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Methane (CH4) is a powerful greenhouse gas that is produced by a diverse set of natural and anthropogenic emission sources. Biogenic methane sources generally involve anaerobic decay processes such as those occurring in wetlands, melting permafrost, or the digestion of organic matter in the guts of ruminant animals. Thermogenic CH4 sources originate from the breakdown of organic material at high temperatures and pressure within the Earth's crust, a process which also produces more complex trace hydrocarbons such as ethane (C2H6). Here, we present the development and deployment of an uncrewed aerial system (UAS) that employs a fast (1 Hz) and sensitive (1–0.5 ppb s−1) CH4 and C2H6 sensor and ultrasonic anemometer. The UAS platform is a vertical-takeoff, hexarotor drone (DJI Matrice 600 Pro, M600P) capable of vertical profiling to 120 m altitude and plume sampling across scales up to 1 km. Simultaneous measurements of CH4 and C2H6 concentrations, vector winds, and positional data allow for source classification (biogenic versus thermogenic), differentiation, and emission rates without the need for modeling or a priori assumptions about winds, vertical mixing, or other environmental conditions. The system has been used for direct quantification of methane point sources, such as orphan wells, and distributed emitters, such as landfills and wastewater treatment facilities. With detectable source rates as low as 0.04 and up to ∼ 1500 kg h−1, this UAS offers a direct and repeatable method of horizontal and vertical profiling of emission plumes at scales that are complementary to regional aerial surveys and localized ground-based monitoring.

Precipitable water vapor (PWV) is the vertically integrated amount of water vapor in the atmosphere, and it is a valuable predictor for weather forecasting. Currently, the use of sophisticated instrumentation can limit the number of PWV measurement sites, which affects the accuracy of forecast models in regards to storm formation, strength, and the potential for precipitation. We have analyzed relationships between PWV and zenith sky temperature measurements for the dry climate zone found in the North American Desert Southwest, specifically over Socorro, New Mexico (34∘ N, 107∘ W). Daily measurements of the ground and zenith sky temperatures have been made at Socorro for two complete annual cycles using low-cost infrared thermal sensors. Radiosonde measurements of PWV from National Weather Service stations located in nearby Albuquerque and Santa Teresa, New Mexico, are input into our dataset and analyzed via a newly developed computational tool. Our results show that an exponential relationship between PWV and zenith sky temperature holds for the Desert Southwest, but with parameters that are different than those obtained previously over the more moist climate zone of the North American Gulf Coast. Model simulations can accurately reproduce the observed relationship between PWV and temperature, and the results suggest that half of the signal in temperature is directly related to changes in opacity due to changes in PWV, while the other half is due to changes in air temperature that usually accompany changes in PWV.

We quantify ozone variability in the upper troposphere and lower stratosphere (UTLS) by investigating lamination features in balloon measurements of ozone mixing ratio and potential temperature. Laminae are defined as stratified variations in ozone that meet or exceed a 10 % threshold for deviations from a basic state vertical profile of ozone. The basic state profiles are derived for each sounding using smoothing methods applied within a vertical coordinate system relative to the World Meteorological Organization (WMO) tropopause. We present results of this analysis for the 25-year record of ozonesonde measurements from Boulder, Colorado. The mean number of ozone laminae identified per sounding is about 9±2 (1σ). The root-mean-square relative amplitude is 20 %, and laminae with much larger amplitudes (>40 %) are seen in ∼ 2 % of the profiles. The vertical scale of detected ozone laminae typically ranges between 0.5 and 1.2 km. The lamina occurrence frequency varies significantly with altitude and is largest within ∼2 km of the tropopause. Overall, ozone laminae identified in our analysis account for more than one-third of the total intra-seasonal variability in ozone. A correlation technique between ozone and potential temperature is used to classify the subset of ozone laminae that are associated with gravity wave (GW) phenomena, which accounts for 28 % of all laminar ozone features. The remaining 72 % of laminae arise from non-gravity wave (NGW) phenomena. There are differences in both the vertical distribution and seasonality of GW versus NGW ozone laminae that are linked to the contrast in main generating mechanisms for each laminae type.

We present a comprehensive comparison of polar processing diagnostics derived from the National Aeronautics and Space Administration (NASA) Modern Era Retrospective-analysis for Research and Applications (MERRA) and the European Centre for Medium-Range Weather Forecasts (ECMWF) Interim Reanalysis (ERA-Interim). We use diagnostics that focus on meteorological conditions related to stratospheric chemical ozone loss based on temperatures, polar vortex dynamics, and air parcel trajectories to evaluate the effects these reanalyses might have on polar processing studies. Our results show that the agreement between MERRA and ERA-Interim changes significantly over the 34 years from 1979 to 2013 in both hemispheres and in many cases improves. By comparing our diagnostics during five time periods when an increasing number of higher-quality observations were brought into these reanalyses, we show how changes in the data assimilation systems (DAS) of MERRA and ERA-Interim affected their meteorological data. Many of our stratospheric temperature diagnostics show a convergence toward significantly better agreement, in both hemispheres, after 2001 when Aqua and GOES (Geostationary Operational Environmental Satellite) radiances were introduced into the DAS. Other diagnostics, such as the winter mean volume of air with temperatures below polar stratospheric cloud formation thresholds (VPSC) and some diagnostics of polar vortex size and strength, do not show improved agreement between the two reanalyses in recent years when data inputs into the DAS were more comprehensive. The polar processing diagnostics calculated from MERRA and ERA-Interim agree much better than those calculated from earlier reanalysis data sets. We still, however, see fairly large differences in many of the diagnostics in years prior to 2002, raising the possibility that the choice of one reanalysis over another could significantly influence the results of polar processing studies. After 2002, we see overall good agreement among the diagnostics, which demonstrates that the ERA-Interim and MERRA reanalyses are equally appropriate choices for polar processing studies of recent Arctic and Antarctic winters.

The lifetimes of CFC-11 and CFC-12 have been evaluated using global observations of their stratospheric distributions from satellite-based instruments over the time period from 1992 to 2010. The chlorofluorocarbon (CFC) datasets are from the Cryogen Limb Array Etalon Spectrometer (CLAES), the Cryogenic Infrared Spectrometers and Telescopes for the Atmosphere (CRISTA-1 and CRISTA-2), the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), and the Atmospheric Chemistry Experiment (ACE). Stratospheric loss rates were calculated using an ultraviolet radiative transfer code with updated cross section and solar irradiance data. Mean steady-state lifetimes based on these observations are 44.7 (36–58) yr for CFC-11 and 106.6 (90–130) yr for CFC-12, which are in good agreement with the most recent WMO ozone assessment. There are two major sources of error in calculating lifetimes using this method. The first important error arises from uncertainties in tropical stratospheric observations, particularly for CFC-11. Another large contribution to the error is due to uncertainties in the penetration of solar ultraviolet radiation at wavelengths between 185 and 220 nm, primarily in the tropical stratosphere between 20 and 35 km altitude.

Diurnal variations in hydroxyl (OH) in the stratosphere and mesosphere are analyzed using measurements from the Aura Microwave Limb Sounder (MLS). The primary driver for OH diurnal variations is the ultraviolet actinic flux that initiates the photochemical production of reactive hydrogen species. The magnitude of this flux is governed largely by changes in solar zenith angle (SZA) throughout the day, and OH diurnal variations are well approximated by an exponential function of the secant of SZA. Measured OH concentrations are fit to a function of the form exp[−βsec(SZA)], where the parameter β is a function of altitude. We examine the magnitude of β and show that it is related to the optical depths of ultraviolet absorption by ozone and molecular oxygen. Values of β from SLIMCAT model simulations show the same vertical structure as those from MLS and the average level of agreement between model and measurements is 6%. The vertical profile of β from MLS can be represented by a simple analytic formulation involving the ozone and water vapor photodissociation rates. This formulation is used to infer the altitude dependence of the primary production mechanisms for OH: the reaction of excited-state atomic oxygen with water vapor versus the direct photodissociation of water vapor.

An unusually strong and prolonged stratospheric sudden warming (SSW) in January 2006 was the first major SSW for which globally distributed long-lived trace gas data are available covering the upper troposphere through the lower mesosphere. We use Aura Microwave Limb Sounder (MLS), Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) data, the SLIMCAT Chemistry Transport Model (CTM), and assimilated meteorological analyses to provide a comprehensive picture of transport during this event. The upper tropospheric ridge that triggered the SSW was associated with an elevated tropopause and layering in trace gas profiles in conjunction with stratospheric and tropospheric intrusions. Anomalous poleward transport (with corresponding quasi-isentropic troposphere-to-stratosphere exchange at the lowest levels studied) in the region over the ridge extended well into the lower stratosphere. In the middle and upper stratosphere, the breakdown of the polar vortex transport barrier was seen in a signature of rapid, widespread mixing in trace gases, including CO, H2O, CH4 and N2O. The vortex broke down slightly later and more slowly in the lower than in the middle stratosphere. In the middle and lower stratosphere, small remnants with trace gas values characteristic of the pre-SSW vortex lingered through the weak and slow recovery of the vortex. The upper stratospheric vortex quickly reformed, and, as enhanced diabatic descent set in, CO descended into this strong vortex, echoing the fall vortex development. Trace gas evolution in the SLIMCAT CTM agrees well with that in the satellite trace gas data from the upper troposphere through the middle stratosphere. In the upper stratosphere and lower mesosphere, the SLIMCAT simulation does not capture the strong descent of mesospheric CO and H2O values into the reformed vortex; this poor CTM performance in the upper stratosphere and lower mesosphere results primarily from biases in the diabatic descent in assimilated analyses.

Airborne in situ observations of molecules with a wide range of lifetimes (methane, nitrous oxide, reactive nitrogen, ozone, chlorinated halocarbons, and halon-1211), used in a tropical tracer model, show that mid-latitude air is entrained into the tropical lower stratosphere within about 13.5 months; transport is faster in the reverse direction. Because exchange with the tropics is slower than global photochemical models generally assume, ozone at mid-latitudes appears to be more sensitive to elevated levels of industrial chlorine than is currently predicted. Nevertheless, about 45 percent of air in the tropical ascent region at 21 kilometers is of mid-latitude origin, implying that emissions from supersonic aircraft could reach the middle stratosphere.