Journal
CHEMPHYSCHEM
Volume 17, Issue 24, Pages 4052-4058Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201600811
Keywords
circular dichroism; mass spectrometry; resonance-enhanced multiphoton ionization; rotational spectroscopy; supersonic beam cooling
Funding
- German Research Foundation [KA4166/2-1, BO718/10]
- European Research Council [246645-ASC3]
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UV spectroscopy and electronic circular dichroism (ECD) experiments on supersonic-beam-cooled deuterated (R)-(+)-3-methylcyclopentanone ([D-4]-(R)-(+)-3-MCP) have been performed by using a laser mass spectrometer. The spectral resolution not only allowed excitation and CD measurements for single vibronic transitions but also for the rotational P, Q, and R branches of these transitions. The investigated n ->pi*(18(0)(4) 25(0)(1)) transition showed the largest anisotropy factor ever observed for chiral molecules in the gas phase, which, due to residual satu-ration of the excited transition, represents only a lower limit for the real anisotropy factor. Furthermore, one-color (1+1+1) and two-color (1+ 1') resonance-enhanced multiphoton ionization (REMPI) measurements were performed and the effusive-beam (room temperature) and supersonic-beam results for [D-4]-(R)-(+)-3-MCP were compared. These results allowed a differentiation between single-step ECD (comparable to conventional ECD) and cumulative ECD (only possible in multiphoton excitation) under supersonic- beam conditions.
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