Tropospheric Observations Research Articles

Simultaneous observation on the post-sunset occurrence of travelling ionospheric disturbance alongside ionospheric irregularities over the East Africa low latitude region

Using a data set from the network of more than 30 GNSS receivers within the East Africa sector; a study on the transient wave-like total electron content (TEC) modulation alongside the post-sunset irregularities has been presented. The study period is during the years 2019 to 2021 and the year 2014. The TEC modulation was detected from the quasi-periodic variation of detrended TEC and occurs nearly on a day-to-day basis at post-sunset hours just like the post-sunset ionospheric irregularities. The wavelike TEC modulation is likely due to gravity waves generated at the lower atmosphere that propagates into the F region and is quantified as travelling ionospheric disturbance (TIDs). The dominant quasi-periods of these TIDs are between 10 and 50 min. The TIDS, just like the irregularities, were confined in the latitudinal range of 0–9.4oS magnetic latitudes within the East Africa sector. A statistical analysis of simultaneous observations of the post-sunset TIDs shows that the day-to-day variations are identical to that of the ionospheric irregularity occurrence rate. The TIDs exhibit a relatively strong wave oscillation with multiple wavelengths preceding/accompanying the occurrence of irregularities. The simultaneous observation of TIDs and irregularities shows that the wavelike seeding perturbation associated with gravity waves from the lower atmosphere combined with strong seeding forces (unknown source) could facilitate the observed growth rate of the Rayleigh Taylor Instability mechanism that is associated with the formation of ionospheric irregularities. Additional experiments and tropospheric observation may be required to ascertain the source of gravity waves that are linked to TEC perturbation during nighttime hours.

Multi‐Layer Evolution of Acoustic‐Gravity Waves and Ionospheric Disturbances Over the United States After the 2022 Hunga Tonga Volcano Eruption

AbstractThe Hunga‐Tonga Hunga‐Ha'apai volcano underwent a series of large‐magnitude eruptions that generated broad spectra of mechanical waves in the atmosphere. We investigate the spatial and temporal evolutions of fluctuations driven by atmospheric acoustic‐gravity waves (AGWs) and, in particular, the Lamb wave modes in high spatial resolution data sets measured over the Continental United States (CONUS), complemented with data over the Americas and the Pacific. Along with >800 barometer sites, tropospheric observations, and Total Electron Content data from >3,000 receivers, we report detections of volcano‐induced AGWs in mesopause and ionosphere‐thermosphere airglow imagery and Fabry‐Perot interferometry. We also report unique AGW signatures in the ionospheric D‐region, measured using Long‐Range Navigation pulsed low‐frequency transmitter signals. Although we observed fluctuations over a wide range of periods and speeds, we identify Lamb wave modes exhibiting 295–345 m s−1 phase front velocities with correlated spatial variability of their amplitudes from the Earth's surface to the ionosphere. Results suggest that the Lamb wave modes, tracked by our ray‐tracing modeling results, were accompanied by deep fluctuation fields coupled throughout the atmosphere, and were all largely consistent in arrival times with the sequence of eruptions over 8 hr. The ray results also highlight the importance of winds in reducing wave amplitudes at CONUS midlatitudes. The ability to identify and interpret Lamb wave modes and accompanying fluctuations on the basis of arrival times and speeds, despite complexity in their spectra and modulations by the inhomogeneous atmosphere, suggests opportunities for analysis and modeling to understand their signals to constrain features of hazardous events.

Problems with and Improvement of HCHO/NO2 for Diagnosing Ozone Sensitivity—A Case in Beijing

Rfn (formaldehyde/nitrogen dioxide) is a common indicator based on satellite observations used to classify ozone formation sensitivity. However, it may underestimate anthropogenic volatile organic compounds (VOCs) in heavily polluted cities when only formaldehyde (HCHO) is used in Rfn to measure VOCs, since it is mainly derived from natural sources worldwide. In this study, we used multiaxis differential optical absorption spectroscopy to acquire tropospheric observations of nitrogen dioxide (NO2), HCHO and glyoxal (CHOCHO) in Beijing from 1 April 2019 to 31 March 2020. Combined with VOCs detected simultaneously by gas chromatography—mass spectrometry and proton transfer reaction–time-of-flight/mass spectrometry near the ground, we evaluated the representativeness of HCHO column densities on total VOCs (TVOC) in equivalent propylene concentrations, which is called reactivity. The results showed that there were significant seasonal differences in the response of HCHO to TVOC reactivity, with fitting slopes of 2.3 (spring), 2.6 (summer), 2.9 (autumn) and 1.0 (winter) in the four seasons, respectively. Since CHOCHO can be used to partly characterize the contribution of anthropogenic VOC emissions and demonstrated a better response to TVOC reactivity in winter, with fitting slopes of 0.2 (spring), 0.2 (summer), 0.2 (autumn) and 0.5 (winter) in the four seasons, respectively, we introduced CHOCHO to construct a new indicator (HCHO + 6 × CHOCHO). The fitting slopes of the four seasons were more similar, being 3.2 (spring), 3.6 (summer), 4.0 (autumn) and 4.0 (winter). The ratio of the new indicator to NO2, Rmn ((HCHO + 6 × CHOCHO)/NO2), was used to reclassify the ozone formation sensitivity of urban areas in North China, revealing that it is a transition regime before 1300 LST (LST = UST + 8) and an NOx-limited regime afterwards. Rmn improved the sensitivity from the VOC-limited regime to the NOx-limited regime, enhancing the sensitivity of NOx and providing new robust support for ozone pollution prevention and control.

Observations of Diurnal Variability under the Cirrus Canopy of Typhoon Kong-rey (2018)

AbstractA growing body of work has documented the existence of diurnal oscillations in the tropical cyclone outflow layer. These diurnal pulses have been examined primarily using satellites or numerical models, and detailed full tropospheric observations or case study analyses of diurnal pulses are lacking. Questions remain on the vertical extent of diurnal pulses and whether diurnal pulses are coupled to convective bands or constrained to the outflow layer. During the Propagation of Intraseasonal Tropical Oscillations (PISTON) field campaign, diurnal oscillations in the upper-level clouds were observed during Typhoon Kong-rey’s (2018) rapid intensification. Over a 3.5 day period where a broad distribution of cold upper-level clouds was overhead, detailed observations of Typhoon Kong-rey’s rainbands show that convection had reduced echo tops but enhanced reflectivity and differential reflectivity aloft compared to other observations during PISTON. Shortwave heating in the upper-levels increased the stability profile in an overall favorable thermodynamic environment for convection during the day, which could help to explain the diurnal differences in convective structure. Under the cirrus canopy, nocturnal convection was deeper and daytime convection shallower in contrast to the rest of the PISTON dataset. Diurnal oscillations in the brightness temperatures were found to be coupled to radially outward propagating convective rainbands that were preceded ~6 hours by outflow jets. The cooling pulses occurred earlier than found in previous studies. The pulses were asymmetric spatially which is likely due to a combination of the vertical wind shear and storm intensity.

Air quality in the Galapagos Islands: A baseline view from remote sensing and in situ measurements

AbstractA characterization of ambient air levels of PM2.5, O3, SO2, NO2 and CO in the Galapagos Islands of Ecuador is presented from in situ and remote sensing observations. PM2.5 was derived from aerosol optical depth (AOD; AERONET) measured at the Universidad San Francisco de Quito, Galapagos Campus (2017–2019). Boundary layer (BL) ozone was obtained from Southern Hemisphere Additional Ozonesondes (SHADOZ) profiles (1998–2016). Background SO2 and pollution events during volcanic eruptions (2005–2018) were estimated from Ozone Monitoring Instrument (OMI) total column measurements through a well‐mixed volume approach. Similarly, ambient NO2 was estimated from OMI data (2012–2019). CO was obtained from Measurement Of Pollution In The Troposphere (MOPITT) observations (2012–2017). The study was complemented using Modern‐Era Retrospective Analysis for Research and Applications (MERRA‐2) reanalysis products and backward trajectory model runs. From the results, baseline levels of the analysed species (PM2.5 = 3.8 μg·m−3, O3 = 17 ppbv, SO2 = 3.6 ppbv, CO = 80 ppbv, NO2 in populated islands = 23 pptv as one year averages) are comparable with other pristine regions, but some factors can cause increased concentrations. First, high tourism seasons (February–April and July–September) raise background PM2.5, NO2 and CO. Furthermore, signals in July–September can be augmented by transport from biomass‐burning regions in the Amazon. This latter factor episodically causes ozone to increase up to 45–75 ppbv (1 hr mean). Lastly, volcanic eruptions raise SO2 up to almost 700 ppbv (24 hr mean) and increase PM2.5 to 29.5 μg·m−3 (1 hr mean). The present study provides for the first time baseline levels of air contaminants in the Galapagos, and identifies specific sources whose effect in time is necessary to monitor given global conditions of vulnerable environmental quality.

A Factor and Trends Analysis of Multidecadal Lower Tropospheric Observations of Arctic Aerosol Composition, Black Carbon, Ozone, and Mercury at Alert, Canada

AbstractObservations from 1980 to 2013 of 20 aerosol constituents, ozone and mercury at Alert, Canada (82.50°N, 62.35°W), were analyzed for trends and dominant factors of the Arctic haze during winter and spring. Trends reflect changing emissions in Eurasia, the main source region for surface pollution in the high Arctic. SO42−, H+, NH4+, K+, Cu, Ni, Pb, Zn, nonsoil V, nonsoil Mn, and equivalent black carbon decreased between 23% and 80% as emissions declined rapidly in northern Eurasia during the early 1990s. NO3− increased by 20% as aerosol acidity declined. Metals were linked to emissions from smelting and fossil fuel combustion. In winter, ozone increased by 5% over 23 years, consistent with other observations and global modeling. Twelve PMF factors emerged for the dark period (November to February) and 13 for the light period (March to May). Eleven PMF factors are common to both dark and light, a twelfth factor was associated with sulfate in the dark and nitrate in the light, and the thirteenth (light period) was related to ozone and gaseous mercury depletion near Alert. IODINE and NITRATE factors, important for Arctic chemistry, changed with sunlight. In the light, 50% of all NO3− was on the NITRATE factor, while in the dark, most was associated with MODIFIED SEA SALT and equivalent black carbon. In the dark (light), 90% (28%) of iodine were found on the factor IODINE and 58% associated with SEA‐SALT and MODIFIED SEA‐SALT. These results help in understanding the role of atmospheric chemistry in weather and climate processes.

Assimilation of GNSS tomography products into the Weather Research and Forecasting model using radio occultation data assimilation operator

Abstract. From Global Navigation Satellite Systems (GNSS) signals, accurate and high-frequency atmospheric parameters can be determined in all-weather conditions. GNSS tomography is a technique that takes advantage of these parameters, especially of slant troposphere observations between GNSS receivers and satellites, traces these signals through a 3-D grid of voxels, and estimates by an inversion process the refractivity of the water vapour content within each voxel. In the last years, the GNSS tomography development focused on numerical methods to stabilize the solution, which has been achieved to a great extent. Currently, we are facing new challenges and possibilities in the application of GNSS tomography in numerical weather forecasting, the main research objective of this paper. In the first instance, refractivity fields were estimated using two different GNSS tomography models (TUW, WUELS), which cover the area of central Europe during the period of 29 May–14 June 2013, when heavy-precipitation events were observed. For both models, slant wet delays (SWDs) were calculated based on estimates of zenith total delay (ZTD) and horizontal gradients, provided for 88 GNSS sites by Geodetic Observatory Pecny (GOP). In total, three sets of SWD observations were tested (set0 without compensation for hydrostatic anisotropic effects, set1 with compensation of this effect, set2 cleaned by wet delays outside the inner voxel model), in order to assess the impact of different factors on the tomographic solution. The GNSS tomography outputs have been assimilated into the nested (12 and 36 km horizontal resolution) Weather Research and Forecasting (WRF) model, using its three-dimensional variational data assimilation (WRFDA 3D-Var) system, in particular, its radio occultation observation operator (GPSREF). As only total refractivity is assimilated in GPSREF, it was calculated as the sum of the hydrostatic part derived from the ALADIN-CZ model and the wet part from the GNSS tomography. We compared the results of the GNSS tomography data assimilation to the radiosonde (RS) observations. The validation shows the improvement in the weather forecasting of relative humidity (bias, standard deviation) and temperature (standard deviation) during heavy-precipitation events. Future improvements to the assimilation method are also discussed.

Tropospheric observations of CFC-114 and CFC-114a with a focus on long-term trends and emissions

Abstract. Chlorofluorocarbons (CFCs) are ozone-depleting substances as well as strong greenhouse gases, and the control of their production and use under the Montreal Protocol has had demonstrable benefits to both mitigation of increasing surface UV radiation and climate forcing. A global ban on consumption came into force in 2010, but there is evidence of continuing emissions of certain CFCs from a range of sources. One compound has received little attention in the literature, namely CFC-114 (C2Cl2F4). Of particular interest here is the differentiation between CFC-114 (CClF2CClF2) and its asymmetric isomeric form CFC-114a (CF3CCl2F) as atmospheric long-term measurements in the peer-reviewed literature to date have been assumed to represent the sum of both isomers with a time-invariant isomeric speciation. Here we report the first long-term measurements of the two isomeric forms separately, and find that they have different origins and trends in the atmosphere. Air samples collected at Cape Grim (41° S), Australia, during atmospheric background conditions since 1978, combined with samples collected from deep polar snow (firn) enable us to obtain a near-complete record of both gases since their initial production and release in the 1940s. Both isomers were present in the unpolluted atmosphere in comparably small amounts before 1960. The mixing ratio of CFC-114 doubled from 7.9 to 14.8 parts per trillion (ppt) between the start of the Cape Grim record in 1978 and the end of our record in 2014, while over the same time CFC-114a trebled from 0.35 to 1.03 ppt. Mixing ratios of both isomers are slowly decreasing by the end of this period. This is consistent with measurements of recent aircraft-based samples showing no significant interhemispheric mixing ratio gradient. We also find that the fraction of CFC-114a mixing ratio relative to that of CFC-114 increased from 4.2 to 6.9 % over the 37-year period. This contradicts the current tacit assumption used in international climate change and ozone depletion assessments that both isomers have been largely co-emitted and that their atmospheric concentration ratio has remained approximately constant in time. Complementary observations of air collected in Taiwan indicate a persisting source of CFC-114a in South East Asia which may have been contributing to the changing balance between the two isomers. In addition we present top-down global annual emission estimates of CFC-114 and CFC-114a derived from these measurements using a two-dimensional atmospheric chemistry-transport model. In general, the emissions for both compounds grew steadily during the 1980s, followed by a substantial reduction from the late 1980s onwards, which is consistent with the reduction of emission in response to the Montreal Protocol, and broadly consistent with bottom-up estimates derived by industry. However, we find that small but significant emissions of both isomers remain in 2014. Moreover the inferred changes to the ratio of emissions of the two isomers since the 1990s also indicate that the sources of the two gases are, in part, independent.

BAECC: A Field Campaign to Elucidate the Impact of Biogenic Aerosols on Clouds and Climate

Abstract During Biogenic Aerosols—Effects on Clouds and Climate (BAECC), the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) Program deployed the Second ARM Mobile Facility (AMF2) to Hyytiälä, Finland, for an 8-month intensive measurement campaign from February to September 2014. The primary research goal is to understand the role of biogenic aerosols in cloud formation. Hyytiälä is host to the Station for Measuring Ecosystem–Atmosphere Relations II (SMEAR II), one of the world’s most comprehensive surface in situ observation sites in a boreal forest environment. The station has been measuring atmospheric aerosols, biogenic emissions, and an extensive suite of parameters relevant to atmosphere–biosphere interactions continuously since 1996. Combining vertical profiles from AMF2 with surface-based in situ SMEAR II observations allows the processes at the surface to be directly related to processes occurring throughout the entire tropospheric column. Together with the inclusion of extensive surface precipitation measurements and intensive observation periods involving aircraft flights and novel radiosonde launches, the complementary observations provide a unique opportunity for investigating aerosol–cloud interactions and cloud-to-precipitation processes in a boreal environment. The BAECC dataset provides opportunities for evaluating and improving models of aerosol sources and transport, cloud microphysical processes, and boundary layer structures. In addition, numerical models are being used to bridge the gap between surface-based and tropospheric observations.

Sulfur Isotopic Fractionation of Carbonyl Sulfide during Degradation by Soil Bacteria.

We performed laboratory incubation experiments on the degradation of gaseous phase carbonyl sulfide (OCS) by soil bacteria to determine its sulfur isotopic fractionation constants ((34)ε). Incubation experiments were conducted using strains belonging to the genera Mycobacterium, Williamsia, and Cupriavidus isolated from natural soil environments. The (34)ε values determined were -3.67 ± 0.33‰, -3.99 ± 0.19‰, -3.57 ± 0.22‰, and -3.56 ± 0.23‰ for Mycobacterium spp. strains THI401, THI402, THI404, and THI405; -3.74 ± 0.29‰ for Williamsia sp. strain THI410; and -2.09 ± 0.07‰ and -2.38 ± 0.35‰ for Cupriavidus spp. strains THI414 and THI415. Although OCS degradation rates divided by cell numbers (cell-specific activity) were different among strains of the same genus, the (34)ε values for same genus showed no significant differences. Even though the numbers of bacterial species examined were limited, our results suggest that (34)ε values for OCS bacterial degradation depend not on cell-specific activities, but on genus-level biological differences, suggesting that (34)ε values are dependent on enzymatic and/or membrane properties. Taking our (34)ε values as representative for bacterial OCS degradation, the expected atmospheric changes in δ(34)S values of OCS range from 0.5‰ to 0.9‰, based on previously reported decreases in OCS concentrations at Mt. Fuji, Japan. Consequently, tropospheric observation of δ(34)S values for OCS coupled with (34)ε values for OCS bacterial degradation can potentially be used to investigate soil as an OCS sink.

Disturbances of the upper atmosphere and ionosphere caused by acoustic-gravity wave sources in the lower atmosphere

The results of observations of acoustic-gravity waves in the troposphere and the ionosphere at middle latitudes during periods of passage of the solar terminator are presented. Tropospheric observations were performed using a lidar. The frequency characteristics of variations of the tropospheric parameters are determined based on observations of the intensity of the scattered lidar signal. The characteristics of variations of the total electron content (TEC) in the atmosphere are determined from data collected by GPS navigation satellites. An analysis of the observational data showed that the spectrum of variations of the atmospheric and ionospheric parameters is indicative of acoustic-gravity waves (AGW) propagating from the lower atmosphere. Modeling studies of the vertical propagation of AGW from the Earth’s surface showed that such waves quickly (within ~15 min) reach altitudes of the upper atmosphere (~300 km). The refraction and dissipation of waves in the upper atmosphere produces perturbations of the background state of the atmosphere and gives rise to the waveguide propagation of infrasonic wave components. The observed manifestations of TEC disturbances caused by AGW propagating from the lower atmosphere can be explained by the diurnal variation of the altitude of the ionosphere and the waveguide propagation of infrasonic waves.

Consistency of tropospheric ozone observations made by different platforms and techniques in the global databases

A large quantity of tropospheric ozone observations are conducted all over the world using different platforms and techniques for different purposes and goals. These observations are commonly used to derive seasonal cycles, interannual variations and long-term trends of ozone in the troposphere. In addition, they are used for comparison with three-dimensional chemistry-transport models to evaluate their performance and hence to test our current understanding of the tropospheric ozone variability. It is still challenging to provide robust tropospheric ozone trends throughout the world because of the great variability of ozone, its complex photochemical reactions, the rarity of long-term records, the diversity of measurement techniques and platforms, and the issues with data quality. In this work, we evaluated, with emphasis on the lower troposphere, the consistency of tropospheric ozone observations made by means of multiple platforms, including surface sites, sondes and regular aircraft, that are publicly available in the global databases, but excluding space-borne platforms. Concomitant observations were examined on an hourly basis (except for ±3 hours for sonde versus aircraft) for pairs of locations at less than 100-km distance. Generally, we found good agreement between sonde and surface observations. We also found that there was no need to apply any correction factor to ozonesonde observations except for Brewer–Mast sondes at Hohenpeissenberg. Because of a larger distance between the site pairs, the correlations found between the aircraft and surface measurements were poorer than those between sonde and surface measurements. However, a relatively simple wind segregation improved the agreement between the aircraft versus surface measurements. We found also that due to diurnal cycles, the sonde launching at a fixed local time led to positive or negative biases against the surface observations, suggesting that great attention should be paid to local time and diurnal variations when using ozonesonde in the analysis of seasonal cycles, long-term trends and interannual variations of lower tropospheric ozone. The comparison of surface data at Mt. Happo to regular aircraft data over Tokyo/Narita showed a relatively reasonable agreement, ensuring regionally representative ozone data sets in this region for trend analysis.

The first tropospheric wind profiler observations of a severe typhoon over a coastal area in South China

The first tropospheric wind profiler observations of a severe typhoon over a coastal area in South China

Advances in <inline-formula> <tex-math notation="TeX"> $\hbox{CO}_{2}$</tex-math></inline-formula> Observations From AIRS and ACOS

NASA Goddard Earth Sciences Data and Information Services Center (GES DISC) archives and distributes pioneering collections of data on atmospheric greenhouse gases. In September of 2012, the Atmospheric Infrared Sounder (AIRS) marked a decade of tropospheric observations of carbon dioxide (CO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> ). Most recently, the Atmospheric CO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> Observations from Space (ACOS) project and GES DISC released CO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> retrievals derived from radiances observed by the Japanese Greenhouse gases Observing SATellite (GOSAT) satellite, launched in 2009. In this letter, we present the most recent estimates of decadal mid-tropospheric trends of CO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> from AIRS, as well as the most recent status of the total column-average distribution of CO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> from ACOS. We also demonstrate that significant discrepancies still exist in the global distribution of observed and modeled column amounts of CO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> using the CO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> retrievals from the ACOS project.

A GPS network for tropospheric tomography in the framework of the Mediterranean hydrometeorological observatory Cévennes-Vivarais (southeastern France)

Abstract. The Mediterranean hydrometeorological observatory Cévennes-Vivarais (OHM-CV) coordinates hydrometeorological observations (radars, rain gauges, water level stations) on a regional scale in southeastern France. In the framework of OHM-CV, temporary GPS measurements have been carried out for 2 months in autumn 2002, when the heaviest rainfall are expected. These measurements increase the spatial density of the existing permanent GPS network, by adding three more receivers between the Mediterranean coast and the Cévennes-Vivarais range to monitor maritime source of water vapour flow feeding the precipitating systems over the Cévennes-Vivarais region. In addition, a local network of 18 receivers covered an area of 30 by 30 km within the field of view of the meteorological radar. These regional and local networks of permanent and temporary stations are used to monitor the precipitable water vapour (PWV) with high temporal resolution (15 min). Also, the dense local network provided data which have been inverted using tomographic techniques to obtain the 3-D field of tropospheric water vapour content. This study presents methodological tests for retrieving GPS tropospheric observations from dense networks, with the aim of assessing the uncertainties of GPS retrievals. Using optimal tropospheric GPS retrieval methods, high resolution measurements of PWV on a local scale (a few kilometres) are discussed for rain events. Finally, the results of 3-D fields of water vapour densities from GPS tomography are analysed with respect to precipitation fields derived from a meteorological radar, showing a good correlation between precipitation and water vapour depletion areas.

Thermodynamic and liquid profiling during the 2010 Winter Olympics

Tropospheric observations by a microwave profiling radiometer and six-hour radiosondes were obtained during the Alpine Venue of the 2010 Winter Olympic Games at Whistler, British Columbia, by Environment Canada. The radiometer provided continuous temperature, humidity and liquid (water) profiles during all weather conditions including rain, sleet and snow. Gridded analysis was provided by the U.S. National Oceanic and Atmospheric Administration. We compare more than two weeks of radiometer neural network and radiosonde temperature and humidity soundings including clear and precipitating conditions. Corresponding radiometer liquid and radiosonde wind soundings are shown. Close correlation is evident between radiometer and radiosonde temperature and humidity profiles up to 10km height and among southwest winds, liquid water and upper level thermodynamics, consistent with up-valley advection and condensation of moist maritime air. We compare brightness temperatures observed by the radiometer and forward-modeled from radiosonde and gridded analysis. Radiosonde-equivalent observation accuracy is demonstrated for radiometer neural network temperature and humidity retrievals up to 800m height and for variational retrievals that combine radiometer and gridded analysis up to 10km height.

An analysis of fast photochemistry over high northern latitudes during spring and summer using in-situ observations from ARCTAS and TOPSE

Abstract. Observations of chemical constituents and meteorological quantities obtained during the two Arctic phases of the airborne campaign ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) are analyzed using an observationally constrained steady state box model. Measurements of OH and HO2 from the Penn State ATHOS instrument are compared to model predictions. Forty percent of OH measurements below 2 km are at the limit of detection during the spring phase (ARCTAS-A). While the median observed-to-calculated ratio is near one, both the scatter of observations and the model uncertainty for OH are at the magnitude of ambient values. During the summer phase (ARCTAS-B), model predictions of OH are biased low relative to observations and demonstrate a high sensitivity to the level of uncertainty in NO observations. Predictions of HO2 using observed CH2O and H2O2 as model constraints are up to a factor of two larger than observed. A temperature-dependent terminal loss rate of HO2 to aerosol recently proposed in the literature is shown to be insufficient to reconcile these differences. A comparison of ARCTAS-A to the high latitude springtime portion of the 2000 TOPSE campaign (Tropospheric Ozone Production about the Spring Equinox) shows similar meteorological and chemical environments with the exception of peroxides; observations of H2O2 during ARCTAS-A were 2.5 to 3 times larger than those during TOPSE. The cause of this difference in peroxides remains unresolved and has important implications for the Arctic HOx budget. Unconstrained model predictions for both phases indicate photochemistry alone is unable to simultaneously sustain observed levels of CH2O and H2O2; however when the model is constrained with observed CH2O, H2O2 predictions from a range of rainout parameterizations bracket its observations. A mechanism suitable to explain observed concentrations of CH2O is uncertain. Free tropospheric observations of acetaldehyde (CH3CHO) are 2–3 times larger than its predictions, though constraint of the model to those observations is sufficient to account for less than half of the deficit in predicted CH2O. The box model calculates gross O3 formation during spring to maximize from 1–4 km at 0.8 ppbv d−1, in agreement with estimates from TOPSE, and a gross production of 2–4 ppbv d−1 in the boundary layer and upper troposphere during summer. Use of the lower observed levels of HO2 in place of model predictions decreases the gross production by 25–50%. Net O3 production is near zero throughout the ARCTAS-A troposphere, and is 1–2 ppbv in the boundary layer and upper altitudes during ARCTAS-B.

Tropospheric methanol observations from space: retrieval evaluation and constraints on the seasonality of biogenic emissions.

Methanol retrievals from nadir-viewing space-based sensors offer powerful new information for quantifying methanol emissions on a global scale. Here we apply an ensemble of aircraft observations over North America to evaluate new methanol measurements from the Tropospheric Emission Spectrometer (TES) on the Aura satellite, and combine the TES data with observations from the Infrared Atmospheric Sounding Interferometer (IASI) on the MetOp-A satellite to investigate the seasonality of methanol emissions from northern midlatitude ecosystems. Using the GEOS-Chem chemical transport model as an intercomparison platform, we find that the TES retrieval performs well when the degrees of freedom for signal (DOFS) are above 0.5, in which case the model:TES regressions are generally consistent with the model:aircraft comparisons. Including retrievals with DOFS below 0.5 degrades the comparisons, as these are excessively influenced by the a priori. The comparisons suggest DOFS >0.5 as a minimum threshold for interpreting retrievals of trace gases with a weak tropospheric signal. We analyze one full year of satellite observations and find that GEOS-Chem, driven with MEGANv2.1 biogenic emissions, underestimates observed methanol concentrations throughout the midlatitudes in springtime, with the timing of the seasonal peak in model emissions 1-2 months too late. We attribute this discrepancy to an underestimate of emissions from new leaves in MEGAN, and apply the satellite data to better quantify the seasonal change in methanol emissions for midlatitude ecosystems. The derived parameters (relative emission factors of 11.0, 0.26, 0.12 and 3.0 for new, growing, mature, and old leaves, respectively, plus a leaf area index activity factor of 0.5 for expanding canopies with leaf area index <1.2) provide a more realistic simulation of seasonal methanol concentrations in midlatitudes on the basis of both the IASI and TES measurements.

Technical Note: Formal blind intercomparison of OH measurements: results from the international campaign HOxComp

Abstract. Hydroxyl radicals (OH) are the major oxidizing species in the troposphere. Because of their central importance, absolute measurements of their concentrations are needed to validate chemical mechanisms of atmospheric models. The extremely low and highly variable concentrations in the troposphere, however, make measurements of OH difficult. Three techniques are currently used worldwide for tropospheric observations of OH after about 30~years of technical developments: Differential Optical Laser Absorption Spectroscopy (DOAS), Laser-Induced Fluorescence Spectroscopy (LIF), and Chemical Ionisation Mass Spectrometry (CIMS). Even though many measurement campaigns with OH data were published, the question of accuracy and precision is still under discussion. Here, we report results of the first formal, blind intercomparison of these techniques. Six OH instruments (4~LIF, 1~CIMS, 1~DOAS) participated successfully in the ground-based, international HOxComp campaign carried out in Jülich, Germany, in summer 2005. Comparisons were performed for three days in ambient air (3~LIF, 1 CIMS) and for six days in the atmosphere simulation chamber SAPHIR (3~LIF, 1~DOAS). All instruments were found to measure tropospheric OH concentrations with high sensitivity and good time resolution. The pairwise correlations between different data sets were linear and yielded high correlation coefficients (r2=0.75−0.96). Excellent absolute agreement was observed for the instruments at the SAPHIR chamber, yielding slopes between 1.01 and 1.13 in the linear regressions. In ambient air, the slopes deviated from unity by factors of 1.06 to 1.69, which can partly be explained by the stated instrumental accuracies. In addition, sampling inhomogeneities and calibration problems have apparently contributed to the discrepancies. The absolute intercepts of the linear regressions did not exceed 0.6×106 cm−3, mostly being insignificant and of minor importance for daytime observations of OH. No relevant interferences with respect to ozone, water vapour, NOx and peroxy radicals could be detected. The HOxComp campaign has demonstrated that OH can be measured reasonably well by current instruments, but also that there is still room for improvement of calibrations.

First results of the refurbished SOUSY radar: Tropopause altitude climatology at 78°N, 16°E, 2008

The second generation SOUSY MST radar at 78°N, 16°E on Svalbard has recently completed its inaugural year of combined troposphere and mesosphere observations. Here, troposphere observations have been processed using a robust detection algorithm designed for obtaining tropopause climatology by automatic data processing, and the resulting monthly statistics have been compared with corresponding surface air temperatures. As our main objective, we describe the new radar system, present the tropopause detection method, and validate the results using radiosonde and surface temperature data. The tropopause height depends on the temperature of the underlying atmosphere but is also influenced by downward control from the stratosphere. We find that the climatological tropopause height is correlated with the surface temperature but with the former lagging the latter by approximately 1 month.