Upper Troposphere/lower Stratosphere Research Articles

An improved OSIRIS NO2 profile retrieval in the upper troposphere–lower stratosphere and intercomparison with ACE-FTS and SAGE III/ISS

Abstract. The v7.2 NO2 retrieval for the Optical Spectrograph and InfraRed Imager System (OSIRIS) was designed to improve sensitivity in the upper troposphere–lower stratosphere (UTLS) and to reduce an observed low bias in the previous version, v6.0. The details of this retrieval are described and then the data are compared to coincident NO2 profiles from the Atmospheric Chemistry Experiment–Fourier Transform Spectrometer (ACE-FTS) and the Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS). The PRATMO photochemical box model was used to account for differences in the measurement times of the instruments: all datasets were scaled to the same local solar time of 12:00 LST. Coincident ACE-FTS and OSIRIS NO2 measurements agree within 20 % throughout much of the stratosphere. Coincident SAGE III/ISS and OSIRIS NO2 measurements also agree within 20 %, with OSIRIS biased low at all altitudes and latitudes. The ACE-FTS, OSIRIS, and SAGE III-ISS NO2 monthly zonal mean data show very similar variability in time at most altitude and latitudes.

Effects of Distant Organized Convection on Forecasts of Widespread Clear-Air Turbulence

Abstract Two cases of observed widespread moderate-or-greater (MOG) clear-air turbulence (CAT) in different synoptic patterns are investigated using a nested high-resolution NWP model. Both of these cases occurred in confluent entrance regions of upper-tropospheric–lower-stratospheric (UTLS) jet streaks, where large-scale anticyclonic outflow from distant organized moist convection strengthened the UTLS jet. Both the strength and vertical sharpness of the resulting jet influence the altitudes of MOG turbulence and the details of simulated turbulence onset mechanisms. In a strong and narrow UTLS jet downstream of a weak synoptic ridge, MOG turbulence arises from Kelvin–Helmholtz (KH) waves that overturn in opposite directions on the vertical flanks of the jet. In broader UTLS jets, MOG turbulence arising from KH waves was favored in strong vertical shear layers beneath the wind maximum, but was inhibited above it due to static stability increases near the tropopause. However, vertically propagating internal gravity waves initiated above KH wave breaking beneath the UTLS jet amplify within the lower stratosphere above the jet, constituting another possible source of turbulence. Turbulence onset mechanisms were often apparent in simulations with minimum horizontal grid spacings of Δx = 1 km. However, amplitudes of the associated grid-resolved vertical motions were unreliable when compared with simulations having minimum horizontal grid spacings of Δx = 1/3 km. In spite of this, turbulence forecasting systems driven by input from coarser-resolution operational NWP models are demonstrated to provide good diagnoses of this type of convectively influenced CAT when the NWP model accurately forecasts upstream convection. Significance Statement In this study we document the role of distant convection on observed widespread strong clear-air turbulence near upper-level jet streams in different weather patterns. Results from nested NWP model simulations, together with similar examples from previous case studies, suggest a strong association of widespread turbulence with jet stream enhancements related to outflow from upstream convection. We also demonstrate how model horizontal grid spacings of <1 km are required to adequately resolve common turbulence onset mechanisms (e.g., Kelvin–Helmholtz instability, gravity wave breaking). Nevertheless, examples are provided showing that turbulence forecasting systems driven by lower-resolution operational NWP models can provide potentially valuable guidance on these widespread turbulence events when those models accurately forecast the timing and locations of upstream convection.

Northern hemispheric atmospheric ethane trends in the upper troposphere and lower stratosphere (2006–2016) with reference to methane and propane

Abstract. Methane, ethane, and propane are among the most abundant hydrocarbons in the atmosphere. These compounds have many emission sources in common and are all primarily removed through OH oxidation. Their mixing ratios and long-term trends in the upper troposphere and stratosphere are rarely reported due to the paucity of measurements. In this study, we present long-term (2006–2016) northern hemispheric ethane, propane, and methane data from airborne observation in the upper troposphere-lower stratosphere (UTLS) region from the IAGOS-CARIBIC project. The methane and propane observations provide additional information for understanding northern hemispheric ethane trends, which is the major focus of this study. The linear trends, moving averages, nonlinear trends and monthly variations of ethane, methane and propane in 2006–2016 are presented for the upper troposphere and lower stratosphere over 5 regions (whole Northern Hemisphere, Europe, North America, Asia and the rest of the world). The growth rates of ethane, methane, and propane in the upper troposphere are −2.24 % yr−1, 0.33 % yr−1, and −0.78 % yr−1, respectively, and in the lower stratosphere they are −3.27 % yr−1, 0.26 % yr−1, and −4.91 % yr−1, respectively, in 2006–2016. This dataset is of value to future global ethane budget estimates and the optimization of current ethane inventories. The data are publicly accessible at https://doi.org/10.5281/zenodo.6536109 (Li et al., 2022a).

Tropopause-Level NOx in the Asian Summer Monsoon.

Deep convection within the Asian summer monsoon (ASM) transports surface level air into the upper troposphere‐lower stratosphere (UTLS). This work aims to understand the distribution of NO2, NO, and NOx in the UTLS ASM anticyclone from satellite measurements. Observations of NO2 from the Optical Spectrograph and InfraRed Imager System, the Atmospheric Chemistry Experiment ‐ Fourier Transform Spectrometer (ACE‐FTS), and the Stratospheric Aerosol and Gas Experiment III on the International Space Station are considered. The PRATMO photochemical box model is used to quantify the NOx photochemistry, and to derive the NOx concentration using OSIRIS NO2 and O3 observations. The satellite data show a relative minimum in NO2 over the ASM in the summer months, while the corresponding NO and NOx anomalies are elevated, mainly due to low O3 and cold temperatures within the ASM. The observations within the ASM show reasonable agreement to simulations from the Whole Atmosphere Community Climate Model.

Intercomparison of upper tropospheric and lower stratospheric water vapor measurements over the Asian Summer Monsoon during the StratoClim campaign

Abstract. In situ measurements in the climatically important upper troposphere–lower stratosphere (UTLS) are critical for understanding controls on cloud formation, the entry of water into the stratosphere, and hydration–dehydration of the tropical tropopause layer. Accurate in situ measurement of water vapor in the UTLS however is difficult because of low water vapor concentrations (<5 ppmv) and a challenging low temperature–pressure environment. The StratoClim campaign out of Kathmandu, Nepal, in July and August 2017, which made the first high-altitude aircraft measurements in the Asian Summer Monsoon (ASM), also provided an opportunity to intercompare three in situ hygrometers mounted on the M-55 Geophysica: ChiWIS (Chicago Water Isotope Spectrometer), FISH (Fast In situ Stratospheric Hygrometer), and FLASH (Fluorescent Lyman-α Stratospheric Hygrometer). Instrument agreement was very good, suggesting no intrinsic technique-dependent biases: ChiWIS measures by mid-infrared laser absorption spectroscopy and FISH and FLASH by Lyman-α induced fluorescence. In clear-sky UTLS conditions (H2O<10 ppmv), mean and standard deviations of differences in paired observations between ChiWIS and FLASH were only (-1.4±5.9) % and those between FISH and FLASH only (-1.5±8.0) %. Agreement between ChiWIS and FLASH for in-cloud conditions is even tighter, at (+0.7±7.6) %. Estimated realized instrumental precision in UTLS conditions was 0.05, 0.2, and 0.1 ppmv for ChiWIS, FLASH, and FISH, respectively. This level of accuracy and precision allows the confident detection of fine-scale spatial structures in UTLS water vapor required for understanding the role of convection and the ASM in the stratospheric water vapor budget.

Synergetic use of IASI profile and TROPOMI total-column level 2 methane retrieval products

Abstract. The thermal infrared nadir spectra of IASI (Infrared Atmospheric Sounding Interferometer) are successfully used for retrievals of different atmospheric trace gas profiles. However, these retrievals offer generally reduced information about the lowermost tropospheric layer due to the lack of thermal contrast close to the surface. Spectra of scattered solar radiation observed in the near-infrared and/or shortwave infrared, for instance by TROPOMI (TROPOspheric Monitoring Instrument), offer higher sensitivity near the ground and are used for the retrieval of total-column-averaged mixing ratios of a variety of atmospheric trace gases. Here we present a method for the synergetic use of IASI profile and TROPOMI total-column level 2 retrieval products. Our method uses the output of the individual retrievals and consists of linear algebra a posteriori calculations (i.e. calculation after the individual retrievals). We show that this approach has strong theoretical similarities to applying the spectra of the different sensors together in a single retrieval procedure but with the substantial advantage of being applicable to data generated with different individual retrieval processors, of being very time efficient, and of directly benefiting from the high quality and most recent improvements of the individual retrieval processors. We demonstrate the method exemplarily for atmospheric methane (CH4). We perform a theoretical evaluation and show that the a posteriori combination method yields a total-column-averaged CH4 product (XCH4) that conserves the good sensitivity of the corresponding TROPOMI product while merging it with the high-quality upper troposphere–lower stratosphere (UTLS) CH4 partial-column information of the corresponding IASI product. As a consequence, the combined product offers additional sensitivity for the tropospheric CH4 partial column, which is not provided by the individual TROPOMI nor the individual IASI product. The theoretically predicted synergetic effect is verified by comparisons to CH4 reference data obtained from collocated XCH4 measurements at 14 globally distributed TCCON (Total Carbon Column Observing Network) stations, CH4 profile measurements made by 36 individual AirCore soundings, and tropospheric CH4 data derived from continuous ground-based in situ observations made at two nearby Global Atmospheric Watch (GAW) mountain stations. The comparisons clearly demonstrate that the combined product can reliably detect the actual variations of atmospheric XCH4, CH4 in the UTLS, and CH4 in the troposphere. A similar good reliability for the latter is not achievable by the individual TROPOMI and IASI products.

Impact of biomass burning and stratospheric intrusions in the remote South Pacific Ocean troposphere

Abstract. The ozone mixing ratio spatiotemporal variability in the pristine South Pacific Ocean is studied, for the first time, using 21-year-long ozone (O3) records from the entire southern tropical and subtropical Pacific between 1994 and 2014. The analysis considered regional O3 vertical observations from ozonesondes, surface carbon monoxide (CO) observations from flasks, and three-dimensional chemistry-transport model simulations of the global troposphere. Two 21-year-long numerical simulations, with and without biomass burning emissions, were performed to disentangle the importance of biomass burning relative to stratospheric intrusions for ambient ozone levels in the region. Tagged tracers of O3 from the stratosphere and CO from various biomass burning regions have been used to track the impact of these different regions on the southern tropical Pacific O3 and CO levels. Patterns have been analyzed based on atmospheric dynamics variability. Considering the interannual variability in the observations, the model can capture the observed ozone gradients in the troposphere with a positive bias of 7.5 % in the upper troposphere/lower stratosphere (UTLS) as well as near the surface. Remarkably, even the most pristine region of the global ocean is affected by distant biomass burning emissions by convective outflow through the mid and high troposphere and subsequent subsidence over the pristine oceanic region. Therefore, the biomass burning contribution to tropospheric CO levels maximizes in the UTLS. The Southeast Asian open fires have been identified as the major contributing source to CO from biomass burning in the tropical South Pacific, contributing on average for the study period about 8.5 and 13 ppbv of CO at Rapa Nui and Samoa, respectively, at an altitude of around 12 km during the burning season in the spring of the Southern Hemisphere. South America is the second-most important biomass burning source region that influences the study area. Its impact maximizes in the lower troposphere (6.5 ppbv for Rapa Nui and 3.8 ppbv for Samoa). All biomass burning sources contribute about 15–23 ppbv of CO at Rapa Nui and Samoa and account for about 25 % of the total CO in the entire troposphere of the tropical and subtropical South Pacific. This impact is also seen on tropospheric O3, to which biomass burning O3 precursor emissions contribute only a few ppbv during the burning period, while the stratosphere–troposphere exchange is the most important source of O3 for the mid troposphere of the South Pacific Ocean, contributing about 15–20 ppbv in the subtropics.

Simulation of Arctic Thin Ice Clouds with Canadian Regional Climate Model Version 6: Verification against CloudSat-CALIPSO

Polar clouds are, as a consequence of the paucity of in situ observations, poorly understood compared to their lower latitude analogs, yet highly climate-sensitive through thermal radiation emission. The prevalence of Thin Ice Clouds (TIC) dominates in cold Polar Regions and the Upper Troposphere Lower Stratosphere (UTLS) altitudes. They can be grouped into 2 broad categories. The first thin ice cloud type (TIC1) is made up of high concentrations of small, non-precipitating ice crystals. The second type (TIC2) is composed of relatively small concentrations of larger, precipitating ice crystals. In this study, we investigate the ability of a developmental version of the Canadian Regional Climate Model (CRCM6) in simulating cold polar-night clouds over the Arctic Ocean, a remote region that is critical to atmospheric circulation reaching out to the mid-latitudes. The results show that, relative to CloudSat-CALIPSO vertical profile products, CRCM6 simulates high-latitude and low spatial frequency variations of Ice Water Content (IWC), effective radius (re) and cooling rates reasonably well with only small to moderate wet and dry biases. The model can also simulate cloud type, location, and temporal occurrence effectively. As well, it successfully simulated higher altitude TIC1 clouds whose small size evaded CloudSat detection while being visible to CALIPSO.

Stability of CubeSat Clocks and Their Impacts on GNSS Radio Occultation

Global Navigation Satellite Systems’ radio occultation (GNSS-RO) provides the upper troposphere-lower stratosphere (UTLS) vertical atmospheric profiles that are complementing radiosonde and reanalysis data. Such data are employed in the numerical weather prediction (NWP) models used to forecast global weather as well as in climate change studies. Typically, GNSS-RO operates by remotely sensing the bending angles of an occulting GNSS signal measured by larger low Earth orbit (LEO) satellites. However, these satellites are faced with complexities in their design and costs. CubeSats, on the other hand, are emerging small and cheap satellites; the low prices of building them and the advancements in their components make them favorable for the GNSS-RO. In order to be compatible with GNSS-RO requirements, the clocks of the onboard receivers that are estimated through the precise orbit determination (POD) should have short-term stabilities. This is essential to correctly time tag the excess phase observations used in the derivation of the GNSS-RO UTLS atmospheric profiles. In this study, the stabilities of estimated clocks of a set of CubeSats launched for GNSS-RO in the Spire Global constellation are rigorously analysed and evaluated in comparison to the ultra-stable oscillators (USOs) onboard the Constellation Observing System for Meteorology, Ionosphere, and Climate (COSMIC-2) satellites. Methods for improving their clock stabilities are proposed and tested. The results (i) show improvement of the estimated clocks at the level of several microseconds, which increases their short-term stabilities, (ii) indicate that the quality of the frequency oscillator plays a dominant role in CubeSats’ clock instabilities, and (iii) show that CubeSats’ derived UTLS (i.e., tropopause) atmospheric profiles are comparable to those of COSMIC-2 products and in situ radiosonde observations, which provided external validation products. Different comparisons confirm that CubeSats, even those with unstable onboard clocks, provide high-quality RO profiles, comparable to those of COSMIC-2. The proposed remedies in POD and the advancements of the COTS components, such as chip-scale atomic clocks and better onboard processing units, also present a brighter future for real-time applications that require precise orbits and stable clocks.

Influence of NOX, Cl, and Br on the upper core of the ozone valley over the Tibetan Plateau during summer: Simulations with a box model

The ozone valley (OV) in the upper troposphere-lower stratosphere (UTLS) over the Tibetan Plateau (TP) has been identified since the 1990s during boreal summer. Recent studies have shown that another upper core of the OV appeared in the middle and upper stratosphere (10–2 hPa); however, the formation mechanism of the OV in the upper stratosphere remains unclear. In this paper, Microwave Limb Sounder (MLS) data from the Aura satellite and the stratospheric heterogeneous chemical reaction box model are used to investigate the impact of chemical substances, including NO, NO2, Cl and Br, on the ozone valley in the middle and upper stratosphere over the TP. The results show that the formation mechanism of the diurnal and nighttime variation in the upper core of the OV over the TP in the summer may be related to the different daytime and nighttime distributions of NO2 and the difference in daytime and nighttime average temperatures between the TP and the same latitude regions.

Evaluating the influence of deep convection on tropopause thermodynamics and lower stratospheric water vapor: A RELAMPAGO case study using the WRF model

Troposphere to stratosphere exchange is generally driven by deep convection capable of overshooting tropospheric materials contributing to stratospheric chemistry. The La Plata Basin region in South America is known for organized deep convection and mesoscale convective systems. This study employs the Weather Research and Forecasting model to simulate deep convection during the RELAMPAGO field campaign in Argentina. This work investigates upper troposphere – lower stratosphere (UTLS) thermodynamics, specifically double tropopause events, and identifies lower stratospheric hydration related to deep convection. Results show that lower stratospheric hydration occurred during two organized convective types, a mesoscale convective complex (MCC) and squall line, which coincided with strong low level jet moisture transport. However, the lower stratosphere was not hydrated during discrete cells. While UTLS moisture was present in all three convective types, during the discrete cell, ice and water vapor were mixed, inhibiting net positive buoyancy and the transport of tropospheric material aloft. During the MCC and squall line events, UTLS moisture was stratified. A dry layer in the tropopause was collocated with an ice layer where net positive buoyancy contributed to stratospheric hydration as high as 20 km.

Day-to-day variability of upper troposphere and lower stratosphere temperature in response to Taal volcanic eruption inferred from COSMIC-2 RO measurements

For the first time after 43 years of its previous eruption in 1977, the Taal volcano in the Philippines (14°N, 120°.59E) erupted in the afternoon of 12 January 2020. Due to the strong anticyclonic circulation in the upper troposphere (~150 hPa), the resultant volcanic ash and sulfur dioxide (SO2) were transported to the downwind tropical central Pacific Ocean within a few days after the initial eruption. In this study, day-to-day variability of upper troposphere lower stratosphere (UTLS) temperature in response to the Taal volcanic eruption event over the source region (±5o latitude and longitude around the volcano) and the downwind Pacific region (10-20oN, 160-180°E) is delineated by using the recently launched Constellation Observing System for Meteorology, Ionosphere, and Climate (COSMIC)-2 radio occultation (RO) data. The daily mean temperature over the source and downwind regions were compared with the background long-term January mean temperature (obtained from 2007 to 2019 COSMIC-1 RO data) over the respective regions. Significant positive temperature anomalies in the lower stratosphere are evident over the source (between 12 and 14 January) and downwind (between 14 and 19 January) regions after the eruption. These positive anomalies may be due to the association of absorption and local radiative heating by volcanic aerosols. The Ozone Monitoring Instrument (OMI) measurements clearly show the presence of SO2 in the UTLS region. The presence of sulfate aerosols in the UTLS region a few days after eruption is also supported by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) images. Furthermore, we also describe the temperature structure near the volcano and away from the volcano and found a quite different structure in the UTLS region. A significant temperature inversion at ~15 km altitude is evident near the volcano, whereas it is noticed at ~16 km away from the volcano. In conclusion, in line with the previous studies, the present study provides further insights to the UTLS temperature in response to volcanic eruptions.

The effects of the COVID-19 lockdowns on the composition of the troposphere as seen by In-service Aircraft for a Global Observing System (IAGOS) at Frankfurt

Abstract. The European research infrastructure IAGOS (In-service Aircraft for a Global Observing System) equips commercial aircraft with a system for measuring atmospheric composition. A range of essential climate variables and air quality parameters are measured throughout the flight, from take-off to landing, giving high-resolution information in the vertical in the vicinity of international airports and in the upper troposphere–lower stratosphere during the cruise phase of the flight. Six airlines are currently involved in the programme, achieving a quasi-global coverage under normal circumstances. During the COVID-19 crisis, many airlines were forced to ground their fleets due to a fall in passenger numbers and imposed travel restrictions. Deutsche Lufthansa, a partner in IAGOS since 1994 was able to operate an IAGOS-equipped aircraft during the COVID-19 lockdown, providing regular measurements of ozone and carbon monoxide at Frankfurt Airport. The data form a snapshot of an unprecedented time in the 27-year time series. In May 2020, we see a 32 % increase in ozone near the surface with respect to a recent reference period, a magnitude similar to that of the 2003 heatwave. The anomaly in May is driven by an increase in ozone at nighttime which might be linked to the reduction in NO during the COVID-19 lockdowns. The anomaly diminishes with altitude becoming a slightly negative anomaly in the free troposphere. The ozone precursor carbon monoxide shows an 11 % reduction in MAM (March–April–May) near the surface. There is only a small reduction in CO in the free troposphere due to the impact of long-range transport on the CO from emissions in regions outside Europe. This is confirmed by data from the Infrared Atmospheric Sounding Interferometer (IASI) using retrievals performed by SOftware for a Fast Retrieval of IASI Data (SOFRID), which display a clear drop of CO at 800 hPa over Europe in March but otherwise show little change to the abundance of CO in the free troposphere.

Short vertical-wavelength gravity wave activities in the upper troposphere lower stratosphere observed with global navigation satellite system radio occultation under different QBO phases

Gravity Waves (GWs) are believed to play important role in the generation of the driving force of the stratospheric Quasi-Biennial Oscillation (QBO). Deep convection in the equatorial region can generate large amount of GW with short vertical wavelength (λz <1 km) but studies of these wave activities in the upper troposphere lower stratosphere (UTLS) region are still limited. Recent advances in Global Navigation Satellite System (GNSS) Radio Occultation (RO) retrieval techniques have made it possible to derive global temperature profile with vertical resolution of less than 1 km. In this research, activities of GW with λz from 0.5 to 3.5 km in the UTLS region of 20-27 km heights are identified by calculating the GW potential energy (E p). Correlation between GW activities and QBO phases is examined using 50 hPa zonal wind as the QBO index. The results show that during both easterly and westerly QBO phases, the GW E p value increases gradually with time and reaches its peak in the transition periods. This pattern is seen in E p with all vertical wavelengths between 0.5-3.5 km but the percentage value of E p for λz<1 km is higher during the transition from westerly to easterly QBO. The GW E p values exhibit downward propagation with the QBO phase but there are also discernible upward propagations of GW activities below 24 km height and intersect those two bring large changes in QBO phases. Additionally, higher percentage of E p with λz<1 km is also found to be associated with El Niño events.

In situ observation of new particle formation (NPF) in the tropical tropopause layer of the 2017 Asian monsoon anticyclone – Part 1: Summary of StratoClim results

Abstract. During the monsoon season of the year 2017 the airborne StratoClim mission took place in Kathmandu, Nepal, with eight mission flights of the M-55 Geophysica in the upper troposphere–lower stratosphere (UTLS) of the Asian monsoon anticyclone (AMA) over northern India, Nepal, and Bangladesh. More than 100 events of new particle formation (NPF) were observed. In total, more than 2 h of flight time was spent under NPF conditions as indicated by the abundant presence of nucleation-mode aerosols, i.e. with particle diameters dp smaller than 15 nm, which were detected in situ by means of condensation nuclei counting techniques. Mixing ratios of nucleation-mode particles (nnm) of up to ∼ 50 000 mg−1 were measured at heights of 15–16 km (θ ≈ 370 K). NPF was most frequently observed at ∼ 12–16 km altitude (θ ≈ 355–380 K) and mainly below the tropopause. Resulting nnm remained elevated (∼ 300–2000 mg−1) up to altitudes of ∼ 17.5 km (θ ≈ 400 K), while under NPF conditions the fraction (f) of sub-micrometre-sized non-volatile residues (dp &gt; 10 nm) remained below 50 %. At ∼ 12–14 km (θ ≈ 355–365 K) the minimum of f (&lt; 15 %) was found, and underneath, the median f generally remains below 25 %. The persistence of particles at nucleation-mode sizes is limited to a few hours, mainly due to coagulation, as demonstrated by a numerical simulation. The frequency of NPF events observed during StratoClim 2017 underlines the importance of the AMA as a source region for UTLS aerosols and for the formation and maintenance of the Asian tropopause aerosol layer (ATAL). The observed abundance of NPF-produced nucleation-mode particles within the AMA is not unambiguously attributable to (a) specific source regions in the boundary layer (according to backward trajectory analyses), or (b) the direct supply with precursor material by convective updraught (from correlations of NPF with carbon monoxide), or (c) the recent release of NPF-capable material from the convective outflow (according to air mass transport times in the tropical tropopause layer, TTL). Temperature anomalies with ΔT of 2 K (peak-to-peak amplitude), as observed at a horizontal wavelength of ∼ 70–100 km during a level flight of several hours, match with NPF detections and represent an additional mechanism for local increases in supersaturation of the NPF precursors. Effective precursor supply and widely distributed temperature anomalies within the AMA can explain the higher frequency of intense NPF observed during StratoClim 2017 than all previous NPF detections with COPAS (COndensation PArticle counting System) at TTL levels over Brazil, northern Australia, or West Africa.

Spatial-temporal distribution of atmospheric temperature anomalies connected with seismic activity in Tien-Shan

In this paper we analyzed spatial-temporal temperature changes in the upper troposphere/lower stratosphere (UTLS) above the Northern and Central Tien-Shan detected by satellite remote sensing which have been compared against seismic activity in (1992-2015). These anomalous changes in temperature time series were used as pre-seismic indicators. Anomalous variation parameters were calculated accounting for amplitude and phase of short-time temperature variations at UTLS isobaric levels separated by the tropopause. The results show that the spatial structure and dynamics of temperature anomalies in the area of UTLS have a sufficiently stable relation to seismic activity. We estimated the spatial and time variability of anomalous temperature perturbations on the basis of 12 strongest earthquakes with magnitudes Mï5.0. The temperature anomalies were observed in all considered cases from ~3 to 72 hours before the main seismic event.

On the occurrence of strong vertical wind shear in the tropopause region: a 10-year ERA5 northern hemispheric study

Abstract. A climatology of the occurrence of strong wind shear in the upper troposphere–lower stratosphere (UTLS) is presented, which gives rise to defining a tropopause shear layer (TSL). Strong wind shear in the tropopause region is of interest because it can generate turbulence, which can lead to cross-tropopause mixing. The analysis is based on 10 years of daily northern hemispheric ECMWF ERA5 reanalysis data. The vertical extent of the region analyzed is limited to the altitudes from 1.5 km above the surface up to 25 km, to exclude the planetary boundary layer as well as strong wind shear in higher atmospheric layers like the mesosphere–lower thermosphere. A threshold value of St2=4×10-4s-2 of the squared vertical shear of the horizontal wind is applied, which marks the top end of the distribution of atmospheric wind shear to focus on situations which cannot be sustained by the mean static stability in the troposphere according to linear theory. This subset of the vertical wind shear spectrum is analyzed for its vertical, geographical, and seasonal occurrence frequency distribution. A set of metrics is defined to narrow down the relation to planetary circulation features, as well as indicators for momentum-gradient-sharpening mechanisms. The vertical distribution reveals that strong vertical wind shear above the threshold occurs almost exclusively at tropopause altitudes, within a vertically confined layer of about 1–2 km in extent directly above the local lapse rate tropopause. The TSL emerges as a distinct feature in the tropopause-based 10-year temporal and zonal mean climatology, spanning from the tropics to latitudes around 70∘ N, with average occurrence frequencies on the order of 1 %–10 %. The horizontal distribution of the strong vertical wind shear near the tropopause exhibits distinctly separated regions of occurrence, which are generally associated with jet streams and their seasonality. At midlatitudes, strong wind shear values occur most frequently in regions with an elevated tropopause and at latitudes around 50∘ N, associated with jet streaks within northward-reaching ridges of baroclinic waves. At lower latitudes in the region of the subtropical jet stream, which is mainly apparent over the east Asian continent, the occurrence frequency of strong wind shear near the tropopause reaches maximum values of about 30 % during winter and is tightly linked to the jet stream seasonality. The interannual variability of the occurrence frequency for strong wind shear might furthermore be linked to the variability of the zonal location and strength of the jet. The east-equatorial region features a bi-annual seasonality in the occurrence frequencies of strong vertical wind shear near the tropopause. During the summer months, large areas of the tropopause region over the Indian Ocean are up to 70 % of the time exposed to strong wind shear, which can be attributed to the emergence of the tropical easterly jet. During winter, this occurrence frequency maximum shifts eastward over the maritime continent, where it is exceptionally pronounced during the DJF 2010/11 La Niña phase, as well as quite weak during the El Niño phases of 2009/10, 2014/15, and 2015/16. This agrees with the atmospheric response of the Pacific Walker circulation cell in the El Niño–Southern Oscillation (ENSO) ocean–atmosphere coupling.

3-D tomographic observations of Rossby wave breaking over the North Atlantic during the WISE aircraft campaign in 2017

Abstract. This paper presents measurements of ozone, water vapour and nitric acid (HNO3) in the upper troposphere/lower stratosphere (UTLS) over North Atlantic and Europe. The measurements were acquired with the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the Wave Driven Isentropic Exchange (WISE) campaign in October 2017. GLORIA is an airborne limb imager capable of acquiring both 2-D data sets (curtains along the flight path) and, when the carrier aircraft is flying around the observed air mass, spatially highly resolved 3-D tomographic data. Here, we present a case study of a Rossby wave (RW) breaking event observed during two subsequent flights 2 d apart. RW breaking is known to steepen tracer gradients and facilitate stratosphere–troposphere exchange (STE). Our measurements reveal complex spatial structures in stratospheric tracers (ozone and nitric acid) with multiple vertically stacked filaments. Backward-trajectory analysis is used to demonstrate that these features are related to several previous Rossby wave breaking events and that the small-scale structure of the UTLS in the Rossby wave breaking region, which is otherwise very hard to observe, can be understood as stirring and mixing of air masses of tropospheric and stratospheric origin. It is also shown that a strong nitric acid enhancement observed just above the tropopause is likely a result of NOx production by lightning activity. The measurements showed signatures of enhanced mixing between stratospheric and tropospheric air near the polar jet with some transport of water vapour into the stratosphere. Some of the air masses seen in 3-D data were encountered again 2 d later, stretched to very thin filament (horizontal thickness down to 30 km at some altitudes) rich in stratospheric tracers. This repeated measurement allowed us to directly observe and analyse the progress of mixing processes in a thin filament over 2 d. Our results provide direct insight into small-scale dynamics of the UTLS in the Rossby wave breaking region, which is of great importance to understanding STE and poleward transport in the UTLS.

Oxidation of low-molecular-weight organic compounds in cloud droplets: global impact on tropospheric oxidants

Abstract. In liquid cloud droplets, superoxide anion (O2(aq)-) is known to quickly consume ozone (O3(aq)), which is relatively insoluble. The significance of this reaction as a tropospheric O3 sink is sensitive to the abundance of O2(aq)- and therefore to the production of its main precursor, the hydroperoxyl radical (HO2(aq)). The aqueous-phase oxidation of oxygenated volatile organic compounds (OVOCs) is the major source of HO2(aq) in cloud droplets. Hence, the lack of explicit aqueous-phase chemical kinetics in global atmospheric models leads to a general underestimation of clouds as O3 sinks. In this study, the importance of in-cloud OVOC oxidation for tropospheric composition is assessed by using the Chemistry As A Boxmodel Application (CAABA) and the global ECHAM/MESSy Atmospheric Chemistry (EMAC) model, which are both capable of explicitly representing the relevant chemical transformations. For this analysis, three different in-cloud oxidation mechanisms are employed: (1) one including the basic oxidation of SO2(aq) by O3(aq) and H2O2(aq), which thus represents the capabilities of most global models; (2) the more advanced standard EMAC mechanism, which includes inorganic chemistry and simplified degradation of methane oxidation products; and (3) the detailed in-cloud OVOC oxidation scheme Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC). By using EMAC, the global impact of each mechanism is assessed focusing mainly on tropospheric volatile organic compounds (VOCs), HOx (HOx=OH+HO2), and O3. This is achieved by performing a detailed HOx and O3 budget analysis in the gas and aqueous phase. The resulting changes are evaluated against O3 and methanol (CH3OH) satellite observations from the Infrared Atmospheric Sounding Interferometer (IASI) for 2015. In general, the explicit in-cloud oxidation leads to an overall reduction in predicted OVOC levels and reduces EMAC's overestimation of some OVOCs in the tropics. The in-cloud OVOC oxidation shifts the HO2 production from the gas to the aqueous phase. As a result, the O3 budget is perturbed with scavenging being enhanced and the gas-phase chemical losses being reduced. With the simplified in-cloud chemistry, about 13 Tg yr−1 of O3 is scavenged, which increases to 336 Tg yr−1 when JAMOC is used. The highest O3 reduction of 12 % is predicted in the upper troposphere–lower stratosphere (UTLS). These changes in the free troposphere significantly reduce the modelled tropospheric ozone columns, which are known to be generally overestimated by EMAC and other global atmospheric models.

Lidar observations of cirrus clouds in Palau (7°33′ N, 134°48′ E)

Abstract. A polarization diversity elastic backscatter lidar was deployed on the equatorial island of Palau in February and March 2016 in the framework of the EU StratoClim project. The system operated unattended in the Palau Atmosferic Observatory from 15 February to 25 March 2016 during the nighttime. Each lidar profile extends from the ground to 30 km height. Here, the dataset is presented and discussed in terms of the temperature structure of the upper troposphere–lower stratosphere (UTLS) obtained from co-located radiosoundings. The cold-point tropopause (CPT) was higher than 17 km. During the campaign, several high-altitude clouds were observed, peaking approximately 3 km below the CPT. Their occurrence was associated with cold anomalies in the upper troposphere (UT). Conversely, when warm UT anomalies occurred, the presence of cirrus was restricted to a 5 km thick layer centred 5 km below the CPT. Thin and subvisible cirrus (SVC) were frequently detected close to the CPT. The particle depolarization ratios of these cirrus were generally lower than the values detected in the UT clouds. CPT cirrus occurrence showed a correlation with cold anomalies likely triggered by stratospheric wave activity penetrating the UT. The back-trajectories study revealed a thermal and convective history compatible with the convective outflow formation for most of the cirrus clouds, suggesting that the majority of air masses related to the clouds had encountered convection in the past and had reached the minimum temperature during its transport in less than 48 h before the observation. A subset of SVC with low depolarization and no sign of significative recent uplifting may have originated in situ.