title: Chemical Analysis of a "Miller-Type" Complex Prebiotic Broth : Part II: Gas, Oil, Water and the Oil/Water-Interface.
abstract: We have analyzed the chemical variety obtained by Miller-Urey-type experiments using nuclear magnetic resonance (NMR) spectroscopy and coherent anti-Stokes Raman scattering (CARS) spectroscopy, gas chromatography followed by mass spectrometry (GC/MS) and two-dimensional gas chromatography followed by mass spectrometry (GCxGC/MS). In the course of a running Miller-Urey-type experiment, a hydrophobic organic layer emerged besides the hydrophilic aqueous phase and the gaseous phase that were initially present. The gas phase mainly consisted of aromatic compounds and molecules containing C≡C or C≡N triple bonds. The hydrophilic phase contained at least a few thousands of different molecules, primarily distributed in a range of 50 and 500 Da. The hydrophobic phase is characterized by carbon-rich, oil-like compounds and their amphiphilic derivatives containing oxygen with tensioactive properties. The presence of a wide range of oxidized molecules hints to the availability of oxygen radicals. We suggest that they intervene in the formation of alkylated polyethylene glycol (PEG) in the oil/water interface. CARS spectroscopy revealed distinct vibrational molecular signatures. In particular, characteristic spectral bands for cyanide compounds were observed if the broth was prepared with electric discharges in the gaseous phase. The characteristic spectral bands were absent if discharges were released onto the water surface. NMR spectroscopy on the same set of samples independently confirmed the observation. In addition, NMR spectroscopy revealed overall high chemical variability that suggests strong non-linearities due to interdependent, sequential reaction steps.
authors.affiliation: Biologische Experimentalphysik, Universität des Saarlandes, Campus, Geb. B2 1, 66123, Saarbrücken, Germany. sabrina.scherer@physik.uni-saarland.de.
authors.forename: Sabrina
authors.initials: S
authors.lastname: Scherer
authors.affiliation: Biologische Experimentalphysik, Universität des Saarlandes, Campus, Geb. B2 1, 66123, Saarbrücken, Germany.|Laboratory of Microbial Morphogenesis and Growth, Institut Pasteur, 75724, Paris, Cedex 15, France.
authors.forename: Eva
authors.initials: E
authors.lastname: Wollrab
authors.affiliation: Centre of Biomolecular Drug Research, Leibniz University, Schneiderberg 38, 30167, Hannover, Germany.
authors.forename: Luca
authors.initials: L
authors.lastname: Codutti
authors.affiliation: Centre of Biomolecular Drug Research, Leibniz University, Schneiderberg 38, 30167, Hannover, Germany.
authors.forename: Teresa
authors.initials: T
authors.lastname: Carlomagno
authors.affiliation: Coherent Raman Scattering Microscopy and Single-Molecule Spectroscopy Group, 3. Institute of Physics, University of Stuttgart, Pfaffenwaldring 57, 70569, Stuttgart, Germany.
authors.forename: Stefan Gomes
authors.initials: SG
authors.lastname: da Costa
authors.affiliation: Coherent Raman Scattering Microscopy and Single-Molecule Spectroscopy Group, 3. Institute of Physics, University of Stuttgart, Pfaffenwaldring 57, 70569, Stuttgart, Germany.
authors.forename: Andreas
authors.initials: A
authors.lastname: Volkmer
authors.affiliation: Applied Analytical Chemistry, University of Duisburg-Essen, Campus Essen, S05 T01 B35, Universitaetsstr. 5, 45141, Essen, Germany.
authors.forename: Amela
authors.initials: A
authors.lastname: Bronja
authors.affiliation: Applied Analytical Chemistry, University of Duisburg-Essen, Campus Essen, S05 T01 B35, Universitaetsstr. 5, 45141, Essen, Germany.
authors.forename: Oliver J
authors.initials: OJ
authors.lastname: Schmitz
authors.affiliation: Biologische Experimentalphysik, Universität des Saarlandes, Campus, Geb. B2 1, 66123, Saarbrücken, Germany.
authors.forename: Albrecht
authors.initials: A
authors.lastname: Ott
mesh_terms: D005740:Gases / Q000032:analysis*; D009821:Oils / Q000032:analysis*; D000069497:Origin of Life; D014867:Water / Q000032:analysis*
chemical_list: D005740:Gases; D009821:Oils; D014867:Water
keywords: Complex chemical mixture; GC/MS; GCxGC/MS; Miller-Urey experiment; Molecular vibrations; NMR; Oil/water interface; Origin of Life; Phase-transfer-catalysis; Radicals; coherent anti-Stokes Raman scattering (CARS)