Improved atmospheric constraints on Southern Ocean CO2 exchange.

We present improved estimates of air-sea CO2 exchange over three latitude bands of the Southern Ocean using atmospheric CO2 measurements from global airborne campaigns and an atmospheric 4-box inverse model based on a mass-indexed isentropic coordinate (Mθe). These flux estimates show two features not clearly resolved in previous estimates based on inverting surface CO2 measurements: a weak winter-time outgassing in the polar region and a sharp phase transition of the seasonal flux cycles between polar/subpolar and subtropical regions. The estimates suggest much stronger summer-time uptake in the polar/subpolar regions than estimates derived through neural-network interpolation of pCO2 data obtained with profiling floats but somewhat weaker uptake than a recent study by Long et al. [Science 374, 1275-1280 (2021)], who used the same airborne data and multiple atmospheric transport models (ATMs) to constrain surface fluxes. Our study also uses moist static energy (MSE) budgets from reanalyses to show that most ATMs tend to have excessive diabatic mixing (transport across moist isentrope, θe, or Mθe surfaces) at high southern latitudes in the austral summer, which leads to biases in estimates of air-sea CO2 exchange. Furthermore, we show that the MSE-based constraint is consistent with an independent constraint on atmospheric mixing based on combining airborne and surface CO2 observations.

Unpiloted Aircraft System Instrument for the Rapid Collection of Whole Air Samples and Measurements for Environmental Monitoring and Air Quality Studies.

A new airborne system, the Whole Air Sampling Pilotless Platform (WASPP), is described for the collection of whole air samples and in situ meteorological measurements onboard a commercial hexacopter. Rapid sample collection enables the collection ≤15 air samples per flight in positively pressurized miniature canisters, subsequently analyzed on a mated analytical system for up to 80 nonmethane volatile organic compounds (VOCs). The WASPP is well suited to investigate VOC gradients in urban environments impacted by traffic, industry, and oil and natural gas (O&NG) development, but has the sensitivity to characterize continental background conditions, as shown here using a subset of >40 species. We document empirical tests to minimize the influence of rotor wash and other sampling artifacts and report favorable results of laboratory-based calibrations of the WASPP's meteorological sensors and field-based comparisons of WASPP's VOC measurements and horizontal wind velocity measurements. Airborne WASPP measurements can complement and enhance ground-based VOC monitoring efforts by providing substantial meteorological and VOC measurement capability across vertical and horizontal spatial scales. These measurements reveal strong vertical gradients in VOC mixing ratios, depending on local meteorology and sources. WASPP has wide applicability for pollution source identification and quantification of hazardous air pollutants and precursors of criteria pollutants, including monitoring O&NG emissions or industry fenceline monitoring.

Long-term urban carbon dioxide observations reveal spatial and temporal dynamics related to urban characteristics and growth.

Cities are concentrated areas of CO2 emissions and have become the foci of policies for mitigation actions. However, atmospheric measurement networks suitable for evaluating urban emissions over time are scarce. Here we present a unique long-term (decadal) record of CO2 mole fractions from five sites across Utah's metropolitan Salt Lake Valley. We examine "excess" CO2 above background conditions resulting from local emissions and meteorological conditions. We ascribe CO2 trends to changes in emissions, since we did not find long-term trends in atmospheric mixing proxies. Three contrasting CO2 trends emerged across urban types: negative trends at a residential-industrial site, positive trends at a site surrounded by rapid suburban growth, and relatively constant CO2 over time at multiple sites in the established, residential, and commercial urban core. Analysis of population within the atmospheric footprints of the different sites reveals approximately equal increases in population influencing the observed CO2, implying a nonlinear relationship with CO2 emissions: Population growth in rural areas that experienced suburban development was associated with increasing emissions while population growth in the developed urban core was associated with stable emissions. Four state-of-the-art global-scale emission inventories also have a nonlinear relationship with population density across the city; however, in contrast to our observations, they all have nearly constant emissions over time. Our results indicate that decadal scale changes in urban CO2 emissions are detectable through monitoring networks and constitute a valuable approach to evaluate emission inventories and studies of urban carbon cycles.

Effect of increasing CO2 on the terrestrial carbon cycle.

Feedbacks from the terrestrial carbon cycle significantly affect future climate change. The CO2 concentration dependence of global terrestrial carbon storage is one of the largest and most uncertain feedbacks. Theory predicts the CO2 effect should have a tropical maximum, but a large terrestrial sink has been contradicted by analyses of atmospheric CO2 that do not show large tropical uptake. Our results, however, show significant tropical uptake and, combining tropical and extratropical fluxes, suggest that up to 60% of the present-day terrestrial sink is caused by increasing atmospheric CO2. This conclusion is consistent with a validated subset of atmospheric analyses, but uncertainty remains. Improved model diagnostics and new space-based observations can reduce the uncertainty of tropical and temperate zone carbon flux estimates. This analysis supports a significant feedback to future atmospheric CO2 concentrations from carbon uptake in terrestrial ecosystems caused by rising atmospheric CO2 concentrations. This feedback will have substantial tropical contributions, but the magnitude of future carbon uptake by tropical forests also depends on how they respond to climate change and requires their protection from deforestation.

Assessment of ground-based atmospheric observations for verification of greenhouse gas emissions from an urban region.

International agreements to limit greenhouse gas emissions require verification to ensure that they are effective and fair. Verification based on direct observation of atmospheric greenhouse gas concentrations will be necessary to demonstrate that estimated emission reductions have been actualized in the atmosphere. Here we assess the capability of ground-based observations and a high-resolution (1.3 km) mesoscale atmospheric transport model to determine a change in greenhouse gas emissions over time from a metropolitan region. We test the method with observations from a network of CO(2) surface monitors in Salt Lake City. Many features of the CO(2) data were simulated with excellent fidelity, although data-model mismatches occurred on hourly timescales due to inadequate simulation of shallow circulations and the precise timing of boundary-layer stratification and destratification. Using two optimization procedures, monthly regional fluxes were constrained to sufficient precision to detect an increase or decrease in emissions of approximately 15% at the 95% confidence level. We argue that integrated column measurements of the urban dome of CO(2) from the ground and/or space are less sensitive than surface point measurements to the redistribution of emitted CO(2) by small-scale processes and thus may allow for more precise trend detection of emissions from urban regions.

Persistent reduced ecosystem respiration after insect disturbance in high elevation forests.

Amid a worldwide increase in tree mortality, mountain pine beetles (Dendroctonus ponderosae Hopkins) have led to the death of billions of trees from Mexico to Alaska since 2000. This is predicted to have important carbon, water and energy balance feedbacks on the Earth system. Counter to current projections, we show that on a decadal scale, tree mortality causes no increase in ecosystem respiration from scales of several square metres up to an 84 km(2) valley. Rather, we found comparable declines in both gross primary productivity and respiration suggesting little change in net flux, with a transitory recovery of respiration 6-7 years after mortality associated with increased incorporation of leaf litter C into soil organic matter, followed by further decline in years 8-10. The mechanism of the impact of tree mortality caused by these biotic disturbances is consistent with reduced input rather than increased output of carbon.

A multi-city urban atmospheric greenhouse gas measurement data synthesis.

Urban regions emit a large fraction of anthropogenic emissions of greenhouse gases (GHG) such as carbon dioxide (CO2) and methane (CH4) that contribute to modern-day climate change. As such, a growing number of urban policymakers and stakeholders are adopting emission reduction targets and implementing policies to reach those targets. Over the past two decades research teams have established urban GHG monitoring networks to determine how much, where, and why a particular city emits GHGs, and to track changes in emissions over time. Coordination among these efforts has been limited, restricting the scope of analyses and insights. Here we present a harmonized data set synthesizing urban GHG observations from cities with monitoring networks across North America that will facilitate cross-city analyses and address scientific questions that are difficult to address in isolation.

Strong Southern Ocean carbon uptake evident in airborne observations.

The Southern Ocean plays an important role in determining atmospheric carbon dioxide (CO2), yet estimates of air-sea CO2 flux for the region diverge widely. In this study, we constrained Southern Ocean air-sea CO2 exchange by relating fluxes to horizontal and vertical CO2 gradients in atmospheric transport models and applying atmospheric observations of these gradients to estimate fluxes. Aircraft-based measurements of the vertical atmospheric CO2 gradient provide robust flux constraints. We found an annual mean flux of ­0.53 ± 0.23 petagrams of carbon per year (net uptake) south of 45°S during the period 2009­2018. This is consistent with the mean of atmospheric inversion estimates and surface-ocean partial pressure of CO2 (Pco2)­based products, but our data indicate stronger annual mean uptake than suggested by recent interpretations of profiling float observations.

Coupled Air Quality and Boundary-Layer Meteorology in Western U.S. Basins during Winter: Design and Rationale for a Comprehensive Study.

Wintertime episodes of high aerosol concentrations occur frequently in urban and agricultural basins and valleys worldwide. These episodes often arise following development of persistent cold-air pools (PCAPs) that limit mixing and modify chemistry. While field campaigns targeting either basin meteorology or wintertime pollution chemistry have been conducted, coupling between interconnected chemical and meteorological processes remains an insufficiently studied research area. Gaps in understanding the coupled chemical-meteorological interactions that drive high pollution events make identification of the most effective air-basin specific emission control strategies challenging. To address this, a September 2019 workshop occurred with the goal of planning a future research campaign to investigate air quality in Western U.S. basins. Approximately 120 people participated, representing 50 institutions and 5 countries. Workshop participants outlined the rationale and design for a comprehensive wintertime study that would couple atmospheric chemistry and boundary-layer and complex-terrain meteorology within western U.S. basins. Participants concluded the study should focus on two regions with contrasting aerosol chemistry: three populated valleys within Utah (Salt Lake, Utah, and Cache Valleys) and the San Joaquin Valley in California. This paper describes the scientific rationale for a campaign that will acquire chemical and meteorological datasets using airborne platforms with extensive range, coupled to surface-based measurements focusing on sampling within the near-surface boundary layer, and transport and mixing processes within this layer, with high vertical resolution at a number of representative sites. No prior wintertime basin-focused campaign has provided the breadth of observations necessary to characterize the meteorological-chemical linkages outlined here, nor to validate complex processes within coupled atmosphere-chemistry models.

Global atmospheric CO2 inverse models converging on neutral tropical land exchange, but disagreeing on fossil fuel and atmospheric growth rate.

We have compared a suite of recent global CO2 atmospheric inversion results to independent airborne observations and to each other, to assess their dependence on differences in northern extratropical (NET) vertical transport and to identify some of the drivers of model spread. We evaluate posterior CO2 concentration profiles against observations from the High-Performance Instrumented Airborne Platform for Environmental Research (HIAPER) Pole-to-Pole Observations (HIPPO) aircraft campaigns over the mid-Pacific in 2009-2011. Although the models differ in inverse approaches, assimilated observations, prior fluxes, and transport models, their broad latitudinal separation of land fluxes has converged significantly since the Atmospheric Carbon Cycle Inversion Intercomparison (TransCom 3) and the REgional Carbon Cycle Assessment and Processes (RECCAP) projects, with model spread reduced by 80% since TransCom 3 and 70% since RECCAP. Most modeled CO2 fields agree reasonably well with the HIPPO observations, specifically for the annual mean vertical gradients in the Northern Hemisphere. Northern Hemisphere vertical mixing no longer appears to be a dominant driver of northern versus tropical (T) annual flux differences. Our newer suite of models still gives northern extratropical land uptake that is modest relative to previous estimates (Gurney et al., 2002; Peylin et al., 2013) and near-neutral tropical land uptake for 2009-2011. Given estimates of emissions from deforestation, this implies a continued uptake in intact tropical forests that is strong relative to historical estimates (Gurney et al., 2002; Peylin et al., 2013). The results from these models for other time periods (2004-2014, 2001-2004, 1992-1996) and reevaluation of the TransCom 3 Level 2 and RECCAP results confirm that tropical land carbon fluxes including deforestation have been near neutral for several decades. However, models still have large disagreements on ocean-land partitioning. The fossil fuel (FF) and the atmospheric growth rate terms have been thought to be the best-known terms in the global carbon budget, but we show that they currently limit our ability to assess regional-scale terrestrial fluxes and ocean-land partitioning from the model ensemble.

Weak northern and strong tropical land carbon uptake from vertical profiles of atmospheric CO2.

Measurements of midday vertical atmospheric CO2 distributions reveal annual-mean vertical CO2 gradients that are inconsistent with atmospheric models that estimate a large transfer of terrestrial carbon from tropical to northern latitudes. The three models that most closely reproduce the observed annual-mean vertical CO2 gradients estimate weaker northern uptake of -1.5 petagrams of carbon per year (Pg C year(-1)) and weaker tropical emission of +0.1 Pg C year(-1) compared with previous consensus estimates of -2.4 and +1.8 Pg C year(-1), respectively. This suggests that northern terrestrial uptake of industrial CO2 emissions plays a smaller role than previously thought and that, after subtracting land-use emissions, tropical ecosystems may currently be strong sinks for CO2.