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arXiv · 1409.7767

Laser pulses for coherent xuv Raman excitation

Loren Greenman·Christiane P. Koch·K. Birgitta Whaley
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Abstract

We combine multi-channel electronic structure theory with quantum optimal control to derive Raman pulse sequences that coherently populate a valence excited state. For a neon atom, Raman target populations of up to 13% are obtained. Superpositions of the ground and valence Raman states with a controllable relative phase are found to be reachable with up to 4.5% population and phase control facilitated by the pump pulse carrier envelope phase. Our results open a route to creating core-hole excitations in molecules and aggregates that locally address specific atoms and represent the first step towards realization of multidimensional spectroscopy in the xuv and x-ray regimes.

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Loren Greenman, Christiane P. Koch, K. Birgitta Whaley. 2014-09-27. Laser pulses for coherent xuv Raman excitation. https://doi.org/10.1103/physreva.92.013407

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