[1] We interpret observations of trace-gases from three satellite platforms to provide topdown constraints on the production of NO by lightning. The space-based observations are tropospheric NO 2 columns from SCIAMACHY, tropospheric O 3 columns from OMI and MLS, and upper tropospheric HNO 3 from ACE-FTS. A global chemical transport model (GEOS-Chem) is used to identify locations and time periods in which lightning would be expected to dominate the trace gas observations. The satellite observations are sampled at those locations and time periods. All three observations exhibit a maximum in the tropical Atlantic region and a minimum in the tropical Pacific. This wave-1 pattern is driven by injection of lightning NO into the upper troposphere over the tropical continents, followed by photochemical production of NO 2 , HNO 3 , and O 3 during transport. Lightning produces a broad enhancement over the tropical Atlantic

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From the earliest observations of ozone in the lower atmosphere in the 19th century, both measurement methods and the portion of the globe observed have evolved and changed. These methods have different uncertainties and biases, and the data records differ with respect to coverage (space and time), information content, and representativeness. In this study, various ozone measurement methods and ozone datasets are reviewed and selected for inclusion in the historical record of background ozone levels, based on relationship of the measurement technique to the modern UV absorption standard, absence of interfering pollutants, representativeness of the well-mixed boundary layer and expert judgement of their credibility. There are significant uncertainties with the 19th and early 20th-century measurements related to interference of other gases. Spectroscopic methods applied before 1960 have likely underestimated ozone by as much as 11% at the surface and by about 24% in the free troposphere, due to the use of differing ozone absorption coefficients.There is no unambiguous evidence in the measurement record back to 1896 that typical mid-latitude background surface ozone values were below about 20 nmol mol -1 , but there is robust evidence for increases in the temperate and polar regions of the northern hemisphere of 30-70%, with large uncertainty, between the period of historic observations, 1896-1975, and the modern period (1990-2014). Independent historical observations from balloons and aircraft indicate similar changes in the free troposphere. Changes in the southern hemisphere are much less. Regional representativeness of the available observations remains a potential source of large errors, which are difficult to quantify.The great majority of validation and intercomparison studies of free tropospheric ozone measurement methods use ECC ozonesondes as reference. Compared to UV-absorption measurements they show a modest (~1-5% ±5%) high bias in the troposphere, but no evidence of a change with time. Umkehr, lidar, and FTIR methods all show modest low biases relative to ECCs, and so, using ECC sondes as a transfer standard, all appear to agree to within one standard deviation with the modern UV-absorption standard. Other sonde types show an increase of 5-20% in sensitivity to tropospheric ozone from 1970-1995. Biases and standard deviations of satellite retrieval comparisons are often 2-3 times larger than those of other free tropospheric measurements. The lack of information on temporal changes of bias for satellite measurements of tropospheric ozone is an area of concern for long-term trend studies.

Increases in ultraviolet fluxes (300 nm to 340 nm) reaching the ground between 1979 and 1992 are estimated using measured stratospheric ozone amounts and reflectivity data from Nimbus‐7/TOMS (Total Ozone Mapping Spectrometer). The UV‐increases are estimated from an ozone data set obtained using a new algorithm incorporating improved in‐flight instrument calibration. The 380 nm radiance data are used to show that there were no changes in ultraviolet atmospheric albedo due to clouds and aerosols from 1979 to 1992 within the 1% uncertainty of the measurements. Linear least squares fits to the monthly and annual increases in UV exposure since 1979 are given for 3 wavelengths (300 nm, 310 nm, and 320 nm) that are strongly, moderately, and weakly absorbed by ozone. The estimated linear changes for the 3 wavelengths become significant (2 standard deviations) poleward of about 40° latitude. In the 45°±5° latitude band, the slope of linear fits to the annual zonally averaged changes for these wavelengths are about 13%, 3%, and 1% per decade in the southern hemisphere, and 10%, 3%, and 1% per decade in the northern hemisphere. Similarly derived values are estimated for DNA, plant, and erythema action spectra. Monthly values of exposure changes are larger towards higher latitudes and during the spring and winter months (e.g., 8.6%, 9.8%, and 5.1% per decade during April at 45°N). Erythemal UV‐increases obtained from TOMS data disagree with previously determined ground based UV‐decreases from an average of 8 U.S. Robertson‐Berger sites.

[1] The El Niño-Southern Oscillation (ENSO) is the dominant mode of inter-annual variability in the tropical ocean and troposphere. Its impact on tropospheric circulation causes significant changes to the distribution of ozone. Here we derive the lower tropospheric to lower stratospheric ozone response to ENSO from observations by the Tropospheric Emission Spectrometer (TES) and the Microwave Limb Sounder (MLS) instruments, both on the Aura satellite, and compare to the simulated response from the Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM). Measurement ozone sensitivity is derived using multiple linear regression to include variations from ENSO as well as from the first two empirical orthogonal functions of the quasi-biennial oscillation. Both measurements and simulation show features such as the negative ozone sensitivity to ENSO over the tropospheric tropical Pacific and positive ozone sensitivity over Indonesia and the Indian Ocean region. Ozone sensitivity to ENSO is generally positive over the midlatitude lower stratosphere, with greater sensitivity in the Northern Hemisphere. GEOSCCM reproduces both the overall pattern and magnitude of the ozone response to ENSO obtained from observations. We demonstrate the combined use of ozone measurements from MLS and TES to quantify the lower atmospheric ozone response to ENSO and suggest its possible usefulness in evaluating chemistry-climate models.

We estimate the tropospheric column ozone using a forward trajectory model to increase the horizontal resolution of the Aura Microwave Limb Sounder (MLS) derived stratospheric column ozone. Subtracting the MLS stratospheric column from Ozone Monitoring Instrument total column measurements gives the trajectory enhanced tropospheric ozone residual (TTOR). Because of different tropopause definitions, we validate the basic residual technique by computing the 200‐hPa‐to‐surface column and comparing it to the same product from ozonesondes and Tropospheric Emission Spectrometer measurements. Comparisons show good agreement in the tropics and reasonable agreement at middle latitudes, but there is a persistent low bias in the TTOR that may be due to a slight high bias in MLS stratospheric column. With the improved stratospheric column resolution, we note a strong correlation of extratropical tropospheric ozone column anomalies with probable troposphere‐stratosphere exchange events or folds. The folds can be identified by their colocation with strong horizontal tropopause gradients. TTOR anomalies due to folds may be mistaken for pollution events since folds often occur in the Atlantic and Pacific pollution corridors. We also compare the 200‐hPa‐to‐surface column with Global Modeling Initiative chemical model estimates of the same quantity. While the tropical comparisons are good, we note that chemical model variations in 200‐hPa‐to‐surface column at middle latitudes are much smaller than seen in the TTOR.

Tropospheric ozone is an important greenhouse gas, is detrimental to human health and crop and ecosystem productivity, and controls the oxidizing capacity of the troposphere. Because of its high spatial and temporal variability and limited observations, quantifying net tropospheric ozone changes across the Northern Hemisphere on time scales of two decades had not been possible. Here, we show, using newly available observations from an extensive commercial aircraft monitoring network, that tropospheric ozone has increased above 11 regions of the Northern Hemisphere since the mid-1990s, consistent with the OMI/MLS satellite product. The net result of shifting anthropogenic ozone precursor emissions has led to an increase of ozone and its radiative forcing above all 11 study regions of the Northern Hemisphere, despite NOx emission reductions at midlatitudes.