Advances in geochemistry have resulted in new analytical techniques for the isolation and identification of ancient molecules or their diageneic products. Sediments or fossils themselves, carefully selected to prevent recent contamination, are first solvent extracted with a Soxhlet apparatus. Extracts are separated into saturates and aromatic fractions through the use of high-performance liquid chromatography. The extracts are analyzed using gas chromatography-mass spectrometry (GC-MS) and metastable reaction monitoring GC-MS (MRM-GC-MS) to confirm the presence of specific molecular fossils, that demonstrate the occurrence of several groups of organisms geologically earlier than their first documented micro-/megafossils. These techniques are now beginning to be applied to plant groups. For example, molecular fossils linked to particular dinoflagellates, diatoms, and chrysophytes have been documented in many sedimentary rocks and petroleum. The use of polycyclic diterpanes as higher plant markers is only beginning. We present preliminary data from Carboniferous coals of eastern North America. The existence of a widespread and unique tetracyclic diterpane signature in Late-Carboniferous coals from Germany, Turkey, and the North America is evidence of a stable and cosmopolitan vegetation community inhabiting these coal swamps. Variations in diterpane abundance appear to track variations in marine influence and dramatically separate paleo-mid latitude coals of Nigeria from paleo-equatorial coals of Europe and North America. A sample set of monospecific coal balls, heterogeneous coals, and fossilized woods is being analyzed to determine which plants are contributing to the diterpane signature. Although individual contributors remain elusive, several microbially produced diterpanes have been identified, and it appears that the higher plant diterpane precursors originated as components of leaf waxes and resinous exudates. Our future goal is ultimately to set up a molecular stratigraphy that will allow the crude dating of petroleum and source rocks that have significant higher plant input.

Key words: Carboniferous, Geochemistry, molecular fossil, MRM-GC-MS.