Upper Troposphere/lower Stratosphere Research Articles

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.

Water Vapor in the Asian Summer Monsoon Anticyclone: Comparison of Balloon‐Borne Measurements and ECMWF Data

AbstractWater vapor (H2O) is the strongest greenhouse gas in our atmosphere. Hence, accurate measurements and a correct representation in global models of H2O in the upper troposphere/lower stratosphere (UTLS) are important for understanding and projecting climate. Here we compare balloon‐borne measurements of UTLS H2O, performed by cryogenic frostpoint hygrometers (CFH) and meteorological radiosondes (Vaisala RS41) during two intensive field campaigns in the Asian summer monsoon anticyclone region, with humidity data from three products of the European Centre for Medium‐range Weather Forecasts (ECMWF): operational analysis and forecast (termed OPERA), ERA‐Interim reanalysis, and the newly released ERA5 reanalysis. Taking CFH as a reference, we show that OPERA and ERA5 provide a more accurate representation of UTLS H2O than ERA‐Interim. In particular, OPERA and ERA5 similarly overestimate H2O mixing ratios by on average 0.7–0.8 ppmv (14–15%) and 0.7–0.9 ppmv (15–17%) at pressures 60–100 hPa, respectively, and both provide a good representation of the observed vertical distribution (including fine structures) and natural variability of UTLS H2O. In contrast, ERA‐Interim underestimates UTLS H2O by 0.6–1.7 ppmv (14–30%), and it fails to capture relevant features of the vertical distribution of UTLS H2O. At pressures (p) lower than 60 hPa, all three ECMWF products are in good agreement with CFH. Humidity measurements by RS41 show an average dry bias of 0.1–0.5 ppmv (3–9%) compared to CFH for 60–100 hPa, and a moist bias increasing with altitude for p < 60 hPa, exceeding 100% for p < 40 hPa.

Observational evidence of particle hygroscopic growth in the upper troposphere–lower stratosphere (UTLS) over the Tibetan Plateau

Abstract. We measured the vertical profiles of backscatter ratio (BSR) using the balloon-borne, lightweight Compact Optical Backscatter AerosoL Detector (COBALD) instruments above Linzhi, located in the southeastern Tibetan Plateau, in the summer of 2014. An enhanced aerosol layer in the upper troposphere–lower stratosphere (UTLS), with BSR (455 nm) > 1.1 and BSR (940 nm) > 1.4, was observed. The color index (CI) of the enhanced aerosol layer, defined as the ratio of aerosol backscatter ratios (ABSRs) at wavelengths of 940 and 455 nm, varied from 4 to 8, indicating the prevalence of fine particles with a mode radius of less than 0.1 µm. We find that unlike the very small particles (mode radius smaller than 0.04 µm) at low relative humidity (RHi < 40 %), the relatively large particles in the aerosol layer were generally very hydrophilic as their size increased dramatically with relative humidity. This result indicates that water vapor can play a very important role in increasing the size of fine particles in the UTLS over the Tibetan Plateau. Our observations provide observation-based evidence supporting the idea that aerosol particle hygroscopic growth is an important factor influencing the radiative properties of the Asian Tropopause Aerosol Layer (ATAL) during the Asian summer monsoon.

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.

Tropospheric water vapor profiles obtained with FTIR: comparison with balloon-borne frost point hygrometers and influence on trace gas retrievals

Abstract. Retrievals of vertical profiles of key atmospheric gases provide a critical long-term record from ground-based Fourier transform infrared (FTIR) solar absorption measurements. However, the characterization of the retrieved vertical profile structure can be difficult to validate, especially for gases with large vertical gradients and spatial–temporal variability such as water vapor. In this work, we evaluate the accuracy of the most common water vapor isotope (H216O, hereafter WV) FTIR retrievals in the lower and upper troposphere–lower stratosphere. Coincident high-quality vertically resolved WV profile measurements obtained from 2010 to 2016 with balloon-borne NOAA frost point hygrometers (FPHs) are used as reference to evaluate the performance of the retrieved profiles at two sites: Boulder (BLD), Colorado, and at the mountaintop observatory of Mauna Loa (MLO), Hawaii. For a meaningful comparison, the spatial–temporal variability has been investigated. We present results of comparisons among FTIR retrievals with unsmoothed and smoothed FPH profiles to assess WV vertical gradients. Additionally, we evaluate the quantitative impact of different a priori profiles in the retrieval of WV. An orthogonal linear regression analysis shows the best correlation among tropospheric layers using ERA-Interim (ERA-I) a priori profiles and biases are lower for unsmoothed comparisons. In Boulder, we found a negative bias of 0.02±1.9 % (r=0.95) for the 1.5–3 km layer. A larger negative bias of 11.1±3.5 % (r=0.97) was found in the lower free troposphere layer of 3–5 km attributed to rapid vertical change of WV, which is not always captured by the retrievals. The bias improves in the 5–7.5 km layer (1.0±5.3 %, r=0.94). The bias remains at about 13 % for layers above 7.5 km but below 13.5 km. At MLO the spatial mismatch is significantly larger due to the launch of the sonde being farther from the FTIR location. Nevertheless, we estimate a negative bias of 5.9±4.6 % (r=0.93) for the 3.5–5.5 km layer and 9.9±3.7 % (r=0.93) for the 5.5–7.5 km layer, and we measure positive biases of 6.2±3.6 % (r=0.95) for the 7.5–10 km layer and 12.6 % and greater values above 10 km. The agreement for the first layer is significantly better at BLD because the air masses are similar for both FTIR and FPH. Furthermore, for the first time we study the influence of different WV a priori profiles in the retrieval of selected gas profiles. Using NDACC standard retrievals we present results for hydrogen cyanide (HCN), carbon monoxide (CO), and ethane (C2H6) by taking NOAA FPH profiles as the ground truth and evaluating the impact of other WV profiles. We show that the effect is minor for C2H6 (bias <0.5 % for all WV sources) among all vertical layers. However, for HCN we found significant biases between 6 % for layers close to the surface and 2 % for the upper troposphere depending on the WV profile source. The best results (reduced bias and precision and r values closer to unity) are always found for pre-retrieved WV. Therefore, we recommend first retrieving WV to use in subsequent retrieval of gases.

Source apportionment of rainwater chemical composition to investigate the transport of lower atmospheric pollutants to the UTLS region

Efforts to understand the chemical composition of Asian Tropopause Aerosol Layer (ATAL) in the Upper Troposphere Lower Stratosphere (UTLS) region have revealed the dominance of nitrates in the samples collected from ATAL layer during the recent balloon campaigns. Potential sources have been thought to be in-situ formation, convective uplift and long-range transport. Rainwater chemical composition consists water-soluble chemical ions that are wet scavenged during rain events and gives an indirect indication of lower atmospheric pollutants. Keeping this in focus, total monsoon precipitation chemistry at Gadanki (13.5°N, 79.2°E) has been studied to understand the convective uplift possibilities to the UTLS region. About 32 rainwater samples collected during July to December 2017 were analysed for their chemical composition using Ion Chromatography. Total 16 ions comprising of 5 anions (F−, Cl−, NO3−, SO42− and PO43−), 6 cations (Na+, K+, Ca2+, Mg2+, Li+ and NH4+) and 5 trace metals (Cd2+, Ni2+, Co2+, Mn2+ and Zn2+) have been detected in different rainwater samples. Rainwater chemical composition data has been subjected to the Principal Component Analysis (PCA) to understand the correlations between different chemical species and to identify the possible sources of origin qualitatively. It has been observed that the chemical composition of the rainwater is very different from the chemical composition of the ATAL layer indicating non-existence of convective transport of lower level pollutants to the UTLS region at Gadanki. This observation is also well supported by the vertical distribution of CALIPSO derived aerosol types and ERA interim vertical pressure velocities during the sampling period.

QBO Influence on MJO Amplitude over the Maritime Continent: Physical Mechanisms and Seasonality

AbstractThe quasi-biennial oscillation (QBO) is stratified by stratospheric zonal wind direction and height into four phase pairs [easterly midstratospheric winds (QBOEM), easterly lower-stratospheric winds, westerly midstratospheric winds (QBOWM), and westerly lower-stratospheric winds] using an empirical orthogonal function analysis of daily stratospheric (100–10 hPa) zonal wind data during 1980–2017. Madden–Julian oscillation (MJO) events in which the MJO convective envelope moved eastward across the Maritime Continent (MC) during 1980–2017 are identified using the Real-time Multivariate MJO (RMM) index and the outgoing longwave radiation (OLR) MJO index (OMI). Comparison of RMM amplitudes by the QBO phase pair over the MC (RMM phases 4 and 5) reveals that boreal winter MJO events have the strongest amplitudes during QBOEM and the weakest amplitudes during QBOWM, which is consistent with QBO-driven differences in upper-tropospheric lower-stratospheric (UTLS) static stability. Additionally, boreal winter RMM events over the MC strengthen during QBOEM and weaken during QBOWM. In the OMI, those amplitude changes generally shift eastward to the eastern MC and western Pacific Ocean, which may result from differences in RMM and OMI index methodologies. During boreal summer, as the northeastward-propagating boreal summer intraseasonal oscillation (BSISO) becomes the dominant mode of intraseasonal variability, these relationships are reversed. Zonal differences in UTLS stability anomalies are consistent with amplitude changes of eastward-propagating MJO events across the MC during boreal winter, and meridional stability differences are consistent with amplitude changes of northeastward-propagating BSISO events during boreal summer. Results remain consistent when stratifying by neutral ENSO phase.

Attributing differences in the fate of lateral boundary ozone in AQMEII3 models to physical process representations.

Increasing emphasis has been placed on characterizing the contributions and the uncertainties of ozone imported from outside the US. In chemical transport models (CTMs), the ozone transported through lateral boundaries (referred to as LB ozone hereafter) undergoes a series of physical and chemical processes in CTMs, which are important sources of the uncertainty in estimating the impact of LB ozone on ozone levels at the surface. By implementing inert tracers for LB ozone, the study seeks to better understand how differing representations of physical processes in regional CTMs may lead to differences in the simulated LB ozone that eventually reaches the surface across the US. For all the simulations in this study (including WRF/CMAQ, WRF/CAMx, COSMO-CLM/CMAQ, and WRF/DEHM), three chemically inert tracers that generally represent the altitude ranges of the planetary boundary layer (BC1), free troposphere (BC2), and upper troposphere-lower stratosphere (BC3) are tracked to assess the simulated impact of LB specification. Comparing WRF/CAMx with WRF/CMAQ, their differences in vertical grid structure explain 10 %-60 % of their seasonally averaged differences in inert tracers at the surface. Vertical turbulent mixing is the primary contributor to the remaining differences in inert tracers across the US in all seasons. Stronger vertical mixing in WRF/CAMx brings more BC2 downward, leading to higher BCT (BCT = BC1+BC2+BC3) and BC2/BCT at the surface in WRF/CAMx. Meanwhile, the differences in inert tracers due to vertical mixing are partially counteracted by their difference in sub-grid cloud mixing over the southeastern US and the Gulf Coast region during summer. The process of dry deposition adds extra gradients to the spatial distribution of the differences in DM8A BCT by 5-10 ppb during winter and summer. COSMO-CLM/CMAQ and WRF/CMAQ show similar performance in inert tracers both at the surface and aloft through most seasons, which suggests similarity between the two models at process level. The largest difference is found in summer. Sub-grid cloud mixing plays a primary role in their differences in inert tracers over the southeastern US and the oceans in summer. Our analysis of the vertical profiles of inert tracers also suggests that the model differences in dry deposition over certain regions are offset by the model differences in vertical turbulent mixing, leading to small differences in inert tracers at the surface in these regions.

Balloon-borne measurements of temperature, water vapor, ozone and aerosol backscatter on the southern slopes of the Himalayas during StratoClim 2016–2017

Abstract. The Asian summer monsoon anticyclone (ASMA) is a major meteorological system of the upper troposphere–lower stratosphere (UTLS) during boreal summer. It is known to contain enhanced tropospheric trace gases and aerosols, due to rapid lifting from the boundary layer by deep convection and subsequent horizontal confinement. Given its dynamical structure, the ASMA represents an efficient pathway for the transport of pollutants to the global stratosphere. A detailed understanding of the thermal structure and processes in the ASMA requires accurate in situ measurements. Within the StratoClim project we performed state-of-the-art balloon-borne measurements of temperature, water vapor, ozone and aerosol backscatter from two stations on the southern slopes of the Himalayas. In total, 63 balloon soundings were conducted during two extensive monsoon-season campaigns, in August 2016 in Nainital, India (29.4∘ N, 79.5∘ E), and in July–August 2017 in Dhulikhel, Nepal (27.6∘ N, 85.5∘ E); one shorter post-monsoon campaign was also carried out in November 2016 in Nainital. These measurements provide unprecedented insights into the UTLS thermal structure, the vertical distributions of water vapor, ozone and aerosols, cirrus cloud properties and interannual variability in the ASMA. Here we provide an overview of all of the data collected during the three campaign periods, with focus on the UTLS region and the monsoon season. We analyze the vertical structure of the ASMA in terms of significant levels and layers, identified from the temperature and potential temperature lapse rates and Lagrangian backward trajectories, which provides a framework for relating the measurements to local thermodynamic properties and the large-scale anticyclonic flow. Both the monsoon-season campaigns show evidence of deep convection and confinement extending up to 1.5–2 km above the cold-point tropopause (CPT), yielding a body of air with high water vapor and low ozone which is prone to being lifted further and mixed into the free stratosphere. Enhanced aerosol backscatter also reveals the signature of the Asian tropopause aerosol layer (ATAL) over the same region of altitudes. The Dhulikhel 2017 campaign was characterized by a 5 K colder CPT on average than in Nainital 2016 and a local water vapor maximum in the confined lower stratosphere, about 1 km above the CPT. Data assessment and modeling studies are currently ongoing with the aim of fully exploring this dataset and its implications with respect to stratospheric moistening via the ASMA system and related processes.

The Simulation of Stratospheric Water Vapor over the Asian Summer Monsoon Region in CESM1(WACCM) Models.

Previous observational studies have found a persistent maximum in stratospheric water vapor (SWV) in the upper troposphere lower stratosphere (UTLS) confined by the upper-level anticyclone over the Asian summer monsoon region. This study investigates the simulation of SWV in the Whole Atmosphere Community Climate Model (WACCM). WACCM generally tends to simulate a SWV maximum over the central Pacific Ocean, but this bias is largely improved in the high vertical resolution version. The high vertical resolution model with increased vertical layers in the UTLS is found to have a less stratified UTLS over the central Pacific Ocean compared with the low vertical resolution model. It therefore simulates a steepened PV gradient over the central Pacific Ocean that better closes the upper-level anticyclone and confines the SWV within the enhanced transport barrier.

Trapped Gravity Waves and Their Association with Turbulence in a Large Thunderstorm Anvil during PECAN

Abstract Geostationary Operational Environmental Satellite-14 (GOES-14) 1-km visible satellite data with 1-min frequency revealed horizontally propagating internal gravity waves emanating from tropopause-penetrating deep convection on 3–4 June 2015 during the Plains Elevated Convection at Night (PECAN) field experiment. These waves had horizontal wavelengths of ~6–8 km and approximate ground-relative phase speeds of 35 m s−1. PECAN radiosonde data are used to document the environment supporting the horizontally propagating gravity waves within the 200-km-long downstream thunderstorm anvil. Comparisons among soundings within the anvil core, at the downstream anvil edge, and outside of the anvil, together with supporting high-resolution numerical simulations, establish the importance of the storm-induced upper-tropospheric/lower-stratospheric (UTLS) outflow in providing conditions allowing vertical trapping of internal gravity waves over large horizontal distances within the mesoscale anvil. Turbulence was reported by commercial aviation in proximity to the gravity waves near the downstream anvil edge. The simulations suggest that the strongest turbulence was consistent with a mesoscale destabilization of the outer portion of the downstream anvil at elevations immediately below the outflow jet, where differential temperature advection owing to the strong associated vertical shear reduces static stability. The simulated gravity waves are trapped at this elevation and extend for several kilometers below. Local minima of moist gradient Richardson number occur immediately above the simulated warm gravity wave temperature perturbations at anvil base, suggesting a possible role these waves could play in establishing precise locations for the onset of turbulence.

The MUSICA IASI CH<sub>4</sub> and N<sub>2</sub>O products and their comparison to HIPPO, GAW and NDACC FTIR references

Abstract. This work presents the methane (CH4) and nitrous oxide (N2O) products as generated by the IASI (Infrared Atmospheric Sounding Interferometer) processor developed during the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water). The processor retrieves CH4 and N2O with different water vapour and water vapour isotopologues (as well as HNO3) and uses a single a priori data set for all the retrievals (no variation in space and time). Firstly, the characteristics and errors of the products are analytically described. Secondly, the products are comprehensively evaluated by comparisons to the following reference data measured by different techniques and from different platforms as follows: (1) aircraft CH4 and N2O profiles from the five HIAPER Pole-to-Pole Observation (HIPPO) missions; (2) continuous in situ CH4 and N2O observations performed between 2007 and 2017 at subtropical and mid-latitude high-mountain observatories (Izaña Atmospheric Observatory and Jungfraujoch, respectively) in the framework of the WMO–GAW (World Meteorological Organization–Global Atmosphere Watch) programme; (3) ground-based FTIR (Fourier-transform infrared spectrometer) measurements made between 2007 and 2017 in the framework of the NDACC (Network for the Detection of Atmospheric Composition Change) at the subtropical Izaña Atmospheric Observatory, the mid-latitude station of Karlsruhe and the Kiruna polar site.The theoretical estimations and the comparison studies suggest a precision for the N2O and CH4 retrieval products of about 1.5–3 % and systematic errors due to spectroscopic parameters of about 2 %. The MUSICA IASI CH4 data offer a better sensitivity than N2O data. While for the latter the sensitivity is mainly limited to the UTLS (upper troposphere–lower stratosphere) region, for CH4 we are able to prove that at low latitudes the MUSICA IASI processor can detect variations that take place in the free troposphere independently from the variations in the UTLS region. We demonstrate that the MUSICA IASI data qualitatively capture the CH4 gradients between low and high latitudes and between the Southern Hemisphere and Northern Hemisphere; however, we also find an inconsistency between low- and high-latitude CH4 data of up to 5 %. The N2O latitudinal gradients are very weak and cannot be detected. We make comparisons over a 10-year time period and analyse the agreement with the reference data on different timescales. The MUSICA IASI data can detect day-to-day signals (only in the UTLS), seasonal cycles and long-term evolution (in the UTLS and for CH4 also in the free troposphere) similar to the reference data; however, there are also inconsistencies in the long-term evolution connected to inconsistencies in the used atmospheric temperature a priori data.Moreover, we present a method for analytically describing the a posteriori-calculated logarithmic-scale difference of the CH4 and N2O retrieval estimates. By correcting errors that are common in the CH4 and N2O retrieval products, the a posteriori-calculated difference can be used for generating an a posteriori-corrected CH4 product with a theoretically better precision than the original CH4 retrieval products. We discuss and evaluate two different approaches for such a posteriori corrections. It is shown that the correction removes the inconsistencies between low and high latitudes and enables the detection of day-to-day signals also in the free troposphere. Furthermore, they reduce the impact of short-term atmospheric dynamics, which is an advantage, because respective signals are presumably hardly comparable to model data. The approach that affects the correction solely on the scales on which the errors dominate is identified as the most efficient, because it reduces the inconsistencies and errors without removing measurable real atmospheric signals. We give a brief outlook on a possible usage of this a posteriori-corrected MUSICA IASI CH4 product in combination with inverse modelling.

Influence of the wintertime North Atlantic Oscillation on European tropospheric composition: an observational and modelling study

Abstract. We have used satellite observations and a simulation from the TOMCAT chemistry transport model (CTM) to investigate the influence of the well-known wintertime North Atlantic Oscillation (NAO) on European tropospheric composition. Under the positive phase of the NAO (NAO-high), strong westerlies tend to enhance transport of European pollution (e.g. nitrogen oxides, NOx; carbon monoxide, CO) away from anthropogenic source regions. In contrast, during the negative phase of the NAO (NAO-low), more stable meteorological conditions lead to a build-up of pollutants over these regions relative to the wintertime average pollution levels. However, the secondary pollutant ozone shows the opposite signal of larger values during NAO-high. NAO-high introduces Atlantic ozone-enriched air into Europe, while under NAO-low westerly transport of ozone is reduced, yielding lower values over Europe. Furthermore, ozone concentrations are also decreased by chemical loss through the reaction with accumulated primary pollutants such as nitric oxide (NO) in NAO-low. Peroxyacetyl nitrate (PAN) in the upper troposphere–lower stratosphere (UTLS) peaks over Iceland and southern Greenland in NAO-low, between 200 and 100 hPa, consistent with the trapping by an anticyclone at this altitude. Model simulations show that enhanced PAN over Iceland and southern Greenland in NAO-low is associated with vertical transport of polluted air from the mid-troposphere into the UTLS. Overall, this work shows that NAO circulation patterns are an important governing factor for European wintertime composition and air pollution.

Characterizing Global Ozonesonde Profile Variability from Surface to the UT/LS with a Clustering Technique and MERRA-2 Reanalysis.

Our previous studies employing the self-organizing map (SOM) clustering technique to ozonesonde data have found significant links among meteorological and chemical regimes, and the shape of the ozone (O3) profile from the troposphere to the lower stratosphere. These studies, which focused on specific northern hemisphere mid-latitude geographical regions, demonstrated the advantages of SOM clustering by quantifying O3 profile variability and the O3/meteorological correspondence. We expand SOM to a global set of ozonesonde profiles spanning 1980-present from 30 sites to summarize the connections among O3 profiles, meteorology, and chemistry, using the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) reanalysis and other ancillary data. Four clusters of O3 mixing ratio profiles from the surface to the upper troposphere/lower stratosphere (UT/LS) are generated for each site, which show dominant profile shapes and typical seasonality (or lack thereof) that generally correspond to latitude (i.e. Tropical, Subtropical, Mid-Latitude, Polar). Examination of MERRA-2 output reveals a clear relationship among SOM clusters and covarying meteorological fields (geopotential height, potential vorticity, and tropopause height) for Polar and Mid-latitude sites. However, these relationships break down within ±30° latitude. Carbon monoxide satellite data, along with velocity potential, a proxy for convection, calculated from MERRA-2 wind fields assist characterization of the Tropical and Subtropical sites, where biomass burning and convective transport linked to the Madden-Julian Oscillation (MJO) dominate O3 variability. In addition to geophysical characterization of O3 profile variability, these results can be used to evaluate chemical transport model output and satellite measurements of O3.

Climatology and long-term evolution of ozone and carbon monoxide in the upper troposphere–lower stratosphere (UTLS) at northern midlatitudes, as seen by IAGOS from 1995 to 2013

Abstract. In situ measurements in the upper troposphere–lower stratosphere (UTLS) have been performed in the framework of the European research infrastructure IAGOS (In-service Aircraft for a Global Observing System) for ozone since 1994 and for carbon monoxide (CO) since 2002. The flight tracks cover a wide range of longitudes in the northern extratropics, extending from the North American western coast (125° W) to the eastern Asian coast (135° E) and more recently over the northern Pacific Ocean. Several tropical regions are also sampled frequently, such as the Brazilian coast, central and southern Africa, southeastern Asia, and the western half of the Maritime Continent. As a result, a new set of climatologies for O3 (August 1994–December 2013) and CO (December 2001–December 2013) in the upper troposphere (UT), tropopause layer, and lower stratosphere (LS) are made available, including gridded horizontal distributions on a semi-global scale and seasonal cycles over eight well-sampled regions of interest in the northern extratropics. The seasonal cycles generally show a summertime maximum in O3 and a springtime maximum in CO in the UT, in contrast to the systematic springtime maximum in O3 and the quasi-absence of a seasonal cycle of CO in the LS. This study highlights some regional variabilities in the UT, notably (i) a west–east difference of O3 in boreal summer with up to 15 ppb more O3 over central Russia compared with northeast America, (ii) a systematic west–east gradient of CO from 60 to 140° E, especially noticeable in spring and summer with about 5 ppb by 10 degrees longitude, (iii) a broad spring/summer maximum of CO over northeast Asia, and (iv) a spring maximum of O3 over western North America. Thanks to almost 20 years of O3 and 12 years of CO measurements, the IAGOS database is a unique data set to derive trends in the UTLS at northern midlatitudes. Trends in O3 in the UT are positive and statistically significant in most regions, ranging from +0.25 to +0.45 ppb yr−1, characterized by the significant increase in the lowest values of the distribution. No significant trends of O3 are detected in the LS. Trends of CO in the UT, tropopause, and LS are almost all negative and statistically significant. The estimated slopes range from −1.37 to −0.59 ppb yr−1, with a nearly homogeneous decrease in the lowest values of the monthly distribution (5th percentile) contrasting with the high interregional variability in the decrease in the highest values (95th percentile).

Variability and trend in ozone over the southern tropics and subtropics

Abstract. Long-term variability in ozone trends was assessed over eight Southern Hemisphere tropical and subtropical sites (Natal, Nairobi, Ascension Island, Java, Samoa, Fiji, Reunion and Irene), using total column ozone data (TCO) and vertical ozone profiles (altitude range 15–30 km) recorded during the period January 1998–December 2012. The TCO datasets were constructed by combination of satellite data (OMI and TOMS) and ground-based observations recorded using Dobson and SAOZ spectrometers. Vertical ozone profiles were obtained from balloon-sonde experiments which were operated within the framework of the SHADOZ network. The analysis in this study was performed using the Trend-Run model. This is a multivariate regression model based on the principle of separating the variations of ozone time series into a sum of several forcings (annual and semi-annual oscillations, QBO (Quasi-Biennial Oscillation), ENSO, 11-year solar cycle) that account for most of its variability. The trend value is calculated based on the slope of a normalized linear function which is one of the forcing parameters included in the model. Three regions were defined as follows: equatorial (0–10∘ S), tropical (10–20∘ S) and subtropical (20–30∘ S). Results obtained indicate that ozone variability is dominated by seasonal and quasi-biennial oscillations. The ENSO contribution is observed to be significant in the tropical lower stratosphere and especially over the Pacific sites (Samoa and Java). The annual cycle of ozone is observed to be the most dominant mode of variability for all the sites and presents a meridional signature with a maximum over the subtropics, while semi-annual and quasi-biannual ozone modes are more apparent over the equatorial region, and their magnitude decreases southward. The ozone variation mode linked to the QBO signal is observed between altitudes of 20 and 28 km. Over the equatorial zone there is a strong signal at ∼26 km, where 58 % ±2 % of total ozone variability is explained by the effect of QBO. Annual ozone oscillations are more apparent at two different altitude ranges (below 24 km and in the 27–30 km altitude band) over the tropical and subtropical regions, while the semi-annual oscillations are more significant over the 27–30 km altitude range in the tropical and equatorial regions. The estimated trend in TCO is positive and not significant and corresponds to a variation of ∼1.34±0.50 % decade−1 (averaged over the three regions). The trend estimated within the equatorial region (0–15∘ S) is less than 1 % per decade, while it is assessed at more than 1.5 % decade−1 for all the sites located southward of 17∘ S. With regard to the vertical distribution of trend estimates, a positive trend in ozone concentration is obtained in the 22–30 km altitude range, while a delay in ozone improvement is apparent in the UT–LS (upper troposphere–lower stratosphere) below 22 km. This is especially noticeable at approximately 19 km, where a negative value is observed in the tropical regions.

Mountain waves modulate the water vapor distribution in the UTLS

Abstract. The water vapor distribution in the upper troposphere–lower stratosphere (UTLS) region has a strong impact on the atmospheric radiation budget. Transport and mixing processes on different scales mainly determine the water vapor concentration in the UTLS. Here, we investigate the effect of mountain waves on the vertical transport and mixing of water vapor. For this purpose we analyze measurements of water vapor and meteorological parameters recorded by the DLR Falcon and NSF/NCAR Gulfstream V research aircraft taken during the Deep Propagating Gravity Wave Experiment (DEEPWAVE) in New Zealand. By combining different methods, we develop a new approach to quantify location, direction and irreversibility of the water vapor transport during a strong mountain wave event on 4 July 2014. A large positive vertical water vapor flux is detected above the Southern Alps extending from the troposphere to the stratosphere in the altitude range between 7.7 and 13.0 km. Wavelet analysis for the 8.9 km altitude level shows that the enhanced upward water vapor transport above the mountains is caused by mountain waves with horizontal wavelengths between 22 and 60 km. A downward transport of water vapor with 22 km wavelength is observed in the lee-side of the mountain ridge. While it is a priori not clear whether the observed fluxes are irreversible, low Richardson numbers derived from dropsonde data indicate enhanced turbulence in the tropopause region related to the mountain wave event. Together with the analysis of the water vapor to ozone correlation, we find indications for vertical transport followed by irreversible mixing of water vapor. For our case study, we further estimate greater than 1 W m−2 radiative forcing by the increased water vapor concentrations in the UTLS above the Southern Alps of New Zealand, resulting from mountain waves relative to unperturbed conditions. Hence, mountain waves have a great potential to affect the water vapor distribution in the UTLS. Our regional study may motivate further investigations of the global effects of mountain waves on the UTLS water vapor distributions and its radiative effects.

Understanding the Time Scales of the Tropospheric Circulation Response to Abrupt CO2 Forcing in the Southern Hemisphere: Seasonality and the Role of the Stratosphere

This study examines the time scales of the Southern Hemisphere (SH) tropospheric circulation response to increasing atmospheric CO2 concentrations in models from phase 5 of the Coupled Model Intercomparison Project (CMIP5). In response to an abrupt quadrupling of atmospheric CO2, the midlatitude jet stream and poleward edge of the Hadley circulation shift poleward on the time scale of the rising global-mean surface temperature during the summer and fall seasons but on a much more rapid time scale during the winter and spring seasons. The seasonally varying time scales of the SH circulation response are closely tied to the meridional temperature gradient in the upper troposphere–lower stratosphere and, in particular, to temperatures in the SH polar lower stratosphere. During summer and fall, SH polar lower-stratospheric temperatures cool on the time scale of warming global surface temperatures, as the lifting of the tropopause height with tropospheric warming is associated with cooling at lower-stratospheric levels. However, during winter and spring, SH polar lower-stratospheric temperatures cool primarily from fast time-scale radiative processes, contributing to the faster time-scale circulation response during these seasons. The poleward edge of the SH subtropical dry zone shifts poleward on the time scale of the rising global-mean surface temperature during all seasons in response to an abrupt quadrupling of atmospheric CO2. The dry zone edge initially follows the poleward shift in the Hadley cell edge but is then augmented by the action of eddy moisture fluxes in a warming climate. Consequently, with increasing atmospheric CO2 concentrations, key features of the tropospheric circulation response could emerge sooner than features more closely tied to rising global temperatures.

Relation between geomagnetic field and climate variability. Part 2: Probable mechanism

In this study we show that correspondence of the main structures of geomagnetic field, near surface air temperature and surface pressure in the mid-latitudes, reported previously in the 1st part of the paper, has its physical foundation. The similar pattern, found in latitude-longitude distribution of the lower stratospheric ozone and specific humidity, allows us to close the chain of causal links, and to offer a mechanism through which geomagnetic field could influence on the Earth’s climate. It starts with a geomagnetic modulation of galactic cosmic rays (GCR) and ozone production in the lower stratosphere through ion-molecular reactions initiated by GCR. The alteration of the near tropopause temperature (by O3 variations at these levels) changes the amount of water vapour in the driest part of the upper troposphere/lower stratosphere (UTLS), influencing in such a way on the radiation balance of the planet. This forcing on the climatic parameters is non-uniformly distributed over the globe, due to the heterogeneous geomagnetic field controlling energetic particles entering the Earth’s atmosphere.