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.

中文翻译：

---

“米勒型”复合益生元肉汤的化学分析：第二部分：天然气，石油，水和油/水界面。

我们已经分析了使用核磁共振（NMR）光谱和相干反斯托克斯拉曼散射（CARS）光谱，气相色谱法接着是质谱（GC / MS）和二维气相色谱仪通过Miller-Urey型实验获得的化学品种色谱分析，然后进行质谱分析（GCxGC / MS）。在进行Miller-Urey型实验的过程中，除了最初存在的亲水性水相和气相之外，还出现了疏水性有机层。气相主要由芳族化合物和含有C≡C或C≡N三键的分子组成。亲水相包含至少数千个不同的分子，主要分布在50和500 Da的范围内。疏水相的特征是富含碳，油状化合物及其两亲衍生物，含有具有张活性的氧。各种各样的氧化分子的存在暗示了氧自由基的可用性。我们建议他们干预油/水界面中烷基化聚乙二醇（PEG）的形成。CARS光谱显示出独特的振动分子特征。特别是，如果肉汤是用气相放电制备的，则可以观察到氰化物的特征光谱带。如果释放到水表面，则没有特征谱带。对同一组样品的NMR光谱学独立地证实了这一观察结果。此外，NMR光谱显示整体化学变异性高，这表明由于相互依存，存在强烈的非线性，