Necessary,but Not Sufficient: Raman Identification of Disordered Carbon as a Signature of Ancient Life

Abstract

To identify microscopic particles as actual fossil material, it would be useful to have a means of unambiguously recognizing which carbonaceous deposits found in rocks are residues from once-living organisms(i.e., biogenic material). Those residues consist of many different, mostly aromatic (i.e., benzene ring-containing), C-O-H-dominated molecules, and typically are called kerogens. Raman microprobe spectroscopy can be applied to minute samples of ancient kerogens either isolated from their host rocks or in situ in thin section. The Raman spectra generated by monochromatic blue or green laser excitation (e.g., at 488, 514, 532 nm) typically show only generic spectral features indicative of discontinuous arrays of condensed benzene rings (i.e., structures referred to as "disordered carbonaceous material"). Thus, despite the complex chemistry of kerogens and the expected presence of H, O, and N, the Raman spectra typically do not show any evidence of functional groups, such as CH, CH₂, CH₃, CO, and CN. Moreover, the same kind of Raman spectral signature as is obtained from kerogens also is obtained from many other poorly ordered carbonaceous materials that arise through nonbiological processes, such as in situ heating of organic or inorganic compounds (whether or not they are of biological origin), metamorphic mobilization of preexisting carbon compounds, and high-temperature precipitation from hydrothermal solutions. Thus, neither a Raman spectrum, nor a Raman image derived from such spectra, definitively can identify a sample as "kerogen," but only as "disordered carbonaceous material." Clearly, the fact that small, opaque grains consist of disordered carbonaceous material is necessary, but not sufficient, to prove them to be residues of cellular material and, thus, biogenic.