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. Tracking the sources ofparticulate organic matter (POM) exported from catchments is important tounderstand the transfer of energy from soils to oceans. The suitability ofinvestigating the molecular composition of POM by thermally assistedhydrolysis and methylation using tetramethylammonium hydroxide directlycoupled to gas chromatography and mass spectrometry is presented. The resultsof this molecular-fingerprint approach were compared with previouslypublished elemental (% C, % N) and isotopic data( δ13C , δ15N ) acquired in a nested headwatercatchment in the Piedmont region, eastern United States of America (12 and79  ha ). The concordance between these results highlights theeffectiveness of this molecular tool as a valuable method for sourcefingerprinting of POM. It emphasizes litter as the main source of exportedPOM at the upstream location ( 80±14  %), with an increasingproportion of streambed (SBed) sediment remobilization downstream (42  ±  29 %), specifically during events characterized by high rainfallamounts. At the upstream location, the source of POM seems to be controlledby the maximum and median hourly rainfall intensity. An added value of thismethod is to directly investigate chemical biomarkers and to mine theirdistributions in terms of biogeochemical functioning of an ecosystem. In thiscatchment, the distribution of plant-derived biomarkers characterizinglignin, cutin and suberin inputs were similar in SBed and litter, while theproportion of microbial markers was 4 times higher in SBed than in litter.These results indicate that SBed OM was largely from plant litter that hasbeen processed by the aquatic microbial community.

biogeosciences

Molecular fingerprinting of particulate organic matter as a new tool for its source apportionment: changes along a headwater drainage in coarse, medium and fine particles as a function of rainfalls