Molecular and radiocarbon constraints on sources and degradation of terrestrial organic carbon along the Kolyma paleoriver transect, East Siberian Sea

Abstract

Abstract. Climate warming in northeastern Siberia may induce thaw-mobilization of the organic carbon (OC) now held in permafrost. This study investigated the composition of terrestrial OC exported to Arctic coastal waters to both obtain a natural integration of terrestrial permafrost OC release and to further understand the fate of released carbon in the extensive Siberian Shelf Seas. Application of a variety of elemental, molecular and isotopic (δ13C and Δ14C) analyses of both surface water suspended particulate matter and underlying surface sediments along a 500 km transect from Kolyma River mouth to the mid-shelf of the East Siberian Sea yielded information on the sources, degradation status and transport processes of thaw-mobilized soil OC. A three end-member dual-carbon-isotopic mixing model was applied to deduce the relative contributions from riverine, coastal erosion and marine sources. The mixing model was solved numerically using Monte Carlo simulations to obtain a fair representation of the uncertainties of both end-member composition and the end results. Riverine OC contributions to sediment OC decrease with increasing distance offshore (35±15 to 13±9%), whereas coastal erosion OC exhibits a constantly high contribution (51±11 to 60±12%) and marine OC increases offshore (9±7 to 36±10%). We attribute the remarkably strong imprint of OC from coastal erosion, extending up to ~500 km from the coast, to efficient offshoreward transport in these shallow waters presumably through both the benthic boundary layer and ice-rafting. There are also indications of simultaneous selective preservation of erosion OC compared to riverine OC. Molecular degradation proxies and radiocarbon contents indicated a degraded but young (Δ14C ca. −60‰ or ca. 500 14C years) terrestrial OC pool in surface water particulate matter, underlain by a less degraded but old (Δ14C ca. −500‰ or ca. 5500 14C years) terrestrial OC pool in bottom sediments. We suggest that the terrestrial OC fraction in surface water particulate matter is mainly derived from surface soil and recent vegetation fluvially released as buoyant organic-rich aggregates (e.g., humics), which are subjected to extensive processing during coastal transport. In contrast, terrestrial OC in the underlying sediments is postulated to originate predominantly from erosion of mineral-rich Pleistocene coasts (i.e., yedoma) and inland mineral soils. Sorptive association of this organic matter with mineral particles protects the OC from remineralization and also promotes rapid settling (ballasting) of the OC. Our findings corroborate recent studies by indicating that different Arctic surface soil OC pools exhibit distinguishing susceptibilities to degradation in coastal waters. Consequently, the general postulation of a positive feedback to global warming from degradation of permafrost carbon may be both attenuated (by reburial of one portion) and geographically displaced (degradation of released terrestrial permafrost OC far out over the Arctic shelf seas).