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

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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.