Distinguishing between old and modern permafrost sources in the northeast Siberian land-shelf system with compound-specific delta H-2 analysis

Pleistocene ice complex permafrost deposits contain roughly a quarter of the organic carbon (OC) stored in permafrost (PF) terrain. When permafrost thaws, its OC is remobilized into the (aquatic) environment where it is available for degradation, transport or burial. Aquatic or coastal environments contain sedimentary reservoirs that can serve as archives of past climatic change. As permafrost thaw is increasing throughout the Arctic, these reservoirs are important locations to assess the fate of remobilized permafrost OC. We here present compound-specific deuterium (delta H-2) analysis on leaf waxes as a tool to distinguish between OC released from thawing Pleistocene permafrost (ice complex deposits; ICD) and from thawing Holocene permafrost (from near-surface soils). Bulk geochemistry (%OC; delta C-13; % total nitrogen, TN) was analyzed as well as the concentrations and delta H-2 signatures of long-chain n-alkanes (C-21 to C-33) and midto long-chain n-alkanoic acids (C-16 to C-30) extracted from both ICD-PF samples (n = 9) and modern vegetation and Ohorizon (topsoil-PF) samples (n = 9) from across the northeast Siberian Arctic. Results show that these topsoil-PF samples have higher %OC, higher OC/TN values and more depleted delta(COC)-C-13 values than ICD-PF samples, suggesting that these former samples trace a fresher soil and/or vegetation source. Whereas the two investigated sources differ on the bulk geochemical level, they are, however, virtually indistinguishable when using leaf wax concentrations and ratios. However, on the molecular isotope level, leaf wax biomarker delta H-2 values are statistically different between topsoil PF and ICD PF. For example, the mean delta H-2 value of C-29 n-alkane was -246 +/- 13% (mean +/- SD) for topsoil PF and -280 +/- 12 parts per thousand for ICD PF. With a dynamic isotopic range (difference between two sources) of 34 to 50 parts per thousand; the isotopic fingerprints of individual, abundant, biomarker molecules from leaf waxes can thus serve as endmembers to distinguish between these two sources. We tested this molecular delta H-2 tracer along with another source-distinguishing approach, dual-carbon (delta C-13-Delta C-14) isotope composition of bulk OC, for a surface sediment transect in the Laptev Sea. Results show that general offshore patterns along the shelfslope transect are similar, but the source apportionment between the approaches vary, which may highlight the advan-tages of either. This study indicates that the application of delta H-2 leaf wax values has potential to serve as a complementary quantitative measure of the source and differential fate of OC thawed out from different permafrost compartments.