Abstract. Ammonium-nitrate aerosols are expected to become more important in the future atmosphere due to the expected increase in nitrate precursor emissions and the decline of ammonium-sulphate aerosols in wide regions of this planet. The GISS climate model is used in this study, including atmospheric gas- and aerosol phase chemistry to investigate current and future (2030, following the SRES A1B emission scenario) atmospheric compositions. A set of sensitivity experiments was carried out to quantify the individual impact of emission- and physical climate change on nitrate aerosol formation. We found that future nitrate aerosol loads depend most strongly on changes that may occur in the ammonia sources. Furthermore, microphysical processes that lead to aerosol mixing play a very important role in sulphate and nitrate aerosol formation. The role of nitrate aerosols as climate change driver is analyzed and set in perspective to other aerosol and ozone forcings under pre-industrial, present day and future conditions. In the near future, year 2030, ammonium nitrate radiative forcing is about –0.14 W/m2 and contributes roughly 10% of the net aerosol and ozone forcing. The present day nitrate and pre-industrial nitrate forcings are –0.11 and –0.05 W/m2, respectively. The steady increase of nitrate aerosols since industrialization increases its role as a non greenhouse gas forcing agent. However, this impact is still small compared to greenhouse gas forcings, therefore the main role nitrate will play in the future atmosphere is as an air pollutant, with annual mean near surface air concentrations rising above 3 μg/m3 in China and therefore reaching pollution levels, like sulphate aerosols, in the fine particle mode.
<p>The Integrated Forecasting System (IFS) of ECMWF is used within the Copernicus Atmosphere Monitoring Service (CAMS) to provide global analyses and forecasts of atmospheric composition, including aerosols as well as reactive trace gases and greenhouse gases.</p><p>The aerosol model of the IFS, IFS-AER, is a simple sectional-bulk scheme that forecasts seven species: &#160;dust, sea-salt, black carbon, organic matter, sulfate, and &#160;since July 2019, nitrate and ammonium. &#160;The main developments that have been recently carried out, tested and are now contemplated for implementation in the next operational version (known as cycle 48r1) are presented here.</p><p>The dry deposition velocities are computed as a function of roughness length, particle size and surface friction velocity, while wet deposition depends mainly on the precipitation fluxes. The parameterizations of both dry and wet deposition have been upgraded with more recent schemes, which have been shown to improve the simulated deposition fluxes for several aerosol species. The impact of this upgrade on the skill scores of simulated aerosol optical depth (AOD) and surface particulate matter concentrations against a range of observations is very positive.</p><p>The simulated surface concentration of nitrate and ammonium are frequently strongly overestimated over Europe and the &#160;United States in the current version of the IFS. Nitrate, ammonium, and their precursors nitric acid and ammonia, were evaluated against a range of ground and remote data and it was found that the recently-implemented gas-particle partitioning scheme is too efficient in producing nitrate and ammonium particles.</p><p>A series of small-scale changes, such as adjusting nitrate dry deposition velocity, direct particulate sulphate emission, and limiting nitrate/ammonium production by the concentration of mineral cations, have been implemented and shown to be effective in improving the simulated surface concentration of &#160;nitrate and ammonium.</p><p>The representation of secondary organic aerosol (SOA) in the IFS has been overhauled with the introduction of a new SOA species, distinct from primary organic matter, with anthropogenic and biogenic components. The implementation of this new species leads to a significant improvement of the simulated surface concentration of organic carbon. An evaluation of simulated SOA concentrations at the surface against climatological values derived from observations using Positive Matrix Factorisation (PMF) techniques also shows a reasonable agreement.</p>
Field observation networks are becoming denser, more diverse, and more mobile, while being required to provide real-time results. The ERC urbisphere program is coordinating multiple field campaigns simultaneously to collect datasets on urban atmospheric and environmental conditions and processes in cities of different sizes. The datasets are used for improving climate and weather models and services, including assessing the impact of cities on the atmosphere (e.g. aerosols, greenhouse gases) as well as the exposure of urban populations in the context of atmospheric extreme events (heat waves, heavy precipitation, air pollution). For model development and evaluation, we are using meshed networks of in-situ observations with ground-based and airborne (remote-)sensing platforms. This contribution describes the urbisphere data management infrastructure and processes required to handle a variety of data streams from primarily novel modular observation systems deployed in complex urban environments.The modular observation systems consist of short-term deployed instrumentation and are separated into three thematic modules. Module A aims at characterizing urban form and function affecting urban climates. Module B quantifies the impact of urban emissions (heat, pollutants, greenhouse gases, etc.) on the urban boundary layer over and downwind of cities. Module C provides data on human exposure at street and indoor-level. The three modules are served with consistent data management, documentation and calibration. Systems deployed in Modules A, B and C include customized automatic weather stations, (Doppler) lidars and ceilometers, scintillometers, balloon radio sounding and spectral camera imaging. Systems are street-light-mounted, located on building roof-tops or indoors as well as on mobile platforms (vehicles, drones). Data ingestion processes are automated, delivering moderate data volumes in real-time to central data infrastructure through mobile phone and IOT connectivity. A meta data system helps keep track of the location and configuration of all deployed components and forms the backbone for conversion of instrument records into location-aware, conventions-aligned and quality-assured F.A.I.R. data products. Furthermore, the data management infrastructure provides services (APIs, Apps, IDEs, etc.) for data inspection and computations by scientists and students involved in the campaigns. Select datasets are integrated in near real-time into other global or local data systems such as, e.g., AERONET, the Phenocam Network, ICOS, or PANAME, for multiple uses.Besides technical aspects and design considerations, we discuss how cooperation and attribution are safeguarded when data are being accessed for immediate academic and citizen data science.  
Abstract. A comprehensive comparison between two aerosol thermodynamic equilibrium models used in chemistry-climate simulations, EQUISOLV II and EQSAM3, is conducted for various relative humidities and chemical compositions. Our results show that the concentration of total particulate matter as well as the associated aerosol liquid water content predicted by these two models is comparable for all conditions, which is important for radiative forcing estimates. The normalized absolute difference in the concentration of total particulate matter is 6% on average for all 200 conditions studied, leading to a regression coefficient of about 0.8 for the water associated with the aerosol between these two models. Relatively large discrepancies occur, however, at high ammonium, low nitrate/sodium concentrations at low and medium relative humidities (RH<60–70%), which is analyzed and discussed in detail. In addition, the prediction of the partitioning of ammonium and nitrate is investigated under realistic atmospheric conditions. The data collected during the Mediterranean Intensive Oxidant Study (MINOS) campaign are simulated using both models. The results show that both models can reproduce the concentration of total particulate matter for 90% of the time within a factor of 2, while the predicted concentration of aerosol water by these two models is significantly correlated. The largest difference exists near RH's of 70–80% which is the RH range for the transition of mixed ammonium salts from the solid to the liquid phase.
Timely information on the effects of the increasing intensity, frequency and duration of heatwaves on cities and critical infrastructure is needed for warning, emergency management and for developing context-specific climate adaptation strategies. Aside from the challenge of deploying sensor networks within built environments, there are hardly any operational city-wide networks that continuously measure and communicate human thermal comfort indices in public spaces.  To address this gap, a two-tiered weather and outdoor human thermal comfort monitoring network was developed and deployed in Freiburg in 2022. The monitoring network comprises a total of 42 automatic weather stations primarily mounted on public lamp posts at a height of 3 m, with the Tier-I network consisting of 13 customised stations, which are equipped with an in-house developed data logging unit optimised for this application, that is extend by a spatially dense but less complex Tier-II network consisting of 29 commercial weather stations. Both networks collect data on air temperature, humidity and precipitation, with the Tier-I network providing additional data on wind, radiation, pressure, lightning, solar radiation and black-globe temperature to calculate human-biometeorological thermal indices such as the Physiological Equivalent Temperature (PET).  Over the course of the first year of deployment (01-Sept-2022 to 31-Aug-2023), the stations have continuously collected high-resolution data (30 and 60 sec) with only little data loss. In a case study, the intra-urban differences in thermal comfort were analysed during the hot month of July 2023, in which five official heat warnings were issued by the German Meteorological Service (DWD). The results show expected intra-urban and urban-rural contrasts and that mid-density sites experience the highest number of summer days, totalling 22, compared to 19-20 in the city centre. The highest amount of moderate heat stress and higher (PET > 29°C) was observed in FRLAND (26,3%) compared to 13-19% at rural sites. Also more tropical nights were observed at inner city sites with 5-6, compared to 3 at outer, primarily suburban sites. Remote and rural sites reported no tropical nights.  Over the full annual cycle and the entire network, the number of tropical nights ranged between 0 (rural) and 29 (inner city) per year. The highest number of summer days per year was recorded in industrial and suburban areas (up to 101) compared to 84-97 days in the city centre and 62-90 days at rural sites. The average annual air temperatures reveal a distinct long-term heat island with an annual mean temperature up to 14.0°C in the city centre, and 11.6°C - 12.7°C at rural sites of same elevation. These results highlight the benefit of continued monitoring for real-time assessments, efficient identification of hot-spots for climate adaptation strategies, and model evaluation and to improve our understanding of urban heat islands and human thermal comfort patterns. In addition, an outreach platform and mobile app (uniWeatherTM) have been developed to provide end-users and the public with free access to real-time data and interpretation following FAIR principles.
Abstract. Interactions of desert dust and air pollution over the eastern Mediterranean (EM) have been studied, focusing on two distinct dust transport events on 22 and 28 September 2011. The atmospheric chemistry–climate model EMAC has been used at about 50 km grid spacing, applying an online dust emission scheme and calcium as a proxy for dust reactivity. EMAC includes a detailed tropospheric chemistry mechanism, aerosol microphysics and thermodynamics schemes to describe dust "aging". The model is evaluated using ground-based observations for aerosol concentrations and aerosol optical depth (AOD) as well as satellite observations. Simulation results and back trajectory analysis show that the development of synoptic disturbances over the EM can enhance dust transport from the Sahara and Arabian deserts in frontal systems that also carry air pollution to the EM. The frontal systems are associated with precipitation that controls the dust removal. Our results show the importance of chemical aging of dust, which increases particle size, dust deposition and scavenging efficiency during transport, overall reducing the lifetime relative to non-aged dust particles. The relatively long travel periods of Saharan dust result in more sustained aging compared to Arabian dust. Sensitivity simulations indicate 3 times more dust deposition of aged relative to pristine dust, which significantly decreases the dust lifetime and loading.
The aim of SolaRes is to provide precise and accurate estimates of solar resource for any location on the globe, in any meteorological and ground surface conditions, and for any solar plant technology. To suit most applications, not only the Global Horizontal Irradiance (GHI) is computed at 1-minute time resolution, but also the direct normal irradiance (DNI), the Diffuse Horizontal Irradiance (DifHI) and the components in tilted planes with any orientation (GTI, DifTI). To make comparisons with ground-based measurements, the circumsolar contribution in measured DNI is also computed.SolaRes was validated in clear-sky conditions encountered in northern France, affected by local and transported anthropogenic pollution and irregular incursions of Saharan desert dust to Europe. For the validation, AERONET provided the input spectral AOT data. Tests were also done with CAMS-NRT as input data source, and comparisons with measurements made on the ATmospheric Observations in LiLLe (ATOLL, France, 50.61167°N, 3.141670°E) platform provided RMSD in GHI smaller than 3% at 1-minute resolution, and RMSD in DNI of 8% [Elias et al., submitted to AMT].In this work, the performances of SolaRes are evaluated in all-sky conditions encountered in northern France and in Germany. The Copernicus Atmosphere Monitoring Service in the near real time mode (CAMS-NRT) provides the input spectral aerosol optical thickness (AOT) data, and the Nowcasting Satellite Application Facilities (NWCSAF) provide the cloud optical thickness. The SolaRes estimates of the three solar resource components GHI, DNI, and DifHI are compared with measurements acquired at ATOLL. The SolaRes estimates of GHI and GTI are compared with measurements made by the PVlive network [Lorenz et al., 2022; and Dittmann et al., 2024 for the data]. Each PVlive station is equipped of a horizontal thermopile pyranometer, and 3 tilted silicon sensors, orientated eastwards, southwards and westwards.RMSD in GHI is found to be 18% at the PVlive station of Freiburg for one year of data (2021) at 1-hour resolution. RMSD in GTI slightly increases to reach 20% at a tilt angle of 25° orientated southwards, and 21% at the same tilt angle but orientated westwards.The satisfying comparison scores in GTI are obtained by considering a solar spectrum restricted between 300 and 1100 nm to simulate the Silicon detector. Improvement will be performed by considering the detailed spectral response as well as the angular loss.SolaRes in its standard mode considers horizontal homogeneous cloud field. Performances could be improved by selecting such observed situations. Moreover, DifTI could be individually tested by selecting measurements in shadows occurring for example for the eastwards instrument when the sun sets down.
A chemical transport model has been extended with an aerosol model describing processes which determine the mass distribution of sulfate, nitrate, ammonium, and aerosol associated water. A specific summer episode is simulated, and the results have been compared to surface concentration measurements and with the aerosol optical depth (AOD) retrieved from satellite measurements, with a focus on the European continent. This study is one of the first to use satellite retrievals over land for this purpose. An average difference in AOD between model and satellite measurements of 0.17–0.19 is calculated, and on average only 40–50% of the observed satellite signal can be explained by our modeled aerosol. In contrast, the observed patterns of optical thickness are well simulated by the model. Also, surface concentrations of simulated aerosol components are in close agreement with measurements. Errors in the vertical distribution of sulfate, ammonium, and nitrate, and hence in the vertical distribution of hygroscopic growth, and errors in modeled optical parameters may partly account for the observed differences in AOD. However, we argue that the most important reason for the large difference is due to the fact that organic and mineral aerosol are not taken into account in this model simulation. A sensitivity study with reduced SO 2 emissions in Europe showed that reduction of the emissions of S 2 in the model leads to a better agreement with surface measurements of SO 2 ; however, calculated sulfate was less strongly influenced.
The ECMWF’s Integrated Forecast System (IFS) is the global atmospheric model used by the Copernicus Atmospheric Monitoring Service (CAMS) to provide analyses and forecasts on atmospheric composition. Currently, the CAMS global model includes the aerosol model of the IFS, the aerosol module IFS-AER making use of a sectional-bulk scheme, and the chemistry scheme based on a CB05-based carbon-bond mechanism, with the option to couple this to stratospheric chemistry module BASCOE. The combined BASCOE will be used operationally in the CAMS global system starting from the upgrade to cycle 48R1 planned in June 2023. This abstract focuses on further developments related to stratospheric chemistry and aerosols that are to be implemented in the future operational cycle 49R1, as well as on a first evaluation of IFS’ performances in representing stratospheric aerosols and chemistry against different datasets.Initially focussing on the troposphere, IFS-AER has been extended to include and represent stratospheric sulfate aerosol processes, keeping the existing tracers. The extended IFS-AER(strato) has been coupled to IFS(BASCOE) through the gaseous sulphuric acid tracer, to the IFS radiation scheme, and to the 4Dvar assimilation scheme. The evaluation of aerosol aspects makes use of aerosol datasets (aerosol extinction, AOD, …) from the Global Ozone Monitoring by Occultation of Stars (GOMOS, onboard Envisat), and the Global Space-based Stratospheric Aerosol Climatology (GloSSAC), based on different cases studies including quiescent and (highly) volcanic periods. It has also been tested against reference simulations from WACCM-CARMA. These intercomparisons show a reasonable agreement against retrieval datasets such as GloSSAC and reference simulations from WACCM-CARMA. In quiescent conditions, the new system showed a decreasing trend with respect to the reference datasets.BASCOE includes a simple PSC parameterization, which has been updated and tuned in cycle 49R1. In order to assess the impact of this upgrade, we evaluate the composition of the polar lower stratosphere during the winter-spring seasons ("ozone hole" events) of 2008, 2009 and 2020 above the Antarctic and 2009, 2011, 2012 and 2020 above the Arctic, with a focus on 5 key species observed by Aura-MLS. This evaluation demonstrates the capacity of IFS(BASCOE) to forecast the chemical composition of the polar lower stratosphere above both the Arctic and the Antarctic for several years with very different evolution of the polar vortex. While further improvements are desirable and will require an overhaul of the PSC parameterization, the current performance allows us to study the interannual variability of ozone hole episodes.
Abstract. We introduce a framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, based on the coefficient, νi. This solute specific coefficient was introduced in Metzger et al. (2012) to accurately parameterize the single solution hygroscopic growth, considering the Kelvin effect – accounting for the water uptake of concentrated nanometer sized particles up to dilute solutions, i.e., from the compounds relative humidity of deliquescence (RHD) up to supersaturation (Köhler-theory). Here we extend the νi-parameterization from single to mixed solutions. We evaluate our framework at various levels of complexity, by considering the full gas-liquid-solid partitioning for a comprehensive comparison with reference calculations using the E-AIM, EQUISOLV II, ISORROPIA II models as well as textbook examples. We apply our parameterization in EQSAM4clim, the EQuilibrium Simplified Aerosol Model V4 for climate simulations, implemented in a box model and in the global chemistry-climate model EMAC. Our results show: (i) that the νi-approach enables to analytically solve the entire gas-liquid-solid partitioning and the mixed solution water uptake with sufficient accuracy, (ii) that, e.g., pure ammonium nitrate and mixed ammonium nitrate – ammonium sulfate mixtures can be solved with a simple method, and (iii) that the aerosol optical depth (AOD) simulations are in close agreement with remote sensing observations for the year 2005. Long-term evaluation of the EMAC results based on EQSAM4clim and ISORROPIA II will be presented separately.
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