Large areas of Amazonian evergreen forest experience seasonal droughts extending for three or more months, yet show maximum rates of photosynthesis and evapotranspiration during dry intervals. This apparent resilience is belied by disproportionate mortality of the large trees in manipulations that reduce wet season rainfall, occurring after 2–3 years of treatment. The goal of this study is to characterize the mechanisms that produce these contrasting ecosystem responses. A mechanistic model is developed based on the ecohydrological framework of TIN (Triangulated Irregular Network)-based Real Time Integrated Basin Simulator + Vegetation Generator for Interactive Evolution (tRIBS+VEGGIE). The model is used to test the roles of deep roots and soil capillary flux to provide water to the forest during the dry season. Also examined is the importance of “root niche separation,” in which roots of overstory trees extend to depth, where during the dry season they use water stored from wet season precipitation, while roots of understory trees are concentrated in shallow layers that access dry season precipitation directly. Observational data from the Tapajós National Forest, Brazil, were used as meteorological forcing and provided comprehensive observational constraints on the model. Results strongly suggest that deep roots with root niche separation adaptations explain both the observed resilience during seasonal drought and the vulnerability of canopy-dominant trees to extended deficits of wet season rainfall. These mechanisms appear to provide an adaptive strategy that enhances productivity of the largest trees in the face of their disproportionate heat loads and water demand in the dry season. A sensitivity analysis exploring how wet season rainfall affects the stability of the rainforest system is presented.

Accurately estimating biogenic methane (CH₄) and nitrous oxide (N₂O) fluxes in terrestrial ecosystems is critical for resolving global budgets of these greenhouse gases (GHGs) and continuing to mitigate climate warming. Here, we assess contemporary biogenic CH₄ and N₂O budgets and probable climate-change-related impacts on CH₄ and N₂O emissions in terrestrial North America. Multi-approach estimations show that, during 1990-2010, biogenic CH₄ emissions ranged from 0.159 to 0.502 petagrams of carbon dioxide (CO₂) equivalents per year (Pg CO₂eq yr⁻¹, where 1 Pg = 1 × 10¹⁵ g) and N₂O emissions ranged from 0.802 to 1.016 Pg CO₂ eq yr⁻¹, which offset 47-166% of terrestrial CO₂ sequestration (0.915-2.040 Pg CO₂ eq yr⁻¹, as indicated elsewhere in this Special Issue). According to two future climate scenarios, CH₄ and N₂O emissions are projected to continue increasing by 137-151% and 157-227%, respectively, by the end of this century, as compared with levels during 2000-2010. Strategies to mitigate climate change must account for non-CO₂ GHG emissions, given their substantial warming potentials.

Airborne measurements of methane (CH4) and carbon dioxide (CO2) were taken over the rice growing region of California's Sacramento Valley in the late spring of 2010 and 2011. From these and ancillary measurements, we show that CH4 mixing ratios were higher in the planetary boundary layer above the Sacramento Valley during the rice growing season than they were before it, which we attribute to emissions from rice paddies. We derive daytime emission fluxes of CH4 between 0.6 and 2.0% of the CO2 taken up by photosynthesis on a per carbon, or mole to mole, basis. We also use a mixing model to determine an average CH 4/CO2 flux ratio of -0.6% for one day early in the growing season of 2010. We conclude the CH4/CO2 flux ratio estimates from a single rice field in a previous study are representative of rice fields in the Sacramento Valley. If generally true, the California Air Resources Board (CARB) greenhouse gas inventory emission rate of 2.7×10¹⁰g CH4/yr is approximately three times lower than the range of probable CH4 emissions (7.8-9.3×10 ¹⁰g CH4/yr) from rice cultivation derived in this study. We attribute this difference to decreased burning of the residual rice crop since 1991, which leads to an increase in CH4 emissions from rice paddies in succeeding years, but which is not accounted for in the CARB inventory. © 2012. American Geophysical Union. All Rights Reserved.

We describe a pragmatic approach for evaluating the spatial representativeness of flux tower measurements based on footprint climatology modeling analyses of land cover and remotely sensed vegetation indices. The approach was applied to the twelve flux sites of the Canadian Carbon Program (CCP) that include grassland, wetland, and temperate and boreal forests across an east–west continental gradient. The spatial variation within the footprint area was evaluated by examining the spatial structure of Normalized Difference Vegetation Index (NDVI) and land cover using geostatistical analyses of frequency distribution, variogram and window size. The results show that at most sites (i) the percentages of the target vegetation functional type (dominant land cover) observed by the CCP towers were higher than 60%; (ii) to some extent, most of the CCP sites presented anisotropically distributed patterns of NDVI in the 90% annual footprint climatology area; and (iii) the land surface heterogeneity within the flux footprint area differed among sites. Overall, the forest sites had larger fine-scale spatial variation than the grassland and wetland sites. The coniferous boreal forest sites had greater spatial variability than the two wetland sites and a coniferous temperate forest site. We conclude that the combination of footprint modeling, semivariogram and window size techniques, together with moderate spatial resolution remotely-sensed image data, is a pragmatic approach for assessing the spatial representativeness of flux tower measurements.

Tropical regions, especially the Amazon region, account for large emissions of methane (CH₄). Here, we present CH₄ observations from two airborne campaigns conducted within the BARCA (Balanço Atmosférico Regional de Carbono na Amazônia) project in the Amazon basin in November 2008 (end of the dry season) and May 2009 (end of the wet season). We performed continuous measurements of CH₄ onboard an aircraft for the first time in the Amazon region, covering the whole Amazon basin with over 150 vertical profiles between altitudes of 500 m and 4000 m. The observations support the finding of previous ground-based, airborne, and satellite measurements that the Amazon basin is a large source of atmospheric CH₄. Isotope analysis verified that the majority of emissions can be attributed to CH₄ emissions from wetlands, while urban CH₄ emissions could be also traced back to biogenic origin. A comparison of five TM5 based global CH₄ inversions with the observations clearly indicates that the inversions using SCIAMACHY observations represent the BARCA observations best. The calculated CH₄ flux estimate obtained from the mismatch between observations and TM5-modeled CH₄ fields ranges from 36 to 43 mg m⁻² d⁻¹ for the Amazon lowland region.

We use historical and new atmospheric trace gas observations to refine the estimated source of methane (CH(4)) emitted into California's South Coast Air Basin (the larger Los Angeles metropolitan region). Referenced to the California Air Resources Board (CARB) CO emissions inventory, total CH(4) emissions are 0.44 ± 0.15 Tg each year. To investigate the possible contribution of fossil fuel emissions, we use ambient air observations of methane (CH(4)), ethane (C(2)H(6)), and carbon monoxide (CO), together with measured C(2)H(6) to CH(4) enhancement ratios in the Los Angeles natural gas supply. The observed atmospheric C(2)H(6) to CH(4) ratio during the ARCTAS (2008) and CalNex (2010) aircraft campaigns is similar to the ratio of these gases in the natural gas supplied to the basin during both these campaigns. Thus, at the upper limit (assuming that the only major source of atmospheric C(2)H(6) is fugitive emissions from the natural gas infrastructure) these data are consistent with the attribution of most (0.39 ± 0.15 Tg yr(-1)) of the excess CH(4) in the basin to uncombusted losses from the natural gas system (approximately 2.5-6% of natural gas delivered to basin customers). However, there are other sources of C(2)H(6) in the region. In particular, emissions of C(2)H(6) (and CH(4)) from natural gas seeps as well as those associated with petroleum production, both of which are poorly known, will reduce the inferred contribution of the natural gas infrastructure to the total CH(4) emissions, potentially significantly. This study highlights both the value and challenges associated with the use of ethane as a tracer for fugitive emissions from the natural gas production and distribution system.

We present the results of airborne measurements of carbon monoxide (CO) and aerosol particle number concentration (CN) made during the Balanço Atmosférico Regional de Carbono na Amazônia (BARCA) program. The primary goal of BARCA is to address the question of basin-scale sources and sinks of CO₂ and other atmospheric carbon species, a central issue of the Large-scale Biosphere-Atmosphere (LBA) program. The experiment consisted of two aircraft campaigns during November–December 2008 (BARCA-A) and May–June 2009 (BARCA-B), which covered the altitude range from the surface up to about 4500 m, and spanned most of the Amazon Basin.

Based on meteorological analysis and measurements of the tracer, SF₆, we found that airmasses over the Amazon Basin during the late dry season (BARCA-A, November 2008) originated predominantly from the Southern Hemisphere, while during the late wet season (BARCA-B, May 2009) low-level airmasses were dominated by northern-hemispheric inflow and mid-tropospheric airmasses were of mixed origin. In BARCA-A we found strong influence of biomass burning emissions on the composition of the atmosphere over much of the Amazon Basin, with CO enhancements up to 300 ppb and CN concentrations approaching 10 000 cm⁻³; the highest values were in the southern part of the Basin at altitudes of 1–3 km. The ΔCN/ΔCO ratios were diagnostic for biomass burning emissions, and were lower in aged than in fresh smoke. Fresh emissions indicated CO/CO₂ and CN/CO emission ratios in good agreement with previous work, but our results also highlight the need to consider the residual smoldering combustion that takes place after the active flaming phase of deforestation fires.

During the late wet season, in contrast, there was little evidence for a significant presence of biomass smoke. Low CN concentrations (300–500 cm⁻³) prevailed basinwide, and CO mixing ratios were enhanced by only ~10 ppb above the mixing line between Northern and Southern Hemisphere air. There was no detectable trend in CO with distance from the coast, but there was a small enhancement of CO in the boundary layer suggesting diffuse biogenic sources from photochemical degradation of biogenic volatile organic compounds or direct biological emission.

Simulations of CO distributions during BARCA-A using a range of models yielded general agreement in spatial distribution and confirm the important contribution from biomass burning emissions, but the models evidence some systematic quantitative differences compared to observed CO concentrations. These mismatches appear to be related to problems with the accuracy of the global background fields, the role of vertical transport and biomass smoke injection height, the choice of model resolution, and reliability and temporal resolution of the emissions data base.

Accurately simulating gross primary productivity (GPP) in terrestrial ecosystem models is critical because errors in simulated GPP propagate through the model to introduce additional errors in simulated biomass and other fluxes. We evaluated simulated, daily average GPP from 26 models against estimated GPP at 39 eddy covariance flux tower sites across the United States and Canada. None of the models in this study match estimated GPP within observed uncertainty. On average, models overestimate GPP in winter, spring, and fall, and underestimate GPP in summer. Models overpredicted GPP under dry conditions and for temperatures below 0°C. Improvements in simulated soil moisture and ecosystem response to drought or humidity stress will improve simulated GPP under dry conditions. Adding a low-temperature response to shut down GPP for temperatures below 0°C will reduce the positive bias in winter, spring, and fall and improve simulated phenology. The negative bias in summer and poor overall performance resulted from mismatches between simulated and observed light use efficiency (LUE). Improving simulated GPP requires better leaf-to-canopy scaling and better values of model parameters that control the maximum potential GPP, such asε_max (LUE), V_cmax (unstressed Rubisco catalytic capacity) or J_max (the maximum electron transport rate).

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 CO₂ surface monitors in Salt Lake City. Many features of the CO₂ 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 CO₂ from the ground and/or space are less sensitive than surface point measurements to the redistribution of emitted CO₂ by small-scale processes and thus may allow for more precise trend detection of emissions from urban regions.

We simulate nitrogen deposition over the US in 2006–2008 by using the GEOS-Chem global chemical transport model at 1/2°×2/3° horizontal resolution over North America and adjacent oceans. US emissions of NO_x and NH₃ in the model are 6.7 and 2.9 Tg N a⁻¹ respectively, including a 20% natural contribution for each. Ammonia emissions are a factor of 3 lower in winter than summer, providing a good match to US network observations of NH_x (≡NH₃ gas + ammonium aerosol) and ammonium wet deposition fluxes. Model comparisons to observed deposition fluxes and surface air concentrations of oxidized nitrogen species (NO_y) show overall good agreement but excessive wintertime HNO₃ production over the US Midwest and Northeast. This suggests a model overestimate N₂O₅ hydrolysis in aerosols, and a possible factor is inhibition by aerosol nitrate. Model results indicate a total nitrogen deposition flux of 6.5 Tg N a⁻¹ over the contiguous US, including 4.2 as NO_y and 2.3 as NH_x. Domestic anthropogenic, foreign anthropogenic, and natural sources contribute respectively 78%, 6%, and 16% of total nitrogen deposition over the contiguous US in the model. The domestic anthropogenic contribution generally exceeds 70% in the east and in populated areas of the west, and is typically 50–70% in remote areas of the west. Total nitrogen deposition in the model exceeds 10 kg N ha⁻¹ a⁻¹ over 35% of the contiguous US.

We have developed a mid-infrared continuous-wave quantum cascade laser direct-absorption spectrometer (QCLS) capable of high frequency (≥1 Hz) measurements of 12CH4 and 13CH4 isotopologues of methane (CH4) with in situ 1-s RMS ? precision of 1.5 ‰ and Allan-minimum precision of 0.2 ‰. We deployed this QCLS in a well-studied New Hampshire fen to compare measurements of CH4 isoflux by eddy covariance (EC) to Keeling regressions of data from automated flux chamber sampling. Mean CH4 fluxes of 6.5 ± 0.7 mg CH4 m-2 hr-1 over two days of EC sampling in July, 2009 were indistinguishable from mean autochamber CH4 fluxes (6.6 ± 0.8 mgCH4 m-2 hr-1) over the same period. Mean ? composition of emitted CH4 calculated using EC isoflux methods was -71 ± 8 ‰ (95% C.I.) while Keeling regressions of 332 chamber closing events over 8 days yielded a corresponding value of -64.5 ± 0.8 ‰. Ebullitive fluxes, representing ˜10% of total CH4 fluxes at this site, were on average 1.2 ‰ enriched in 13C compared to diffusive fluxes. CH4 isoflux time series have the potential to improve process-based understanding of methanogenesis, fully characterize source isotopic distributions, and serve as additional constraints for both regional and global CH4 modeling analysis.

Uncertainty in the future atmospheric burden of methane, a potent greenhouse gas1, 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 hydrates2, which are vulnerable to destabilization in a warming climate. Furthermore, methane is produced in the surface ocean3 and the surface waters of the Arctic Ocean are supersaturated with respect to methane4,5. 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.

Uncertainty in the future atmospheric burden of methane, a potent greenhouse gas1, 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 hydrates2, which are vulnerable to destabilization in a warming climate. Furthermore, methane is produced in the surface ocean3 and the surface waters of the Arctic Ocean are supersaturated with respect to methane4,5. 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.

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.

In the ‘Natural and anthropogenic climatic variation’ section of this Review, we incorrectly referred to the North Atlantic Oscillation as a contributor to the 2005 Amazonian droughts. We should instead have referred to the Atlantic Multidecadal Oscillation, which is an oceanic phenomenon related to anomalies in sea surface temperature in the tropical north Atlantic Ocean and can affect drought in the Amazon Basin. We thank L. Aragao for drawing this error to our attention. This has been corrected in the PDF and HTML versions online.

New observations of the vertically integrated CO₂ mixing ratio, ⟨CO₂⟩, from ground-based remote sensing show that variations in CO₂⟩ are primarily determined by large-scale flux patterns. They therefore provide fundamentally different information than observations made within the boundary layer, which reflect the combined influence of large-scale and local fluxes. Observations of both ⟨CO₂⟩ and CO₂ concentrations in the free troposphere show that large-scale spatial gradients induce synoptic-scale temporal variations in ⟨CO₂⟩ in the Northern Hemisphere midlatitudes through horizontal advection. Rather than obscure the signature of surface fluxes on atmospheric CO₂, these synoptic-scale variations provide useful information that can be used to reveal the meridional flux distribution. We estimate the meridional gradient in ⟨CO₂⟩ from covariations in ⟨CO₂⟩ and potential temperature, θ, a dynamical tracer, on synoptic timescales to evaluate surface flux estimates commonly used in carbon cycle models. We find that simulations using Carnegie Ames Stanford Approach (CASA) biospheric fluxes underestimate both the ⟨CO₂⟩ seasonal cycle amplitude throughout the Northern Hemisphere midlatitudes and the meridional gradient during the growing season. Simulations using CASA net ecosystem exchange (NEE) with increased and phase-shifted boreal fluxes better fit the observations. Our simulations suggest that climatological mean CASA fluxes underestimate boreal growing season NEE (between 45–65° N) by ~40%. We describe the implications for this large seasonal exchange on inference of the net Northern Hemisphere terrestrial carbon sink.

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.

The effects of climatic factors and vegetation type on evapotranspiration (E) and water use efficiency (WUE) were analyzed using tower-based eddy-covariance (EC) data for nine mature forest sites, two peatland sites and one grassland site across an east–west continental-scale transect in Canada during the period 2003–2006. The seasonal pattern of E was closely linked to growing-season length and rainfall distribution. Although annual precipitation (P) during the observation period was highly variable among sites (250−1450 mm), minimum annual E was not less than 200 mm and was limited to 400−500 mm where annual P exceeded 700 mm. Site-specific interannual variability in E could be explained by either changes in total P or variations in solar irradiance. A highly positive linear correlation was found between monthly mean values of E and net radiation (R_n) at the grassland site (AB-GRL), the two peatland sites (AB-WPL and ON-EPL), and only one of the forest sites (coastal Douglas-fir, BC-DF49) whereas a hysteretic relationship at the other forest sites indicated that E lagged behind the typical seasonal progression of R_n. Results of a cross-correlation analysis between daily (24-h) E and R_n revealed that site-specific lag times were between 10 and 40 days depending on the lag of vapour pressure deficit (D) behind R_n and the decoupling coefficient, Ω. There was significant seasonal variation in daytime mean dry-foliage Priestley–Taylor α with maxima occurring in the growing season at all sites except BC-DF49 where it was relatively constant (∼0.55) throughout all years. Annual means of daytime dry-foliage α mostly ranging between 0.5 and 0.7 implied stomatal limitation to transpiration. Increasing D significantly decreased canopy conductance (g_c) at the forest sites but had little effect at the peatland and grassland sites, while variation in soil water content caused only minor changes in g_c. At all sites, a strong linear correlation between monthly mean values of gross primary production (GPP) and E resulted in water use efficiency being relatively constant. While at most sites, WUE was in the range of 2.6–3.6 g C kg⁻¹ H₂O, the BC-DF49 site had the highest WUE of the twelve sites with values near 6.0 g C kg⁻¹ H₂O. Of the two peatland sites, AB-WPL, a western treed fen, had a significantly higher WUE (∼3.0 g C kg⁻¹ H₂O) than ON-EPL, an eastern ombrotrophic bog (∼1.8 g C kg⁻¹ H₂O), which was related to peatland productivity and plant functional type.

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 (NO_x = 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 NO_x. In accord with previous assessments, the 2010 airborne and ground-based data show an average decrease in NO_x of 46 ± 11% and 34 ± 4%, respectively, and an average increase in VOC/NO_xratio 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-NO_xoxidation 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 NO_x oxidation show 45 ± 13% and 42 ± 12% more extensive photochemical processing and, when compared with odd oxygen (O_x = 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.

Elevated mixing ratios of chlorofluorocarbons (CFC-11 and CFC-12), and sulfur hexafluoride (SF₆) have been observed at Lamont-Doherty Earth Observatory (LDEO), located approximately 25 km north of New York City (NYC). Emissions and transport of these gases are of interest because of their global warming potential, the role of CFCs in depletion of stratospheric ozone and information they provide on the transport of atmospheric pollutants. Comparison of trace gas time series with meteorological data indicates that both NYC and the region to the southwest (New Jersey and the Philadelphia –Washington DC area) are significant sources of CFCs, and confirms that NYC is an unusually large source of SF₆. From 1996 to 2005 the elevation of CFC-12 mixing ratio above that of the remote (well mixed) atmosphere has decreased on average by 5.2 ± 0.6 ppt y⁻¹, whereas that of CFC-11 has not changed significantly (0.0 ± 2.0 ppt y⁻¹). From 1998 to 2006, the elevation of SF₆ mixing ratios above that of the remote atmosphere declined by 0.4 ± 0.1 ppt y⁻¹. Time series of the same gases measured at Harvard Forest, 205 km northeast of LDEO, demonstrate transport of air masses with elevated levels of these gases from their source region to central Massachusetts. Emissions in the local area around LDEO were quantified through analysis of diurnal cycles. Local CFC-12 emissions decreased ca. 95% between 1996 and 2005 while CFC-11 emission decreased ca. 51% during the same period. Local SF₆ emissions decreased by 47% between 1998 and 2005.