The First Global Evaluation of Dissolved Organic Carbon

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Presentation transcript:

The First Global Evaluation of Dissolved Organic Carbon Sarah Safieddine and Colette Heald 05/01/2017

Emissions [TgCyr-1] Deposition [TgCyr-1] The Reactive Organic Carbon (ROC) is Essential for Tropospheric Chemistry Safieddine, Heald, and Henderson, 2017 CH4 oxidation Emissions [TgCyr-1] Biogenic Anthropogenic/biofuel Biomass Oceans(net) NMVOC: 15 TgC OA : 1 TgC Deposition [TgCyr-1] CO 905 TgCyr-1 Emissions [TgCyr-1] 400 ROC 515 TgCyr-1 415 TgCyr-1 370 TgCyr-1 CO2 1275 TgCyr-1 935 TgCyr-1 460 TgCyr-1 Improving the understanding of the composition and evolution of dissolved organic carbon (DOC) will therefore provide constraints on atmospheric reactive organic carbon (ROC) lifecycle Wet: 272 Dry: 188 ROC is simulated by expanding the GEOS-Chem standard simulation, including: new emissions and chemistry, expanding the wet and dry deposition scheme, and ensuring carbon closure.

Seasonal Dissolved Organic Carbon (DOC) DJF JJA Rain [mm/day] Atmospheric Reactive Organic Carbon (ROC) Column Concentration [µgC/m2] Dissolved Organic Carbon (DOC) concentration [mgC/L] The global DOC is calculated from the wet deposition flux of atmospheric reactive carbon divided by the global precipitation.

DOC Simulated vs Observed: Surprisingly Good Agreement! Iavorivska et al., 2016 Comparison of the 2010 simulated DOC with a 30-year record of available DOC measurements over different environments and regions, shows a good correlation (r= 0.67) with simulated DOC values underestimating the observation by 34%.

Average Carbon Oxidation State: Derived by GEOS-Chem, Measured by AMS The average carbon oxidation state is metric for the degree of oxidation of atmospheric organic species, a quantity that necessarily increases upon oxidation Kroll et al., 2011 Explain x and y axis here Higher organics carbon number are lumped Mass spectrometry techniques provide key information on the chemical composition of organics, such as the average carbon oxidation state, which can be derived from GEOS-Chem. Mass Spectrometry techniques provide key

First Average Carbon Oxidation State (OSc) Derived From a Model we lump thing so less species than in the kroll diagram. In the dissolved form, DOC OSc is generally higher than ROC OSc due to increase of solubility upon oxidation

The First Simulated Spatial Average Carbon Oxidation State Safieddine and Heald, in prep In the atmosphere, ROC OSc is governed by alkanes with lower photochemistry (oxidation) leading to a lower OSc in winter of the Northern Hemisphere In the dissolved form, DOC OSc is more uniform and generally higher than ROC OSc due to increase of solubility upon oxidation

Conclusions and Future Work Wet deposition is the largest physical sink of reactive organic carbon Improving the understanding of the composition and evolution of dissolved organic carbon (DOC) will therefore provide constraints on atmospheric reactive organic carbon (ROC) lifecycle DOC depends on local sources and chemical processing of reactive organic carbon, as well as precipitation Precipitation Dissolved Organic Carbon ROC is dominated by chemically reduced hydrocarbons and acetone and DOC is dominated globally by semi-volatiles, formaldehyde, and POA. 𝑂𝑆 𝑐 is negative for most of ROC and DOC compounds and is higher in dissolved form due to increase of solubility upon oxidation. Focus on the US: analysis of NADP data will provide DOC values and information on the sample chemical composition for model evaluation.