CRASY: Mass- or Electron-Correlated Rotational Alignment Spectroscopy

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Science  19 Aug 2011:
Vol. 333, Issue 6045, pp. 1011-1015
DOI: 10.1126/science.1204352

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Rotational spectra have traditionally been measured without a concurrent means of differentiating the molecular constituents of the sample. Here, we present an all-optical multipulse experiment that allows the correlated measurement of rotational and mass or photoelectron spectra by combining Fourier transform rotational coherence spectroscopy with resonance-enhanced multiphoton ionization. We demonstrate the power of this method with the determination of ground-state rotational constants and fragmentation channels for 10 different isotopes in a natural carbon disulfide sample. Three of the reported rotational constants were previously inaccessible by conventional spectroscopic techniques.

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