉冲比典型的分子旋转更快，因此消除了冻结样品以防止螺旋效应的要求。因此，THZ Stark光谱允许在任意温度下进行时间分辨研究，特别是与生理或手术条件更相关的环境条件。此外，可以在分子振动或旋转的时间尺度上研究动态场效应，例如，高阶的较高贡献或磁滞效应（非马克维亚行为）。我们展示了两个明智地选择的分子系统的THZ Stark光谱法，并将结果与常规的Stark光谱和第一个原理计算进行了比较。
We introduce THz Stark spectroscopy by using intense single-cycle terahertz pulses as the electric field source and monitoring the induced spectral response of an isotropic molecular ensemble with a coincident femtosecond supercontinuum pulse. THz Stark spectroscopy offers several advantages over conventional Stark spectroscopy and opens previously inaccessible perspectives. Most importantly, THz pulses oscillate faster than typical molecular rotations and consequently eliminate the requirement to freeze the samples to prevent poling effects. Hence, THz Stark spectroscopy allows for time-resolved studies at arbitrary temperatures, specifically ambient conditions more relevant to physiological or operative conditions. Moreover, dynamical field effects, e.g., higher order Stark contributions or hysteresis effects (non-Markovian behavior), can be studied on the time scales of molecular vibrations or rotations. We demonstrate THz Stark spectroscopy for two judiciously selected molecular systems and compare the results to conventional Stark spectroscopy and first principle calculations.
