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Lagrangian models are fundamental tools to study atmospheric transport processes and for practical applications such as dispersion modeling for anthropogenic and natural emission sources. However, conducting large-scale Lagrangian transport simulations with millions of air parcels or more can become numerically rather costly. In this study, we assessed the potential of exploiting graphics processing units (GPUs) to accelerate Lagrangian transport simulations. We ported the Massive-Parallel Trajectory Calculations (MPTRAC) model to GPUs using the open accelerator (OpenACC) programming model. The trajectory calculations conducted within the MPTRAC model were fully ported to GPUs, i. e., except for feeding in the meteorological input data and for extracting the particle output data, the code operates entirely on the GPU devices without frequent data transfers between CPU and GPU memory. Model verification, performance analyses, and scaling tests of the MPI/OpenMP/OpenACC hybrid parallelization of MPTRAC were conducted on the JUWELS Booster supercomputer operated by the Jülich Supercomputing Centre, Germany. The JUWELS Booster comprises 3744 NVIDIA A100 Tensor Core GPUs, providing a peak performance of 71.0 PFlop/s. As of June 2021, it is the most powerful supercomputer in Europe and listed among the most energy-efficient systems internationally. For large-scale simulations comprising 108 particles driven by the European Centre for Medium-RangeWeather Forecasts’ ERA5 reanalysis, the performance evaluation showed a maximum speedup of a factor of 16 due to the utilization of GPUs compared to CPU-only runs on the JUWELS Booster. In the large-scale GPU run, about 67% of the runtime is spent on the physics calculations, conducted on the GPUs. Another 15% of the runtime is required for file-I/O, mostly to read the large ERA5 data set from disk. Meteorological data preprocessing on the CPUs also requires about 15% of the runtime. Although this study identified potential for further improvements of the GPU code, we consider the MPTRAC model ready for production runs on the JUWELS Booster in its present form. The GPU code provides a much faster time to solution than the CPU code, which is particularly relevant for near-real-time applications of a Lagrangian transport model. [ABSTRACT FROM AUTHOR]

Measurements of the pollution trace gases ethane (C2H6), ethyne (C2H2), formic acid (HCOOH), and peroxyacetyl nitrate (PAN) were performed in the North Atlantic upper troposphere and lowermost stratosphere (UTLS) region with the airborne limb imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) with high spatial resolution down to cloud top. Observations were made during flights with the German research aircraft HALO (High Altitude and LOng Range Research Aircraft) in the frame of the WISE (Wave -driven ISentropic Exchange) campaign, which was carried out in autumn 2017 from Shannon (Ireland) and Oberpfaffenhofen (Germany). Enhanced volume mixing ratios (VMR) of up to 2.2 ppbv C2H6, 0.2 ppbv C2H2, 0.9 ppbv HCOOH, and 0.4 ppbv PAN were detected during the flight on 13 September 2017 in the upper troposphere and around the tropopause above the British Isles. Since PAN has the longest lifetime of this foursome, elevated quantities of this molecule could be measured even in the lowermost stratosphere (locally up to 14 km). Backward trajectory calculations as well as global three-dimensional CLaMS simulations with artificial tracers of air mass origin have shown that the main sources of the observed pollutant species are forest fires in North America and anthropogenic pollution in South and Southeast Asia uplifted and moved within the Asian monsoon anticyclone (AMA) circulation system. After release from the AMA, these species or their precursor substances are transported by strong tropospheric winds over large distances, depending on their particular atmospheric lifetime of up to months. Observations are compared to simulations with the atmospheric models EMAC (ECHAM5/MESSy Atmospheric Chemistry) and CAMS (Copernicus Atmosphere Monitoring Service). These models are qualitatively able to reproduce the measured VMR enhancements but underestimate the absolute amount of the increase. Increasing the emissions in EMAC by a factor of 2 reduces the disagreement between simulated and measured results and illustrates the importance of the quality of emission databases used in chemical models. [ABSTRACT FROM AUTHOR]

This paper presents measurements of ozone, water vapour and nitric acid 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 two days 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 two days 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 two days. Our results provide direct insight into small-scale dynamics of the UTLS in the Rossby wave breaking region, witch is of great importance to understanding STE and poleward transport in the UTLS. [ABSTRACT FROM AUTHOR]

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 (UT/LS) of the Asian Monsoon Anticyclone (AMA) over northern India, Nepal and Bangladesh. More than hundred events of New Particle Formation (NPF) were observed. In total, more than two hours of flight time were spent under NPF conditions as indicated by the abundant presence of ultrafine aerosols, i.e. with particle diameters dp smaller than 15 nm, which were in-situ detected by means of condensation nuclei counting techniques. Mixing ratios of ultrafine particles (nuf) of up to ~ 50000 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, but nuf remained elevated (~ 300-2000 mg-1) up to altitudes of ~ 17.5 km (θ ≈ 400 K) while under NPF conditions the fraction (f) of submicrometre-sized non-volatile particle residues (dp > 10 nm) remained below 50%. At ~ 12-14 km (θ ≈ 355-365 K) the minimum of f (< 15%) was found, and underneath the median f generally remains below 25%. The persistence of particles at ultrafine sizes is limited to a few hours, mainly due to coagulation, as demonstrated by a numerical simulation. Thus, NPF is detectable only for a limited period of time and the frequency of NPF events observed during StratoClim 2017 underlines the importance of the UT/LS within the AMA as a source region for aerosols. The effective in-situ production of aerosol in the tropopause region and subsequent coagulation and/or condensation likely contribute to the formation and maintenance of the Asian Tropopause Aerosol Layer (ATAL). The observed abundance of NPF-produced ultrafine 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 TTL). Temperature anomalies of more than one Kelvin, as observed with a wavelength of ~ 90 km during a level flight over several hours, could be associated with the NPF process as a possible cause for the increasing supersaturation of the NPF precursor system. The frequency of NPF observed during StratoClim 2017 exceeds all previous NPF detections with COPAS at TTL levels over Brazil, Northern Australia, or West Africa. The observed NPF abundance and productivity of fresh aerosols during StratoClim 2017 indicates that NPF is capable of directly affecting the extent and persistence of the ATAL. [ABSTRACT FROM AUTHOR]

The potential of heterogeneous chlorine activation in the mid-latitude lowermost stratosphere during summer is a matter of debate. The occurrence of heterogeneous chlorine activation through the presence of aerosol particles could cause ozone destruction. This chemical process requires low temperatures and is accelerated by an enhancement of the stratospheric water vapour and sulfate amount. In particular, the conditions present in the lowermost stratosphere during the North American Summer Monsoon season (NAM) are expected to be cold and moist enough for causing the occurrence of heterogeneous chlorine activation. Furthermore, the temperatures, the water vapour mixing ratio and the sulfate aerosol abundance are affected by future climate change and by the potential application of sulfate geoengineering. Hence, both future scenarios could promote this ozone destruction process. We investigate the likelihood for the occurrence of heterogeneous chlorine activation and its impact on ozone in the lowermost stratospheric mixing layer between tropospheric and stratospheric air above central North America (30.6-49.6° N, 72.25-124.75° W) in summer for conditions today, at the mid and at the end of the 21st century. Therefore, the results of the Geoengineering Large Ensemble Simulations (GLENS) for the lowermost stratospheric mixing layer between tropospheric and stratospheric air are considered together with 10 day box-model simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). In GLENS two future scenarios are simulated: the RCP8.5 climate change scenario and a geoengineering scenario, where sulfur is additionally injected in the stratosphere to keep the global mean surface temperature from changing. In the GLENS simulations, the mixing layer will warm and moisten in both future scenarios with a larger effect in the geoengineering scenario. The likelihood for chlorine activation to occur in the mixing layer is highest in the years 2040-2050 if geoengineering is applied, accounting for 3.3%. In comparison, the likelihood for conditions today is 1.0%. At the end of the 21st century, the likelihood of this ozone destruction process to occur decreases. We found that 0.1% of the ozone mixing ratios in the mixing layer above central North America is destroyed for conditions today. A maximum ozone destruction of 0.3% in the mixing layer occurs in the years 2040-2050 if geoengineering is applied. Comparing the southernmost latitude band (30-35° N) and the northernmost latitude band (44-49° N) of the considered region, we found a higher likelihood for the occurrence of heterogeneous chlorine activation in the southernmost latitude band, causing a higher impact on ozone as well. However, the ozone loss process is found to have a minor impact on the mid-latitude ozone column with not more than 0.1 DU today or in the future scenarios. [ABSTRACT FROM AUTHOR]

The South Asian summer monsoon is associated with a large-scale anticyclonic circulation in the Upper Troposphere and Lower Stratosphere (UTLS), which confines the air mass inside. During boreal summer, the confinement of this air mass leads to an accumulation of aerosol between about 13 km and 18 km (360 K and 440 K potential temperature), this accumulation of aerosol constitutes the Asian Tropopause Aerosol Layer (ATAL). We present balloon-borne aerosol backscatter measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) instrument in Nainital in Northern India in August 2016, and compare these with COBALD measurements in the post-monsoon time in November 2016. The measurements demonstrate a strong variability of the ATAL's altitude, vertical extent, aerosol backscatter intensity and cirrus cloud occurrence frequency. Such a variability cannot be deduced from climatological means of the ATAL as they are derived from satellite measurements. To explain this observed variability we performed a Lagrangian back-trajectory analysis using the Chemical Lagrangian Model of the Stratosphere (CLaMS). We identify the transport pathways of air parcels contributing to the ATAL over Nainital in August 2016, as well as the source regions of the air masses contributing to the composition of the ATAL. Our analysis reveals a variety of factors contributing to the observed day-to-day variability of the ATAL: continental convection, tropical cyclones (maritime convection), dynamics of the anticyclone and stratospheric intrusions. Thus, the ATAL is a mixture of air masses coming from different atmospheric height layers. In addition, contributions from the model boundary layer originate in different geographic source regions. The location of strongest updraft along the backward trajectories reveal a cluster of strong upward transport at the southern edge of the Himalayan foothills. From the top of the convective outflow level (about 13 km; 360 K) the air parcels ascend slowly to ATAL altitudes within a large-scale upward spiral driven by the diabatic heating in the anticyclonic flow of the South Asian summer monsoon at UTLS altitudes. Cases with a strong ATAL typically show boundary layer contributions from the Tibetan Plateau, the foothills of the Himalayas and other continental regions below the Asian monsoon. Weaker ATAL cases show higher contributions from the maritime boundary layer, often related to tropical cyclones, indicating a mixing of unpolluted and polluted air masses. Because of the strong growth of Asian economies, increasing anthropogenic emissions in the future are expected to enhance the thickness and intensity of the ATAL, thereby also enhancing the global stratospheric aerosol loading, which likely impacts surface climate. [ABSTRACT FROM AUTHOR]