Tropical Upper Troposphere Lower Stratosphere Research Articles

Evidence of a dual African and Australian biomass burning influence on the vertical distribution of aerosol and carbon monoxide over the southwest Indian Ocean basin in early 2020

Abstract. During the 2020 austral summer, the pristine atmosphere of the southwest Indian Ocean (SWIO) basin experienced significant perturbations. This study examines the variability of aerosols and carbon monoxide (CO) over this remote oceanic region and investigates the underlying processes in the upper troposphere–lower stratosphere (UT-LS). Aerosol profiles in January and February 2020 revealed a multi-layer structure in the tropical UT-LS. Numerical models – the FLEXible PARTicle dispersion model (FLEXPART) and the Modèle Isentropique de transport Mésoéchelle de l'Ozone Stratosphérique par Advection (MIMOSA) – indicated that the lower-stratospheric aerosol content was influenced by the intense and persistent stratospheric aerosol layer generated during the 2019–2020 extreme Australian bushfire events. A portion of this layer was transported eastward by prevailing easterly winds, leading to increased aerosol extinction profiles over Réunion on 27 and 28 January. Analysis of advected potential vorticity revealed isentropic transport of air masses containing Australian biomass burning aerosols from extratropical latitudes to Réunion at the 400 K isentropic level on 28 January. Interestingly, we found that biomass burning (BB) activity in eastern Africa, though weak during this season, significantly influenced (contributed up to 90 % of) the vertical distribution of CO and aerosols in the upper troposphere over the SWIO basin. Ground-based observations at Réunion confirmed the simultaneous presence of African and Australian aerosol layers. This study provides the first evidence of African BB emissions impacting the CO and aerosol distribution in the upper troposphere over the SWIO basin during the convective season.

Characterization of refractory aerosol particles collected in the tropical upper troposphere–lower stratosphere (UTLS) within the Asian tropopause aerosol layer (ATAL)

Abstract. Aerosol particles with diameters larger than 40 nm were collected during the flight campaign StratoClim 2017 within the Asian tropopause aerosol layer (ATAL) of the 2017 monsoon anticyclone above the Indian subcontinent. A multi-impactor system was installed on board the aircraft M-55 Geophysica, which was operated from Kathmandu, Nepal. The size and chemical composition of more than 5000 refractory particles/inclusions of 17 selected particle samples from seven different flights were analyzed by use of scanning electron microscopy (SEM) and transmission electron microscopy (TEM) combined with energy dispersive X-ray (EDX) microanalysis. Based on chemical composition and morphology, the refractory particles were assigned to the following particle groups: extraterrestrial, silicates, Fe-rich, Al-rich, Hg-rich, other metals, C-rich, soot, Cl-rich, and Ca-rich. Most abundant particle groups within the refractory particles are silicates and C-rich (non-volatile organics). In samples taken above the tropopause, extraterrestrial particles are becoming increasingly important with rising altitude. The most frequent particle sources for the small (maximum in size distribution DP-max=120 nm) refractory particles carried into the ATAL are combustion processes at the ground (burning of fossil fuels/biomass burning) and the agitation of soil material. The refractory particles in the ATAL represent only a very small fraction (< 2 % by number for particles > 40 nm) of the total aerosol particles, which are dominated by species like ammonium, sulfate, nitrate, and volatile organics. During one flight, a large number of very small (DP-max=25 nm) cinnabar particles (HgS) were detected, which are supposed to originate from a ground source such as coal combustion or underground coal fires.

Technical note: Reanalysis of Aura MLS chemical observations

Abstract. This paper presents a reanalysis of the atmospheric chemical composition from the upper troposphere to the lower mesosphere from August 2004 to December 2017. This reanalysis is produced by the Belgian Assimilation System for Chemical ObsErvations (BASCOE) constrained by the chemical observations from the Microwave Limb Sounder (MLS) on board the Aura satellite. BASCOE is based on the ensemble Kalman filter (EnKF) method and includes a chemical transport model driven by the winds and temperature from the ERA-Interim meteorological reanalysis. The model resolution is 3.75∘ in longitude, 2.5∘ in latitude and 37 vertical levels from the surface to 0.1 hPa with 25 levels above 100 hPa. The outputs are provided every 6 h. This reanalysis is called BRAM2 for BASCOE Reanalysis of Aura MLS, version 2. Vertical profiles of eight species from MLS version 4 are assimilated and are evaluated in this paper: ozone (O3), water vapour (H2O), nitrous oxide (N2O), nitric acid (HNO3), hydrogen chloride (HCl), chlorine oxide (ClO), methyl chloride (CH3Cl) and carbon monoxide (CO). They are evaluated using independent observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) and N2O observations from a different MLS radiometer than the one used to deliver the standard product and ozonesondes. The evaluation is carried out in four regions of interest where only selected species are evaluated. These regions are (1) the lower-stratospheric polar vortex where O3, H2O, N2O, HNO3, HCl and ClO are evaluated; (2) the upper-stratospheric–lower-mesospheric polar vortex where H2O, N2O, HNO3 and CO are evaluated; (3) the upper troposphere–lower stratosphere (UTLS) where O3, H2O, CO and CH3Cl are evaluated; and (4) the middle stratosphere where O3, H2O, N2O, HNO3, HCl, ClO and CH3Cl are evaluated. In general BRAM2 reproduces MLS observations within their uncertainties and agrees well with independent observations, with several limitations discussed in this paper (see the summary in Sect. 5.5). In particular, ozone is not assimilated at altitudes above (i.e. pressures lower than) 4 hPa due to a model bias that cannot be corrected by the assimilation. MLS ozone profiles display unphysical oscillations in the tropical UTLS, which are corrected by the assimilation, allowing a good agreement with ozonesondes. Moreover, in the upper troposphere, comparison of BRAM2 with MLS and independent observations suggests a positive bias in MLS O3 and a negative bias in MLS H2O. The reanalysis also reveals a drift in MLS N2O against independent observations, which highlights the potential use of BRAM2 to estimate biases between instruments. BRAM2 is publicly available and will be extended to assimilate MLS observations after 2017.

How Does Cloud Overlap Affect the Radiative Heating in the Tropical Upper Troposphere/Lower Stratosphere?

AbstractCharacterizing two‐layer cloud systems has historically been difficult. These systems have a strong radiative impact on the composition of and the processes in the upper troposphere‐lower stratosphere (UTLS). Using 4 years of combined spaceborne lidar and radar observations, the radiative impact of two‐layer cloud systems in the tropical UTLS is characterized, and its sensitivity to the properties of top‐ and bottom‐layer clouds is further quantified. Under these overlapping cloud conditions, the bottom‐layer clouds can fully suppress the radiative heating caused by high clouds in the UTLS, by inducing strong longwave cooling. If the vertical separation between the layers is <4 km, the radiative heating of the high cloud changes sign from positive to negative. Furthermore, the radiative effect at the top of the atmosphere is investigated, and it is found that the characteristic net warming by cirrus with ice water path <50 g/m2 is suppressed in the two‐layered system.

Large Anomalies in the Tropical Upper Troposphere Lower Stratosphere (UTLS) Trace Gases Observed during the Extreme 2015–16 El Niño Event by Using Satellite Measurements

It is well reported that the 2015–16 El Niño event is one of the most intense and long lasting events in the 21st century. The quantified changes in the trace gases (Ozone (O3), Carbon Monoxide (CO) and Water Vapour (WV)) in the tropical upper troposphere and lower stratosphere (UTLS) region are delineated using Aura Microwave Limb Sounder (MLS) and Atmosphere Infrared Radio Sounder (AIRS) satellite observations from June to December 2015. Prior to reaching its peak intensity of El Niño 2015–16, large anomalies in the trace gases (O3 and CO) were detected in the tropical UTLS region, which is a record high in the 21st century. A strong decrease in the UTLS (at 100 and 82 hPa) ozone (~200 ppbv) in July-August 2015 was noticed over the entire equatorial region followed by large enhancement in the CO (150 ppbv) from September to November 2015. The enhancement in the CO is more prevalent over the South East Asia (SEA) and Western Pacific (WP) regions where large anomalies of WV in the lower stratosphere are observed in December 2015. Dominant positive cold point tropopause temperature (CPT-T) anomalies (~5 K) are also noticed over the SEA and WP regions from the high-resolution Constellation Observing System for Meteorology, Ionosphere and Climate (COSMIC) Global Position System (GPS) Radio Occultation (RO) temperature profiles. These observed anomalies are explained in the light of dynamics and circulation changes during El Niño.

Evaluation of water vapour assimilation in the tropical upper troposphere and lower stratosphere by a chemical transport model

Abstract. The present analysis deals with one of the most debated aspects of the studies on the upper troposphere/lower stratosphere (UTLS), namely the budget of water vapour (H2O) at the tropical tropopause. Within the French project “Multiscale water budget in the upper troposphere and lower stratosphere in the TROpics” (TRO-pico), a global-scale analysis has been set up based on space-borne observations, models and assimilation techniques. The MOCAGE-VALENTINA assimilation tool has been used to assimilate the Aura Microwave Limb Sounder (MLS) version 3.3 H2O measurements within the 316–5 hPa range from August 2011 to March 2013 with an assimilation window of 1 h. Diagnostics based on observations minus analysis and forecast are developed to assess the quality of the assimilated H2O fields. Comparison with an independent source of H2O measurements in the UTLS based on the space-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) observations and with meteorological ARPEGE analyses is also shown. Sensitivity studies of the analysed fields have been performed by (1) considering periods when no MLS measurements are available and (2) using H2O data from another MLS version (4.2). The studies have been performed within three different spaces in time and space coincidences with MLS (hereafter referred to as MLS space) and MIPAS (MIPAS space) observations and with the model (model space) outputs and at three different levels: 121 hPa (upper troposphere), 100 hPa (tropopause) and 68 hPa (lower stratosphere) in January and February 2012. In the MLS space, the analyses behave consistently with the MLS observations from the upper troposphere to the lower stratosphere. In the model space, the analyses are wetter than the reference atmosphere as represented by ARPEGE and MLS in the upper troposphere (121 hPa) and around the tropopause (100 hPa), but are consistent with MLS and MIPAS in the lower stratosphere (68 hPa). In the MIPAS space, the sensitivity and the vertical resolution of the MIPAS data set at 121 and 100 hPa prevent assessment of the behaviour of the analyses at 121 and 100 hPa, particularly over intense convective areas as the South American, the African and the Maritime continents but, in the lower stratosphere (68 hPa), the analyses are very consistent with MIPAS. Sensitivity studies show the improvement on the H2O analyses in the tropical UTLS when assimilating space-borne measurements of better quality, particularly over the convective areas.

The Influence of Atmospheric Cloud Radiative Effects on the Large-Scale Atmospheric Circulation

Abstract The influence of clouds on the large-scale atmospheric circulation is examined in numerical simulations from an atmospheric general circulation model run with and without atmospheric cloud radiative effects (ACRE). In the extratropics of both hemispheres, the primary impacts of ACRE on the circulation include 1) increases in the meridional temperature gradient and decreases in static stability in the midlatitude upper troposphere, 2) strengthening of the midlatitude jet, 3) increases in extratropical eddy kinetic energy by up to 30%, and 4) increases in precipitation at middle latitudes but decreases at subtropical latitudes. In the tropics, the primary impacts of ACRE include 1) eastward wind anomalies in the tropical upper troposphere–lower stratosphere (UTLS) and 2) reductions in tropical precipitation. The impacts of ACRE on the atmospheric circulation are interpreted in the context of a series of dynamical and physical processes. The changes in the extratropical circulation and precipitation are consistent with the influence of ACRE on the baroclinicity and eddy fluxes of momentum in the extratropical upper troposphere, the changes in the zonal wind in the UTLS with the influence of ACRE on the amplitude of the equatorial planetary waves, and the changes in the tropical precipitation with the energetic constraints on the tropical troposphere. The results make clear that ACRE have a pronounced influence on the atmospheric circulation not only at tropical latitudes, but at extratropical latitudes as well. They highlight the critical importance of correctly simulating ACRE in global climate models.

The SPARC Data Initiative: Comparison of upper troposphere/lower stratosphere ozone climatologies from limb‐viewing instruments and the nadir‐viewing Tropospheric Emission Spectrometer

AbstractWe present the first comprehensive intercomparison of currently available satellite ozone climatologies in the upper troposphere/lower stratosphere (UTLS) (300–70 hPa) as part of the Stratosphere‐troposphere Processes and their Role in Climate (SPARC) Data Initiative. The Tropospheric Emission Spectrometer (TES) instrument is the only nadir‐viewing instrument in this initiative, as well as the only instrument with a focus on tropospheric composition. We apply the TES observational operator to ozone climatologies from the more highly vertically resolved limb‐viewing instruments. This minimizes the impact of differences in vertical resolution among the instruments and allows identification of systematic differences in the large‐scale structure and variability of UTLS ozone. We find that the climatologies from most of the limb‐viewing instruments show positive differences (ranging from 5 to 75%) with respect to TES in the tropical UTLS, and comparison to a “zonal mean” ozonesonde climatology indicates that these differences likely represent a positive bias for p ≤ 100 hPa. In the extratropics, there is good agreement among the climatologies regarding the timing and magnitude of the ozone seasonal cycle (differences in the peak‐to‐peak amplitude of <15%) when the TES observational operator is applied, as well as very consistent midlatitude interannual variability. The discrepancies in ozone temporal variability are larger in the tropics, with differences between the data sets of up to 55% in the seasonal cycle amplitude. However, the differences among the climatologies are everywhere much smaller than the range produced by current chemistry‐climate models, indicating that the multiple‐instrument ensemble is useful for quantitatively evaluating these models.

Evidence for heterogeneous chlorine activation in the tropical UTLS

Abstract. Airborne in-situ observations of ClO in the tropics were made during the TROCCINOX (Aracatuba, Brazil, February 2005) and SCOUT-O3 (Darwin, Australia, November/December 2005) field campaigns. While during most flights significant amounts of ClO (≈10–20 parts per trillion, ppt) were present only in aged stratospheric air, instances of enhanced ClO mixing ratios of up to 40 ppt – significantly exceeding those expected from gas phase chemistry – were observed in air masses of a more tropospheric character. Most of these observations are associated with low temperatures or with the presence of cirrus clouds (often both), suggesting that cirrus ice particles and/or liquid aerosol at low temperatures may promote significant heterogeneous chlorine activation in the tropical upper troposphere lower stratosphere (UTLS). In two case studies, particularly high levels of ClO observed were reproduced by chemistry simulations only under the assumption that significant denoxification had occurred in the observed air. However, to reproduce the ClO observations in these simulations, O3 mixing ratios higher than observed had to be assumed, and at least for one of these flights, a significant denoxification is in contrast to the observed NO levels, suggesting that the coupling of chlorine and nitrogen compounds in the tropical UTLS may not be completely understood.

Technical Note: Measurement of the tropical UTLS composition in presence of clouds using millimetre-wave heterodyne spectroscopy

Abstract. The MARSCHALS (Millimetre-wave Airborne Receiver for Spectroscopic CHaracterisation of Atmospheric Limb-Sounding) project has the general objectives of demonstrating the measurement capabilities of a limb viewing instrument working in the millimetre and sub-millimetre spectral regions (from 294 to 349 GHz) for the study of the Upper Troposphere – Lower Stratosphere (UTLS). MARSCHALS has flown on board the M-55 stratospheric aircraft (Geophysica) in two measurements campaigns. Here we report the results of the analysis of MARSCHALS measurements during the SCOUT-O3 campaign held in Darwin (Australia) in December 2005 obtained with MARC (Millimetre-wave Atmospheric-Retrieval Code). MARSCHALS measured vertical distributions of temperature, water vapour, ozone and nitric acid in the altitude range from 10 to 20 km in presence of clouds that obscure measurements in the middle infrared spectroscopic region. The minimum altitude at which the retrieval has been possible is determined by the high water concentration typical of the tropical region rather than the extensive cloud coverage experienced during the flight. Water has been measured from 10 km to flight altitude (~18 km) with a 10% accuracy, ozone from 14 km to flight altitude with accuracy ranging from 10% to 60%, while the retrieval of nitric acid has been possible with an accuracy not better than 40% only from 16 km to flight altitude due to the low signal to noise ratio of its emission in the analysed spectral region. The results have been validated using measurement made in a less cloudy region by MIPAS-STR, an infrared limb-viewing instrument on board the M-55, during the same flight.