Studies of Molecules in Strong Laser Fields Using Harmonic Generation and Ion Spectroscopy

利用高强度超快激光脉冲，我们现在可以控制双原子分子的键长和取向。这给了我们一个独特的机会来直接探索分子轨道的结构，并提出一些基本的问题;例如，不同轨道之间是否存在相干性，以及相对论轨道与常规轨道有何不同？除了探测分子结构，我们还将利用我们的能力来操纵分子，以产生分子离子的高激发态，最终目标是在真空紫外光谱区产生粒子数反转。 最后，我们将测试我们的假设，某些配置的分子可能是非常容易产生谐波辐射驱动的一个强大的基本激光。 此外，我们还开发了一种新的相位匹配技术，大大提高了谐波产生的效率，一般。 耦合这两种技术在一起可能会提供一个新的源的强烈的短脉冲真空紫外辐射。更广泛的影响新的相位匹配技术可能会导致一类新的相干，超短脉冲真空紫外辐射源。 该奖项中开发的强场技术可能会导致对物理化学有用的分子结构的重要见解。 更广泛地说，在高次谐波产生，阿秒物理和短脉冲x射线自由电子激光器的兴趣在过去十年中爆炸，这个奖项有助于了解重要的方面，如内轨道电离，激发和振动相干性。 最后，该奖项提供最先进的激光和光学技术的研究培训，并为他们的学术或高科技职业道路做好准备。

Intellectual MeritUsing high-intensity ultra-fast laser pulses we can now control both the bond length and orientation of diatomic molecules. This gives us a unique opportunity to directly probe the structure of molecular orbitals and ask fundamental questions; such as, is there coherence between the different orbitals and how do relativistic orbitals differ from regular orbitals? In addition to probing molecular structure, we will also use our ability to manipulate molecules in order to generate highly excited states of the molecular ions with the ultimate goal of creating population inversions in the vacuum-ultraviolet spectral region. Finally, we will test our hypothesis that certain configurations of the molecule may be highly susceptible to generating harmonic radiation driven by an intense fundamental laser. Moreover, we have developed a new phase-matching technique that greatly enhances the efficiency of harmonic generation, in general. Coupling these two techniques together may provide a new source of intense short-pulse vacuum-ultraviolet radiation.Broader ImpactThe new phase-matching techniques may lead to a new class of coherent, ultra short pulse VUV radiation sources. The strong field techniques developed in this award may lead to important insights into molecular structure useful for physical chemistry. More broadly, interest in high-harmonic generation, attosecond physics, and short-pulse x-ray free electron lasers has exploded over the past decade, and this award contributes towards understanding important aspects such as inner-orbital ionization, excitation, and vibrational coherence. Finally, this award provides hands on research training in state-of-the-art laser and optical technologies and prepares them for academic or high-tech career paths.