Abstract

We present a novel multi-pulse spectroscopic method for the correlated analysis of molecular mass, rotational structure and electronic structure. First experiments investigate carbon disulfide and butadiene.

Highlights

  • We present a novel multi-pulse spectroscopic method for the correlated analysis of molecular mass, rotational structure and electronic structure

  • Electrons and ions formed in molecular ionization can be detected with quantum yields close to one, leading to an extraordinarily sensitive characterization of molecular mass and electronic structure

  • We recently presented the spectroscopic method of correlated rotational alignment spectroscopy (CRASY) to overcome this limitation [5]

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Summary

Introduction

The presented method is based on the excitation of a rotational wave packet in the molecular electronic and vibrational ground state of molecules by means of non-adiabatic or (“impulsive”) alignment. We present a novel multi-pulse spectroscopic method for the correlated analysis of molecular mass, rotational structure and electronic structure. Electrons and ions formed in molecular ionization can be detected with quantum yields close to one, leading to an extraordinarily sensitive characterization of molecular mass and electronic structure. The information content of such experiments, is insufficient for a spectroscopic assignment of molecular structure in all but the most trivial molecules.

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