TY - THES A1 - Menges, Johanna T1 - Organic Carbon Storage, Transfer and Transformation in the Himalaya BT - insights from the Kali Gandaki Valley in Central Nepal N2 - The transfer of particulate organic carbon from continents to the ocean is an important component of the global carbon cycle. Transfer to and burial of photosynthetically fixed biospheric organic carbon in marine sediments can effectively sequester atmospheric carbon dioxide over geological timescales. The exhumation and erosion of fossil organic carbon contained in sedimentary rocks, i.e. petrogenic carbon, can result in remineralization, releasing carbon to the atmosphere. In contrast, eroded petrogenic organic carbon that gets transferred back to the ocean and reburied does not affect atmospheric carbon content. Mountain ranges play a key role in this transfer since they can source vast amounts of sediment including particulate organic carbon. Globally, the export of both, biospheric and petrogenic organic carbon has been linked to sediment export. Additionally, short transfer times from mountains to the ocean and high sediment concentrations have been shown to increase the likelihood of organic carbon burial. While the importance of mountain ranges in the organic carbon cycle is now widely recognized, the processes acting within mountain ranges to influence the storage, cycling and mobilization of organic carbon, as well as carbon fluxes from mountain ranges remain poorly constrained. In this thesis, I employ different methods to assess the nature and fate of particulate organic carbon in mountain belts, ranging from the molecular to regional landscape scale. These studies are located along the Trans-Himalayan Kali Gandaki River in Central Nepal. This river traverses all major geological and climatic zones of the Himalaya, from the dry northern Tibetan plateau to the high-relief, monsoon dominated steep High Himalaya and the lower relief and abundant vegetation of the Lesser Himalayan region. First, I document how biospheric organic matter has accumulated during the Holocene in the headwaters of the Kali Gandaki River valley, by combining compound specific isotope measurements with different dating methods and grain size data, and investigate the stability of this organic carbon reservoir on millennial timescales. I show, that around 1.6 ka an eco-geomorphic tipping point occurred leading to a destabilization of the landscape resulting in today’s high erosion rates and the excavation of the aged organic carbon reservoir. This study highlights the climatic and geomorphic controls on biospheric organic carbon storage and release from mountain ranges. Second, I systematically investigate the spatial variation of particulate organic carbon fluxes across the Himalaya along the Kali Gandaki River, using bulk stable and radioactive isotopes combined with a new Bayesian modeling approach. The detailed dataset allows the distinction of aged and modern biospheric organic carbon as well as petrogenic organic carbon across the Himalayan mountain range and the investigation of the role of climatic and geomorphic factors in their riverine export. The data suggest a decoupling of the particulate organic carbon from the sediment yield along the Kali Gandaki River, partially driven by climatic and geomorphic processes. In contrast to the suspended sediment, a large part of the particulate organic carbon exported by the river originates from the Tibetan part of the catchment and is dominated by petrogenic organic carbon derived from Jurassic shales with only minor contributions of modern and aged biospheric organic carbon. These findings emphasize the importance of organic carbon source distribution and erosion mechanisms in determining the organic carbon export from mountain ranges. In a third step, I explore the potential of ultra-high resolution mass spectrometry for particulate organic carbon transport studies. I have generated a novel and unprecedented high-resolution molecular dataset, which contains up to 103 molecular formulas of the lipid fraction of particulate organic matter for modern and aged biospheric carbon, petrogenic organic carbon and river sediments. First, I test if this dataset can be used to better resolve different organic carbon sources and to identify new geochemical tracers. Using multivariate statistics, I identify up to 10² characteristic molecular formulas for the major organic carbon sources in the upper part of the Kali Gandaki catchment, and trace their transfer from the surrounding landscape into the river sediment. Second, I test the potential of the molecular dataset to trace molecular transformations along source-to-sink pathways. I identify changes in molecular metrics derived from the dataset, which are characteristic of transformation processes during incorporation of litter into soil, the aging of soil material, and the mobilization of the organic carbon into the river. These two studies demonstrate that high-resolution molecular datasets open a promising analytical window on particulate organic carbon and can provide novel insights into the composition, sourcing and transformation of riverine particulate organic carbon. Collectively, these studies advance our understanding of the processes contributing to the storage and mobilization of organic carbon in the Central Himalaya, the mountain belt that dominates global erosional fluxes. They do so by identifying the major sources of particulate organic carbon to the Trans-Himalayan Kali Gandaki River, by elucidating their sensitivity to climate and geomorphic processes, and by identifying some of the transformations of this material on the molecular scale. As a result, the thesis demonstrates that the amount and composition of organic carbon routed from mountain belts is a function of the dynamic interactions of geologic, biologic, geomorphic and climatic processes within the mountain belt. This understanding will ultimately help in answering whether the build-up and erosion of mountain ranges over geological time represents a net carbon source or sink to the atmosphere. Beyond this, the thesis contributes to our technical ability to characterize organic matter and attribute it to sources by scoping the potential of high-end molecular analysis. KW - organic carbon cycle KW - biomarker KW - isotopes KW - Himalaya KW - rivers Y1 - 2020 ER - TY - JOUR A1 - Menges, Johanna A1 - Hovius, Niels A1 - Andermann, Christoff A1 - Lupker, Maarten A1 - Haghipour, Negar A1 - Märki, Lena A1 - Sachse, Dirk T1 - Variations in organic carbon sourcing along a trans-Himalayan river determined by a Bayesian mixing approach JF - Geochimica et cosmochimica acta : journal of the Geochemical Society and the Meteoritical Society N2 - Rivers transfer particulate organic carbon (POC) from eroding mountains into geological sinks. Organic carbon source composition and selective mobilization have been shown to affect the type and quantity of POC export, but their combined effects across complex mountain ranges remain underexplored. Here, we examine the variation in organic carbon sourcing and transport in the trans-Himalayan Kali Gandaki River catchment, along strong gradients in precipitation, rock type and vegetation. Combining bulk stable nitrogen, and stable and radioactive organic carbon isotopic composition of bedrock, litter, soil and river sediment samples with a Bayesian end-member mixing approach, we differentiate POC sources along the river and quantify their export. Our analysis shows that POC export from the Tibetan segment of the catchment, where carbon bearing shales are partially covered by aged and modern soils, is dominated by petrogenic POC. Based on our data we re-assess the presence of aged biospheric OC in this part of the catchment, and its contribution to the river load. In the High Himalayan segment, we observed low inputs of petrogenic and biospheric POC, likely due to very low organic carbon concentrations in the metamorphic bedrock, combined with erosion dominated by deep-seated landslides. Our findings show that along the Kali Gandaki River, the sourcing of sediment and organic carbon are decoupled, due to differences in rock organic carbon content, soil and above ground carbon stocks, and geomorphic process activity. While the fast eroding High Himalayas are the principal source of river sediment, the Tibetan headwaters, where erosion rates are lower, are the principal source of organic carbon. To robustly estimate organic carbon export from the Himalayas, the mountain range should be divided into tectono-physiographic zones with distinct organic carbon yields due to differences in substrate and erosion processes and rates. KW - particulate organic carbon KW - Himalaya KW - rivers KW - carbon cycle KW - stable KW - isotopes KW - erosion KW - end-member mixing Y1 - 2020 U6 - https://doi.org/10.1016/j.gca.2020.07.003 SN - 0016-7037 VL - 286 SP - 159 EP - 176 PB - Elsevier CY - New York [u.a.] ER -