title: Understanding the application of Raman spectroscopy to the detection of traces of life.
abstract: Investigating carbonaceous microstructures and material in Earth's oldest sedimentary rocks is an essential part of tracing the origins of life on our planet; furthermore, it is important for developing techniques to search for traces of life on other planets, for example, Mars. NASA and ESA are considering the adoption of miniaturized Raman spectrometers for inclusion in suites of analytical instrumentation to be placed on robotic landers on Mars in the near future to search for fossil or extant biomolecules. Recently, Raman spectroscopy has been used to infer a biological origin of putative carbonaceous microfossils in Early Archean rocks. However, it has been demonstrated that the spectral signature obtained from kerogen (of known biological origin) is similar to spectra obtained from many poorly ordered carbonaceous materials that arise through abiotic processes. Yet there is still confusion in the literature as to whether the Raman spectroscopy of carbonaceous materials can indeed delineate a signature of ancient life. Despite the similar nature in spectra, rigorous structural interrogation between the thermal alteration products of biological and nonbiological organic materials has not been undertaken. Therefore, we propose a new way forward by investigating the second derivative, deconvolution, and chemometrics of the carbon first-order spectra to build a database of structural parameters that may yield distinguishable characteristics between biogenic and abiogenic carbonaceous material. To place Raman spectroscopy as a technique to delineate a biological origin for samples in context, we will discuss what is currently accepted as a spectral signature for life; review Raman spectroscopy of carbonaceous material; and provide a historical overview of Raman spectroscopy applied to Archean carbonaceous materials, interpretations of the origin of the ancient carbonaceous material, and a future way forward for Raman spectroscopy.
authors.affiliation: Department of Geology, The University of Kansas, Lawrence, KS 66045, USA. cpmarshall@ku.edu
authors.forename: Craig P
authors.initials: CP
authors.lastname: Marshall
authors.forename: Howell G M
authors.initials: HG
authors.lastname: Edwards
authors.forename: Jan
authors.initials: J
authors.lastname: Jehlicka
mesh_terms: D001105:Archaea / Q000378:metabolism; D002244:Carbon / Q000737:chemistry; D018534:Earth, Planet; D005060:Europe; D018559:Exobiology / Q000295:instrumentation* / Q000379:methods*; D005580:Fossils; D019015:Geologic Sediments / Q000032:analysis; D006358:Hot Temperature; D007834:Lasers; D018535:Mars; D008956:Models, Chemical; D013059:Spectrum Analysis, Raman / Q000295:instrumentation* / Q000379:methods*; D014481:United States; D018557:United States National Aeronautics and Space Administration
chemical_list: D002244:Carbon