ALBERT

Description: Accurate simulation of atmospheric circulation, particularly in the lower stratosphere, is challenging due to unresolved wave–mean flow interactions and limited high-resolution observations for validation. Gravity-induced pressure gradients lead to a small but measurable separation of heavy and light gases by molecular diffusion in the stratosphere. Because the relative abundance of Ar to N2 is exclusively controlled by physical transport, the argon-to-nitrogen ratio (Ar∕N2) provides an additional constraint on circulation and the age of air (AoA), i.e., the time elapsed since entry of an air parcel into the stratosphere. Here we use airborne measurements of N2O and Ar∕N2 from nine campaigns with global coverage spanning 2008–2018 to calculate AoA and to quantify gravitational separation in the lowermost stratosphere. To this end, we develop a new N2O–AoA relationship using a Markov chain Monte Carlo algorithm. We observe that gravitational separation increases systematically with increasing AoA for samples with AoA between 0 and 3 years. These observations are compared to a simulation of the TOMCAT/SLIMCAT 3-D chemical transport model, which has been updated to include gravitational fractionation of gases. We demonstrate that although AoA at old ages is slightly underestimated in the model, the relationship between Ar∕N2 and AoA is robust and agrees with the observations. This highlights the potential of Ar∕N2 to become a new AoA tracer that is subject only to physical transport phenomena and can supplement the suite of available AoA indicators.

Description: A regional atmospheric inversion method has been developed to determine the spatial and temporal distribution of CO2 sinks and sources across New Zealand for 2011–2013. This approach infers net air–sea and air–land CO2 fluxes from measurement records, using back-trajectory simulations from the Numerical Atmospheric dispersion Modelling Environment (NAME) Lagrangian dispersion model, driven by meteorology from the New Zealand Limited Area Model (NZLAM) weather prediction model. The inversion uses in situ measurements from two fixed sites, Baring Head on the southern tip of New Zealand's North Island (41.408° S, 174.871° E) and Lauder from the central South Island (45.038° S, 169.684° E), and ship board data from monthly cruises between Japan, New Zealand, and Australia. A range of scenarios is used to assess the sensitivity of the inversion method to underlying assumptions and to ensure robustness of the results. The results indicate a strong seasonal cycle in terrestrial land fluxes from the South Island of New Zealand, especially in western regions covered by indigenous forest, suggesting higher photosynthetic and respiratory activity than is evident in the current a priori land process model. On the annual scale, the terrestrial biosphere in New Zealand is estimated to be a net CO2 sink, removing 98 (±37) Tg CO2 yr−1 from the atmosphere on average during 2011–2013. This sink is much larger than the reported 27 Tg CO2 yr−1 from the national inventory for the same time period. The difference can be partially reconciled when factors related to forest and agricultural management and exports, fossil fuel emission estimates, hydrologic fluxes, and soil carbon change are considered, but some differences are likely to remain. Baseline uncertainty, model transport uncertainty, and limited sensitivity to the northern half of the North Island are the main contributors to flux uncertainty.

Description: Despite the need for researchers to understand terrestrial biospheric carbon fluxes to account for carbon cycle feedbacks and predict future CO2 concentrations, knowledge of these fluxes at the regional scale remains poor. This is particularly true in mountainous areas, where complex meteorology and lack of observations lead to large uncertainties in carbon fluxes. Yet mountainous regions are often where significant forest cover and biomass are found – i.e., areas that have the potential to serve as carbon sinks. As CO2 observations are carried out in mountainous areas, it is imperative that they are properly interpreted to yield information about carbon fluxes. In this paper, we present CO2 observations at three sites in the mountains of the western US, along with atmospheric simulations that attempt to extract information about biospheric carbon fluxes from the CO2 observations, with emphasis on the observed and simulated diurnal cycles of CO2. We show that atmospheric models can systematically simulate the wrong diurnal cycle and significantly misinterpret the CO2 observations, due to erroneous atmospheric flows as a result of terrain that is misrepresented in the model. This problem depends on the selected vertical level in the model and is exacerbated as the spatial resolution is degraded, and our results indicate that a fine grid spacing of ∼ 4 km or less may be needed to simulate a realistic diurnal cycle of CO2 for sites on top of the steep mountains examined here in the American Rockies. In the absence of higher resolution models, we recommend coarse-scale models to focus on assimilating afternoon CO2 observations on mountaintop sites over the continent to avoid misrepresentations of nocturnal transport and influence.

Description: The Southern Ocean is highly under-sampled for the purpose of assessing total carbon uptake and its variability. Since this region dominates the mean global ocean sink for anthropogenic carbon, understanding temporal change is critical. Underway measurements of pCO2 collected as part of the Drake Passage Time-series (DPT) program that began in 2002 inform our understanding of seasonally changing air–sea gradients in pCO2, and by inference the carbon flux in this region. Here, we utilize available pCO2 observations to evaluate how the seasonal cycle, interannual variability, and long-term trends in surface ocean pCO2 in the Drake Passage region compare to that of the broader subpolar Southern Ocean. Our results indicate that the Drake Passage is representative of the broader region in both seasonality and long-term pCO2 trends, as evident through the agreement of timing and amplitude of seasonal cycles as well as trend magnitudes both seasonally and annually. The high temporal density of sampling by the DPT is critical to constraining estimates of the seasonal cycle of surface pCO2 in this region, as winter data remain sparse in areas outside of the Drake Passage. An increase in winter data would aid in reduction of uncertainty levels. On average over the period 2002–2016, data show that carbon uptake has strengthened with annual surface ocean pCO2 trends in the Drake Passage and the broader subpolar Southern Ocean less than the global atmospheric trend. Analysis of spatial correlation shows Drake Passage pCO2 to be representative of pCO2 and its variability up to several hundred kilometers away from the region. We also compare DPT data from 2016 and 2017 to contemporaneous pCO2 estimates from autonomous biogeochemical floats deployed as part of the Southern Ocean Carbon and Climate Observations and Modeling project (SOCCOM) so as to highlight the opportunity for evaluating data collected on autonomous observational platforms. Though SOCCOM floats sparsely sample the Drake Passage region for 2016–2017 compared to the Drake Passage Time-series, their pCO2 estimates fall within the range of underway observations given the uncertainty on the estimates. Going forward, continuation of the Drake Passage Time-series will reduce uncertainties in Southern Ocean carbon uptake seasonality, variability, and trends, and provide an invaluable independent dataset for post-deployment assessment of sensors on autonomous floats. Together, these datasets will vastly increase our ability to monitor change in the ocean carbon sink.

Description: Fluxes of halogenated volatile organic compounds (VOCs) over the Southern Ocean remain poorly understood, and few atmospheric measurements exist to constrain modeled emissions of these compounds. We present observations of CHBr3, CH2Br2, CH3I, CHClBr2, CHBrCl2, and CH3Br during the O2∕N2 Ratio and CO2 Airborne Southern Ocean (ORCAS) study and the second Atmospheric Tomography mission (ATom-2) in January and February of 2016 and 2017. Good model–measurement correlations were obtained between these observations and simulations from the Community Earth System Model (CESM) atmospheric component with chemistry (CAM-Chem) for CHBr3, CH2Br2, CH3I, and CHClBr2 but all showed significant differences in model : measurement ratios. The model : measurement comparison for CH3Br was satisfactory and for CHBrCl2 the low levels present precluded us from making a complete assessment. Thereafter, we demonstrate two novel approaches to estimate halogenated VOC fluxes; the first approach takes advantage of the robust relationships that were found between airborne observations of O2 and CHBr3, CH2Br2, and CHClBr2. We use these linear regressions with O2 and modeled O2 distributions to infer a biological flux of halogenated VOCs. The second approach uses the Stochastic Time-Inverted Lagrangian Transport (STILT) particle dispersion model to explore the relationships between observed mixing ratios and the product of the upstream surface influence of sea ice, chl a, absorption due to detritus, and downward shortwave radiation at the surface, which in turn relate to various regional hypothesized sources of halogenated VOCs such as marine phytoplankton, phytoplankton in sea-ice brines, and decomposing organic matter in surface seawater. These relationships can help evaluate the likelihood of particular halogenated VOC sources and in the case of statistically significant correlations, such as was found for CH3I, may be used to derive an estimated flux field. Our results are consistent with a biogenic regional source of CHBr3 and both nonbiological and biological sources of CH3I over these regions.

Description: The Orbiting Carbon Observatory-2 has been on orbit since 2014, and its global coverage holds the potential to reveal new information about the carbon cycle through the use of top-down atmospheric inversion methods combined with column average CO2 retrievals. We employ a large ensemble of atmospheric inversions utilizing different transport models, data assimilation techniques, and prior flux distributions in order to quantify the satellite-informed fluxes from OCO-2 Version 7r land observations and their uncertainties at continental scales. Additionally, we use in situ measurements to provide a baseline against which to compare the satellite-constrained results. We find that within the ensemble spread, in situ observations, and satellite retrievals constrain a similar global total carbon sink of 3.7±0.5 PgC yr−1, and 1.5±0.6 PgC yr−1 for global land, for the 2015–2016 annual mean. This agreement breaks down in smaller regions, and we discuss the differences between the experiments. Of particular interest is the difference between the different assimilation constraints in the tropics, with the largest differences occurring in tropical Africa, which could be an indication of the global perturbation from the 2015–2016 El Niño. Evaluation of posterior concentrations using TCCON and aircraft observations gives some limited insight into the quality of the different assimilation constraints, but the lack of such data in the tropics inhibits our ability to make strong conclusions there.

Description: Despite the need for researchers to understand terrestrial biospheric carbon fluxes to account for carbon cycle feedbacks and predict future CO2 concentrations, knowledge of these fluxes at the regional scale remains poor. This is particularly true in mountainous areas, where complex meteorology and lack of observations lead to large uncertainties in carbon fluxes. Yet mountainous regions are often where significant forest cover and biomass are found – i.e., areas that have the potential to serve as carbon sinks. As CO2 observations are carried out in mountainous areas, it is imperative that they are properly interpreted to yield information about carbon fluxes. In this paper, we present CO2 observations at 3 sites in the mountains of the Western U.S., along with atmospheric simulations that attempt to extract information about biospheric carbon fluxes from the CO2 observations, with emphasis on the observed and simulated diurnal cycles of CO2. We show that atmospheric models can systematically simulate the wrong diurnal cycle and significantly misinterpret the CO2 observations, due to erroneous atmospheric flows as a result of terrain that is misrepresented in the model. This problem depends on the selected vertical level in the model and are exacerbated as the spatial resolution is degraded, and our results indicate that a fine grid spacing of ~ 4 km or less may be needed to simulate a realistic diurnal cycle of CO2 for sites on top of the steep mountains examined here in the American Rockies. In the absence of higher resolution models, we recommend coarse-scale models to focus on assimilating afternoon CO2 observations on mountaintop sites over the continent to avoid misrepresentations of nocturnal transport and influence.

Description: We present observations of CHBr3, CH2Br2, CH3I, CHClBr2, and CHBrCl2 from the Trace Gas Organic Analyzer (TOGA) during the O2/N2 Ratio and CO2 Airborne Southern Ocean (ORCAS) study and the 2nd Atmospheric Tomography mission (ATom-2), in January and February of 2016 and 2017. We also use CH3Br from the University of Miami Advanced Whole Air Sampler (AWAS) on ORCAS and from the UC Irvine Whole Air Sampler (WAS) on ATom-2. We compare our observations with simulations from the Community Atmosphere Model with Chemistry (CAM-Chem). We report regional enrichment ratios of CHBr3 and CH2Br2 to O2 of 0.19 ± 0.01, and 0.07 ± 0.004 pmol : mol, poleward of 60° S between 180° W and 55° W, and of 0.32 ± 0.02, 0.07 ± 0.004 pmol : mol over the Patagonian Shelf, between 40° S and 55° S and between 70° W and 55° W where we also report enrichment ratios of CH3I to O2 of 0.38 ± 0.03 pmol : mol and of CH2ClBr2 to O2 of 0.19 ± 0.04 pmol: mol. Using the Stochastic Time-Inverted Lagrangian Transport (STILT) particle dispersion model, we use correlations between halogenated hydrocarbon mixing ratios and the upwind influences of chlorophyll a, sea ice, solar radiation, and dissolved organic material to investigate previously hypothesized sources of halogenated volatile organic compounds (HVOCs) in the southern high latitudes. Our results are consistent with a biogenic regional source of CHBr3, and both non-biological and biological sources of CH3I over these regions, but do not corroborate a regional sea-ice source of HVOCs in January and February. Based on these relationships, we estimate the average two-month (Jan.-Feb.) emissions poleward of 60° S between 180° W and 55° W of CHBr3, CH2Br2, CH3I, and CHClBr2 to be 91 ± 8, 31 ± 17, 35 ± 29, and 11 ± 4 pmol m−2 hr−1, and regional emissions of these gases over the Patagonian Shelf to be 329 ± 23, 69 ± 5, 392 ± 32, 24 ± 4 pmol m−2 hr−1 respectively.

Description: Monitoring the terrestrial carbon cycle for responses to disturbances, caused for example by extreme climate events and insect outbreaks, has the potential to provide early warnings about ecosystem change. However, our capability to detect these carbon balance responses by atmospheric CO2 monitoring remains unknown despite sub-ppm comparability of many well-calibrated CO2 measurement sites. Here, this study explores how accurately atmospheric CO2 and transport models can detect imposed carbon flux anomalies against a background terrestrial flux. Air mass back trajectories from three CO2 monitoring stations in the central U.S. Rocky Mountains for one year (2008) were computationally simulated. To simulate reduced CO2 uptake, a constant +0.2 µmol C m−1 s−2 anomaly was added to all surface fluxes within perturbation domains of varying size. A spatially and temporally uniform 10°×10° +0.2 µmol C m−2 s−1 flux anomaly (+6 Tg C m−1) was detectable above a comprehensive model-data mismatch detection threshold in a large majority of months at each site, but only when the perturbation was located in the central Mountain West. The intensity of the perturbation and its area were important to detection, but the effect of area declined exponentially with increasing source-to-station distance. To further evaluate response, a more realistic spatiotemporally varying drought extracted from a dynamic global vegetation model with a monthly varying perturbation area (1°×1° to 5°×5°) and higher peak intensity (+0.8 µmol C m−2 s−1) was applied. Detectability of excess CO2 from this experiment by the nearest CO2 site (Utah) was similar to detectability of the largest (10°×10°) uniform perturbation. These experiments demonstrate disturbance and drought related carbon-cycle perturbations do create a discernible impact on the composite signal of atmospheric CO2 if sufficiently proximal to a measurement station.