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James S Wang

Publications and source records attributed to James S Wang.

The Impacts of Fossil Fuel Emission Uncertainties and Accounting for 3-D Chemical CO2 Production on Inverse Natural Carbon Flux Estimates from Satellite and In Situ Data

Atmospheric carbon dioxide (CO2) inversions for estimating natural carbon fluxes typically do not allow for adjustment of fossil fuel CO2 emissions, despite significant uncertainties in emission inventories and inadequacies in the specification of international bunker emissions in inversions. Also, most inversions place CO2 release from fossil fuel combustion and biospheric sources entirely at the surface. However, a non-negligible portion of the emissions actually occurs in the form of reduced carbon species, which are eventually oxidized to CO2 downwind. Omission of this ‘chemical pump’ can result in a significant redistribution of the inferred total carbon fluxes among regions. We assess the impacts of different prescriptions of fossil fuel emissions and accounting for the chemical pump on flux estimation, with a novel aspect of conducting both satellite CO2 observation-based and surface in situ-based inversions. We apply 3-D carbon monoxide (CO) loss rates archived from a state-of-the-art GEOS chemistry and climate model simulation in a forward transport model run to simulate the distribution of CO2 originating from oxidation of carbon species. We also subtract amounts from the prior surface CO2 fluxes that are actually emitted in the form of fossil and biospheric CO, methane, and nonmethane volatile organic compounds (VOCs). We find that the posterior large-scale fluxes are generally insensitive to the finer-scale spatial differences between the ODIAC and CDIAC fossil fuel CO2 gridded datasets and assumptions about international bunker emissions. However, accounting for 3-D chemical CO2 production and the surface correction shifts the global carbon sink, e.g., from land to ocean and from the tropics to the north, with a magnitude and even direction that depend on assumptions about the surface correction. A GOSAT satellite-based inversion is more sensitive to the chemical pump than one using in situ observations, exhibiting substantial flux impacts of 0.28, 0.53, and -0.47 Pg C yr(exp -1) over tropical land, global land, and oceans, due to differences in the horizontal and vertical sampling of the wo observation types. Overall, the biases from neglecting the chemical pump appear to be minor relative to the flux estimate uncertainties and the differences between the in situ and GOSAT inversions, but their relative importance will grow in the future as observational coverage further increases and satellite retrieval biases decrease.

James S Wang↗

Strong Sensitivity of the Isotopic Composition of Methane to the Plausible Range of Tropospheric Chlorine

The C-13 isotopic ratio of methane, δC-13 of CH4, provides additional constraints on the CH4 budget to complement the constraints from CH4 observations. The interpretation of δC-13 observations is complicated, however, by uncertainties in the methane sink. The reaction of CH4 with Cl is highly fractionating, increasing the relative abundance of 13CH4, but there is currently no consensus on the strength of the tropospheric Cl sink. Global model simulations of halogen chemistry differ strongly from one another in terms of both the magnitude of tropospheric Cl and its geographic distribution. This study explores the impact of the inter-model diversity in Cl fields on the simulated δC-13 of CH4. We use a set of GEOS global model simulations with different predicted Cl fields to test the sensitivity of the δC-13 of CH4 to the diversity of Cl output from chemical transport models. We find that δC-13 is highly sensitive to both the amount and geographic distribution of Cl. Simulations with Cl providing 0.28% or 0.66% of the total CH4 loss bracket the δC-13 observations for a fixed set of emissions. Thus, even when Cl provides only a small fraction of the total CH4 loss and has a small impact on total CH4, it provides a strong lever on δC-13. Consequently, it is possible to achieve a good representation of total CH4 using widely different Cl concentrations, but the partitioning of CH4 loss between the OH and Cl reactions leads to strong differences in isotopic composition depending on which model’s Cl field is used. Comparing multiple simulations, we find that altering the tropospheric Cl field leads to approximately a 0.5‰ increase in δ(13)CH4for each percent increase in how much CH4 is oxidized by Cl. The geographic distribution and seasonal cycle of Cl also impacts the hemispheric gradient and seasonal cycle of δC-13. The large effect of Cl on δC-13 compared to total CH4 broadens the range of CH4 source mixtures that can be reconciled with δC-13 observations. Stronger constraints on tropospheric Cl are necessary to improve estimates of CH4 sources from δC-13 observations.

Global model simulations of halogen chemistry↗

Space-Based Observations for Understanding Changes in the Arctic-Boreal Zone

Observations taken over the last few decades indicate that dramatic changes are occurring in the ArcticBoreal Zone (ABZ), which are having significant impacts on ABZ inhabitants, infrastructure, flora and fauna, and economies. While suitable for detecting overall change, the current capability is inadequate for systematic monitoring and for improving process based and large scale understanding of the integrated components of the ABZ, which includes the cryosphere, biosphere, hydrosphere, and atmosphere. Such knowledge will lead to improvements in Earth system models, enabling more accurate prediction of future changes and development of informed adaptation and mitigation strategies. In this article, we review the strengths and limitations of current space based observational capabilities for several important ABZ components and make recommendations for improving upon these current capabilities. We recommend an interdisciplinary and stepwise approach to develop a comprehensive ABZ Observing Network (ABZON), beginning with an initial focus on observing networks designed to gain process based understanding for individual ABZ components and systems that can then serve as the building blocks for a comprehensive ABZON.

Bryan N Duncan↗

The Description and Validation of a Computationally-Efficient CH4-CO-OH (ECCOH) Module for 3D Model Applications

We present the Efficient CH4-CO-OH Module (ECCOH) that allows for the simulation of the methane, carbon monoxide and hydroxyl radical (CH4-CO-OH cycle, within a chemistry climate model, carbon cycle model, or earth system model. The computational efficiency of the module allows many multi-decadal, sensitivity simulations of the CH4-CO-OH cycle, which primarily determines the global tropospheric oxidizing capacity. This capability is important for capturing the nonlinear feedbacks of the CH4-CO-OH system and understanding the perturbations to relatively long-lived methane and the concomitant impacts on climate. We implemented the ECCOH module into the NASA GEOS-5 Atmospheric Global Circulation Model (AGCM), performed multiple sensitivity simulations of the CH4-CO-OH system over two decades, and evaluated the model output with surface and satellite datasets of methane and CO. The favorable comparison of output from the ECCOH module (as configured in the GEOS-5 AGCM) with observations demonstrates the fidelity of the module for use in scientific research.

Remote Sensing↗