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Seasonal variations of atmospheric carbon dioxide (CO₂) in the Northern Hemisphere have increased since the 1950s, but sparse observations have prevented a clear assessment of the patterns of long-term change and the underlying mechanisms. We compare recent aircraft-based observations of CO₂ above the North Pacific and Arctic Oceans to earlier data from 1958 to 1961 and find that the seasonal amplitude at altitudes of 3 to 6 km increased by 50% for 45° to 90° N but by less than 25% for 10° to 45°N. An increase of 30 to 60% in the seasonal exchange of CO₂ by northern extratropical land ecosystems, focused on boreal forests, is implicated, substantially more than simulated by current land ecosystem models. The observations appear to signal large ecological changes in northern forests and a major shift in the global carbon cycle.

This study investigates the use of total column CH4 (XCH4) retrievals from the SCIAMACHY satellite instrument for quantifying large-scale emissions of methane. A unique data set from SCIAMACHY is available spanning almost a decade of measurements, covering a period when the global CH4 growth rate showed a marked transition from stable to increasing mixing ratios. The TM5 4DVAR inverse modelling system has been used to infer CH4 emissions from a combination of satellite and surface measurements for the period 2003–2010. In contrast to earlier inverse modelling studies, the SCIAMACHY retrievals have been corrected for systematic errors using the TCCON network of ground-based Fourier transform spectrometers. The aim is to further investigate the role of bias correction of satellite data in inversions. Methods for bias correction are discussed, and the sensitivity of the optimized emissions to alternative bias correction functions is quantified. It is found that the use of SCIAMACHY retrievals in TM5 4DVAR increases the estimated inter-annual variability of large-scale fluxes by 22% compared with the use of only surface observations. The difference in global methane emissions between 2-year periods before and after July 2006 is estimated at 27–35 Tg yr−1. The use of SCIAMACHY retrievals causes a shift in the emissions from the extra-tropics to the tropics of 50 ± 25 Tg yr−1. The large uncertainty in this value arises from the uncertainty in the bias correction functions. Using measurements from the HIPPO and BARCA aircraft campaigns, we show that systematic errors in the SCIAMACHY measurements are a main factor limiting the performance of the inversions. To further constrain tropical emissions of methane using current and future satellite missions, extended validation capabilities in the tropics are of critical importance.

The Los Angeles megacity, which is home to more than 40% of the population in California, is the second largest megacity in the United States and an intense source of anthropogenic greenhouse gases (GHGs). Quantifying GHG emissions from the megacity and monitoring their spatiotemporal trends are essential to be able to understand the effectiveness of emission control policies. Here we measure carbon dioxide (CO2) and methane (CH4) across the Los Angeles megacity using a novel approach - ground-based remote sensing from a mountaintop site. A Fourier transform spectrometer (FTS) with agile pointing optics, located on Mount Wilson at 1.67 km above sea level, measures reflected near-infrared sunlight from 29 different surface targets on Mount Wilson and in the Los Angeles megacity to retrieve the slant column abundances of CO2, CH4 and other trace gases above and below Mount Wilson. This technique provides persistent space- and time-resolved observations of path-averaged dry-air GHG concentrations, XGHG, in the Los Angeles megacity and simulates observations from a geostationary satellite. In this study, we combined high-sensitivity measurements from the FTS and the panorama from Mount Wilson to characterize anthropogenic CH4 emissions in the megacity using tracer-tracer correlations. During the period between September 2011 and October 2013, the observed XCH4 : XCO2 excess ratio, assigned to anthropogenic activities, varied from 5.4 to 7.3 ppb CH4 (ppm CO2)-1, with an average of 6.4 plus or minus 0.5 ppb CH4 (ppm CO2)-1 compared to the value of 4.6 plus or minus 0.9 ppb CH4 (ppm CO2)-1 expected from the California Air Resources Board (CARB) bottom-up emission inventory. Persistent elevated XCH4 : XCO2 excess ratios were observed in Pasadena and in the eastern Los Angeles megacity. Using the FTS observations on Mount Wilson and the bottom-up CO2 emission inventory, we derived a top-down CH4 emission of 0.39 plus or minus 0.06 Tg CH4 year-1 in the Los Angeles megacity. This is 18-61% larger than the state government's bottom-up CH4 emission inventory and consistent with previous studies.

Attributing observed CO2 variations to human or natural cause is critical to deducing and tracking emissions from observations. We have used in situ CO2 , CO, and planetary boundary layer height (PBLH) measurements recorded during the CalNex-LA (CARB et al., 2008) ground campaign of 15 May-15 June 2010, in Pasadena, CA, to deduce the diurnally varying anthropogenic component of observed CO2 in the megacity of Los Angeles (LA). This affordable and simple technique, validated by carbon isotope observations and WRF-STILT (Weather Research and Forecasting model - Stochastic Time-Inverted Lagrangian Transport model) predictions, is shown to robustly attribute observed CO2 variation to anthropogenic or biogenic origin over the entire diurnal cycle. During CalNex-LA, local fossil fuel combustion contributed up to ~50% of the observed CO2 enhancement overnight, and ~100% of the enhancement near midday. This suggests that sufficiently accurate total column CO2 observations recorded near midday, such as those from the GOSAT or OCO-2 satellites, can potentially be used to track anthropogenic emissions from the LA megacity.

Uncertainty in the future atmospheric burden of methane—a potent greenhouse gas—represents an important challenge to the development of realistic climate projections. Airborne observations of methane suggest that the remote Arctic Ocean could prove to be a potentially important methane source. Uncertainty in the future atmospheric burden of methane, a potent greenhouse gas 1 , represents an important challenge to the development of realistic climate projections. The Arctic is home to large reservoirs of methane, in the form of permafrost soils and methane hydrates 2 , which are vulnerable to destabilization in a warming climate. Furthermore, methane is produced in the surface ocean 3 and the surface waters of the Arctic Ocean are supersaturated with respect to methane 4 , 5 . However, the fate of this oceanic methane is uncertain. Here, we use airborne observations of methane to assess methane efflux from the remote Arctic Ocean, up to latitudes of 82° north. We report layers of increased methane concentrations near the surface ocean, with little or no enhancement in carbon monoxide levels, indicative of a non-combustion source. We further show that high methane concentrations are restricted to areas over open leads and regions with fractional sea-ice cover. Based on the observed gradients in methane concentration, we estimate that sea–air fluxes amount to around 2 mg d −1 m −2 , comparable to emissions seen on the Siberian shelf. We suggest that the surface waters of the Arctic Ocean represent a potentially important source of methane, which could prove sensitive to changes in sea-ice cover.

Airborne and ground‐based measurements during the CalNex (California Research at the Nexus of Air Quality and Climate Change) field study in May/June 2010 show a weekend effect in ozone in the South Coast Air Basin (SoCAB) consistent with previous observations. The well‐known and much‐studied weekend ozone effect has been attributed to weekend reductions in nitrogen oxide (NOx = NO + NO2) emissions, which affect ozone levels via two processes: (1) reduced ozone loss by titration and (2) enhanced photochemical production of ozone due to an increased ratio of non‐methane volatile organic compounds (VOCs) to NOx. In accord with previous assessments, the 2010 airborne and ground‐based data show an average decrease in NOx of 46 ± 11% and 34 ± 4%, respectively, and an average increase in VOC/NOxratio of 48 ± 8% and 43 ± 22%, respectively, on weekends. This work extends current understanding of the weekend ozone effect in the SoCAB by identifying its major causes and quantifying their relative importance from the available CalNex data. Increased weekend production of a VOC‐NOxoxidation product, peroxyacetyl nitrate, compared to a radical termination product, nitric acid, indicates a significant contribution from increased photochemical production on weekends. Weekday‐to‐weekend differences in the products of NOx oxidation show 45 ± 13% and 42 ± 12% more extensive photochemical processing and, when compared with odd oxygen (Ox = O3 + NO2), 51 ± 14% and 22 ± 17% greater ozone production efficiency on weekends in the airborne and ground‐based data, respectively, indicating that both contribute to higher weekend ozone levels in the SoCAB. Key Points A weekend ozone effect is observed in the South Coast Air Basin Reductions in NOx emissions drive weekday and weekend differences in ozone Photochemical ozone production contributes to observed weekend ozone levels

This paper presents top‐down constraints on the magnitude, spatial distribution, and seasonality of nitrous oxide (N2O) emissions over the central United States. We analyze data from tall towers in 2004 and 2008 using a high resolution Lagrangian particle dispersion model paired with both geostatistical and Bayesian inversions. Our results indicate peak N2O emissions in June with a strong seasonal cycle. The spatial distribution of sources closely mirrors data on fertilizer application with particularly large N2O sources over the US Cornbelt. Existing inventories for N2O predict emissions that differ substantially from the inverse model results in both seasonal cycle and magnitude. We estimate a total annual N2O budget over the central US of 0.9–1.2 TgN/yr and an extrapolated budget for the entire US and Canada of 2.1–2.6 TgN/yr. By this estimate, the US and Canada account for 12–15% of the total global N2O source or 32–39% of the global anthropogenic source as reported by the Intergovernmental Panel on Climate Change in 2007. Key Points N2O from the US & Canada accounts for 12–15% of global emissions Emissions closely follow fertilizer use Emissions display seasonality and magnitude different from most inventories

We validate satellite methane observations from the Tropospheric Emission Spectrometer (TES) with 151 aircraft vertical profiles over the Pacific from the HIAPER Pole-to-Pole Observation (HIPPO) program. We find that a collocation window of ±750 km and ±24 h does not introduce significant error in comparing TES and aircraft profiles. We validate both the TES standard product (V004) and an experimental product with two pieces of information in the vertical (V005). We determine a V004 mean bias of 65.8 ppb and random instrument error of 43.3 ppb. For V005 we determine a mean bias of 42.3 ppb and random instrument error of 26.5 ppb in the upper troposphere, and mean biases (random instrument errors) in the lower troposphere of 28.8 (28.7) and 16.9 (28.9) ppb at high and low latitudes respectively. Even when V005 cannot retrieve two pieces of information it still performs better than V004. An observation system simulation experiment (OSSE) with the GEOS-Chem chemical transport model (CTM) and its adjoint shows that TES V004 has only limited value for constraining methane sources. Our successful validation of V005 encourages its production as a standard retrieval to replace V004.

Measurements of atmospheric N2O spanning altitudes from the surface to 14 km, and latitudes from 67°S to 85°N, show high concentrations in the tropics and subtropics, with strong maxima in the middle and upper troposphere. The pattern varies significantly over time scales of a few weeks. Global simulations do not accurately capture observed distributions with latitude, altitude, or time. Inversion results indicate strong, episodic inputs of nitrous oxide from tropical regions (as large as 1 Tg N‐N2O over 9 weeks) are necessary to produce observed vertical and latitudinal distributions. These findings highlight strong tropical sources of N2O with high temporal variability, and the necessity of using full vertical profile observations in deriving emissions from atmospheric measurements. Key Points Measurements of N2O show high concentrations at altitude in the tropics Analysis finds strong, temporally variant N2O emissions from tropical regions Inverse analysis using remote surface observations miss large tropical emissions

The Hudson Bay Lowlands (HBL) is the second largest boreal wetland ecosystem in the world and an important natural source of global atmospheric methane. We quantify the HBL methane emissions by using the GEOS-Chem chemical transport model to simulate aircraft measurements over the HBL from the ARCTAS and pre-HIPPO campaigns in May–July 2008, together with continuous 2004–2008 surface observations at Fraserdale (southern edge of HBL) and Alert (Arctic background). The difference in methane concentrations between Fraserdale and Alert is shown to be a good indicator of HBL emissions, and implies a sharp seasonal onset of emissions in late May (consistent with the aircraft data), a peak in July–August, and a seasonal shut-off in September. The model, in which seasonal variation of emission is mainly driven by surface temperature, reproduces well the observations in summer but its seasonal shoulders are too broad. We suggest that this reflects the suppression of emissions by snow cover and greatly improve the model simulation by accounting for this effect. Our resulting best estimate for HBL methane emissions is 2.3 Tg a−1, several-fold higher than previous estimates (Roulet et al., 1994; Worthy et al., 2000).