Global simulation of semivolatile organic compounds – development and evaluation of the MESSy submodel SVOC (v1.0)
Abstract. The new submodel SVOC for the Modular Earth Submodel System (MESSy) was developed and applied within the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model to simulate the atmospheric cycling and air–surface exchange processes of semivolatile organic pollutants. Our focus is on four polycyclic aromatic hydrocarbons (PAHs) of largely varying properties. Some new features in input and physics parameterizations of tracers were tested: emission seasonality, the size discretization of particulate-phase tracers, the application of poly-parameter linear free-energy relationships in gas–particle partitioning, and re-volatilization from land and sea surfaces. The results indicate that the pre…
A new radiation infrastructure for the Modular Earth Submodel System (MESSy, based on version 2.51)
Abstract. The Modular Earth Submodel System (MESSy) provides an interface to couple submodels to a basemodel via a highly flexible data management facility (Jöckel et al., 2010). In the present paper we present the four new radiation related submodels RAD, AEROPT, CLOUDOPT and ORBIT. The submodel RAD (with shortwave radiation scheme RAD_FUBRAD) simulates the radiative transfer, the submodel AEROPT calculates the aerosol optical properties, the submodel CLOUDOPT calculates the cloud optical properties, and the submodel ORBIT is responsible for Earth orbit calculations. These submodels are coupled via the standard MESSy infrastructure and are largely based on the original radiation scheme of …
Analysis of variability in divergence and turn-over induced by three idealized convective systems with a 3D cloud resolving model
Abstract. The sensitivity of upper tropospheric and lower stratospheric convective outflows and related divergence fields is analysed using an ensemble of cloud resolving model (CM1) simulations in LES-mode including various physically manipulated simulations for three different convective systems initialized with an idealized trigger. The main goal of this study is to assess to what extend the divergence field depends on cloud microphysical processes, the mode of convection and on the processes of convective momentum transport and moist static energy redistribution. We find that latent heat release (representing the microphysical uncertainty) plays an essential role by explaining much of m…
Implementation of the Community Earth System Model (CESM) version 1.2.1 as a new base model into version 2.50 of the MESSy framework
Abstract. The Community Earth System Model (CESM1), maintained by the United States National Centre for Atmospheric Research (NCAR) is connected with the Modular Earth Submodel System (MESSy). For the MESSy user community, this offers many new possibilities. The option to use the Community Atmosphere Model (CAM) atmospheric dynamical cores, especially the state-of-the-art spectral element (SE) core, as an alternative to the ECHAM5 spectral transform dynamical core will provide scientific and computational advances for atmospheric chemistry and climate modelling with MESSy. The well-established finite volume core from CESM1(CAM) is also made available. This offers the possibility to compare …
The Palaeoanthropocene – The beginnings of anthropogenic environmental change
Abstract As efforts to recognize the Anthropocene as a new epoch of geological time are mounting, the controversial debate about the time of its beginning continues. Here, we suggest the term Palaeoanthropocene for the period between the first, barely recognizable, anthropogenic environmental changes and the industrial revolution when anthropogenically induced changes of climate, land use and biodiversity began to increase very rapidly. The concept of the Palaeoanthropocene recognizes that humans are an integral part of the Earth system rather than merely an external forcing factor. The delineation of the beginning of the Palaeoanthropocene will require an increase in the understanding and …
Aerosol physicochemical effects on CCN activation simulated with the chemistry-climate model EMAC
Abstract This study uses the EMAC atmospheric chemistry-climate model to simulate cloud properties with a prognostic cloud droplet nucleation scheme. We present modeled global distributions of cloud condensation nuclei (CCN) number concentrations and CCN activation rates, together with the effective hygroscopicity parameter κ, to describe the aerosol chemical composition effect on CCN activation. Large particles can easily activate into cloud droplets, even at low κ values due to the dominant size effect in cloud droplet formation. Small particles are less efficiently activated as CCN, and are more sensitive to aerosol composition and supersaturation. Since the dominant fraction of small pa…
Sensitivity of aerosol extinction to new mixing rules in the AEROPT submodel of the ECHAM5/MESSy1.9 atmospheric chemistry (EMAC) model
Abstract. The modelling of aerosol radiative forcing is a major cause of uncertainty in the assessment of global and regional atmospheric energy budgets and climate change. One reason is the strong dependence of the aerosol optical properties on the mixing state of aerosol components like black carbon and sulphates. Using a new column version of the aerosol optical properties and radiative transfer code of the atmospheric chemistry-climate model EMAC, we study the radiative transfer applying various mixing states. The aerosol optics code builds on the AEROPT submodel which assumes homogeneous internal mixing utilising the volume average refractive index mixing rule. We have extended the sub…
The 1-way on-line coupled model system MECO(n) – Part 4: Chemical evaluation (based on MESSy v2.52)
Abstract. For the first time a simulation incorporating tropospheric and stratospheric chemistry using the newly developed MECO(n) model system is performed. MECO(n) is short for MESSyfied ECHAM and COSMO model nested n-times. It features an on-line coupling of the COSMO-CLM model, equipped with the Modular Earth Submodel System (MESSy) interface (called COSMO/MESSy), with the global atmospheric chemistry model ECHAM5/MESSy for Atmospheric Chemistry (EMAC). This on-line coupling allows a consistent model chain with respect to chemical and meteorological boundary conditions from the global scale down to the regional kilometre scale. A MECO(2) simulation incorporating one regional instance ov…
New particle formation inside ice clouds: In-situ observations in the tropical tropopause layer of the 2017 Asian Monsoon Anticyclone
Abstract. From 27 July to 10 August 2017 the airborne StratoClim mission took place in Kathmandu, Nepal where eight mission flights were conducted with the M-55 Geophysica up to altitudes of 20 km. New Particle Formation (NPF) was identified by the abundant presence of ultrafine aerosols, with particle diameters dp smaller than 15 nm, which were in-situ detected by means of condensation nuclei counting techniques. NPF fields in clear-skies as well as in the presence of cloud ice particles (dp > 3 µm) were encountered at upper troposphere/lowermost stratosphere (UT/LS) levels and within the Asian Monsoon Anticyclone (AMA). NPF-generated ultrafine particles in elevated concentrations (Nuf)…
Earth System Chemistry integrated Modelling (ESCiMo) with the Modular Earth Submodel System (MESSy) version 2.51
Abstract. Three types of reference simulations, as recommended by the Chemistry–Climate Model Initiative (CCMI), have been performed with version 2.51 of the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model: hindcast simulations (1950–2011), hindcast simulations with specified dynamics (1979–2013), i.e. nudged towards ERA-Interim reanalysis data, and combined hindcast and projection simulations (1950–2100). The manuscript summarizes the updates of the model system and details the different model set-ups used, including the on-line calculated diagnostics. Simulations have been performed with two diff…
Isoprene and monoterpene simulations using the chemistry-climate model EMAC (v2.55) with interactive vegetation from LPJ-GUESS (v4.0)
Earth system models (ESMs) integrate previously separate models of the ocean, atmosphere and vegetation into one comprehensive modelling system enabling the investigation of interactions between different components of the Earth system. Global isoprene and monoterpene emissions from terrestrial vegetation, which represent the most important source of volatile organic compounds (VOCs) in the Earth system, need to be included in global and regional chemical transport models given their major chemical impacts on the atmosphere. Due to the feedback of vegetation activity involving interactions with weather and climate, a coupled modelling system between vegetation and atmospheric chemistry is r…
A multi-model assessment of the impact of sea spray geoengineering on cloud droplet number
Artificially increasing the albedo of marine boundary layer clouds by the mechanical emission of sea spray aerosol has been proposed as a geoengineering technique to slow the warming caused by anthropogenic greenhouse gases. A previous global model study (Korhonen et al., 2010) found that only modest increases (< 20%) and sometimes even decreases in cloud drop number (CDN) concentrations would result from emission scenarios calculated using a windspeed dependent geoengineering flux parameterisation. Here we extend that work to examine the conditions under which decreases in CDN can occur, and use three independent global models to quantify maximum achievable CDN changes. We find that dec…
Towards an advanced atmospheric chemistry-enabled ESM with dynamic land surface processes: Part I - Linking LPJ-GUESS (v4.0) with EMAC modelling system (v2.53)
Earth System Models (ESMs) are invaluable tools that have emerged from decades of research modelling the earth system. Central to this development has been the coupling of previously separate model types, such as ocean, atmospheric and vegetation models, to provide interactive feedbacks between these earth system components. Here we present the initial steps of coupling LPJ-GUESS, a dynamic global vegetation model, to EMAC, an atmospheric chemistry enabled atmosphere-ocean general circulation model. The LPJ-GUESS framework includes a comparatively detailed tree-individual based model of vegetation dynamics, a crop and managed-land scheme, a nitrogen cycle and a choice of fire models; and he…
Improvements of organic aerosol representations and their effects in large-scale atmospheric models
Organics dominate the composition of the atmospheric aerosol, especially in the fine mode, influencing some of its characteristics such as the hygroscopicity, which is of climatic relevance for the Earth system. This study targets an improvement in the description of organic aerosols suitable for large-scale modelling, making use of recent developments based on laboratory and field measurements. In addition to the organic mass and particle number distribution, the proposed method keeps track of the oxidation state of the aerosol based on the OH exposure time, describing some of its chemical characteristics. This study presents the application of the method in a global chemistry climate mode…
Cold cloud microphysical process rates in a global chemistry–climate model
Microphysical processes in cold clouds which act as sources or sinks of hydrometeors below 0 ∘C control the ice crystal number concentrations (ICNCs) and in turn the cloud radiative effects. Estimating the relative importance of the cold cloud microphysical process rates is of fundamental importance to underpin the development of cloud parameterizations for weather, atmospheric chemistry, and climate models and to compare the output with observations at different temporal resolutions. This study quantifies and investigates the ICNC rates of cold cloud microphysical processes by means of the chemistry–climate model EMAC (ECHAM/MESSy Atmospheric Chemistry) and defines the hierarchy of sources…
Stratospheric sulfur and its implications for radiative forcing simulated by the chemistry climate model EMAC
Multiyear simulations with the atmospheric chemistry general circulation model EMAC with a microphysical modal aerosol module at high vertical resolution demonstrate that the sulfur gases COS and SO2, the latter from low-latitude and midlatitude volcanic eruptions, predominantly control the formation of stratospheric aerosol. Marine dimethyl sulfide (DMS) and other SO2 sources, including strong anthropogenic emissions in China, are found to play a minor role except in the lowermost stratosphere. Estimates of volcanic SO2 emissions are based on satellite observations using Total Ozone Mapping Spectrometer and Ozone Monitoring Instrument for total injected mass and Michelson Interferometer fo…
Evaluation of the coupled high-resolution atmospheric chemistry model system MECO(n) using in situ and MAX-DOAS NO2 measurements
We present high spatial resolution (up to 2.2×2.2 km2) simulations focussed over south-west Germany using the online coupled regional atmospheric chemistry model system MECO(n) (MESSy-fied ECHAM and COSMO models nested n times). Numerical simulation of nitrogen dioxide (NO2) surface volume mixing ratios (VMRs) are compared to in situ measurements from a network with 193 locations including background, traffic-adjacent and industrial stations to investigate the model's performance in simulating the spatial and temporal variability of short-lived chemical species. We show that the use of a high-resolution and up-to-date emission inventory is crucial for reproducing the spatial variability and…
Modeling the aerosol chemical composition of the tropopause over the Tibetan Plateau during the Asian summer monsoon
Enhanced aerosol abundance in the upper troposphere and lower stratosphere (UTLS) associated with the Asian summer monsoon (ASM) is referred to as the Asian Tropopause Aerosol Layer (ATAL). The chemical composition, microphysical properties, and climate effects of aerosols in the ATAL have been the subject of discussion over the past decade. In this work, we use the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model at a relatively fine grid resolution (about 1.1×1.1∘) to numerically simulate the emissions, chemistry, and transport of aerosols and their precursors in the UTLS within the ASM anticyclone during the years 2010–2012. We find a pronounced maximum of aerosol extin…
Effects of model configuration for superparametrised long-term simulations – Implementation of a cloud resolving model in EMAC (v2.50)
Abstract. A new module has been implemented in the ECHAM5/MESSy Atmospheric Chemistry (EMAC) Model that simulates cloud related processes on a much smaller grid. This so called superparametrisation acts as a replacement for the convection parametrisation and large-scale cloud scheme. The concept of embedding an ensemble of cloud resolving models (CRMs) inside of each grid box of a general circulation model leads to an explicit representation of cloud dynamics. The new model component is evaluated against observations and the conventional usage of EMAC using a convection parametrisation. In particular, effects of applying different configurations of the superparametrisation are analyzed in a…
Global aerosol modeling with MADE3 (v3.0) in EMAC (based on v2.53): model description and evaluation
Recently, the aerosol microphysics submodel MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, third generation) was introduced as a successor to MADE and MADE-in. It includes nine aerosol species and nine lognormal modes to represent aerosol particles of three different mixing states throughout the aerosol size spectrum. Here, we describe the implementation of the most recent version of MADE3 into the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model, including a detailed evaluation of a 10-year aerosol simulation with MADE3 as part of EMAC. We compare simulation output to station network measurements of near-surface aerosol component mass con…
Intercomparison and evaluation of global aerosol microphysical properties among AeroCom models of a range of complexity
Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from…
The AeroCom evaluation and intercomparison of organic aerosol in global models
This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and op…
Chemistry-climate interactions of aerosol nitrate from lightning
Abstract. Lightning represents one of the dominant emission source for NOx in the troposphere. The direct release of oxidised nitrogen in the upper troposphere does not only affect ozone formation, but also chemical and microphysical properties of aerosol particles in this region. This study investigates the direct impact of LNOx emissions on upper tropospheric nitrate using a global chemistry climate model. The simulation results show a substantial influence of the lightning emissions on the mixing ratios of nitrate aerosol in the upper troposphere of more than 50%. In addition to the impact on nitrate, lightning substantially affects the oxidising capacity of the atmosphere with substanti…
Simulation of organics in the atmosphere: evaluation of EMACv2.54 with the Mainz Organic Mechanism (MOM) coupled to the ORACLE (v1.0) submodel
Abstract. An updated and expanded representation of organics in the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) has been evaluated. First, the comprehensive Mainz Organic Mechanism (MOM) in the submodel MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) was activated with explicit degradation of organic species up to five carbon atoms and a simplified mechanism for larger molecules. Second, the ORACLE submodel (version 1.0) considers now condensation on aerosols for all organics in the mechanism. Parameterizations for aerosol yields are used only for the lumped species that are not included in the explicit mechanism. The simultaneous…
Evaluation of the coupled high-resolution atmospheric chemistry model system MECO(n) using in situ and MAX-DOAS NO&lt;sub&gt;2&lt;/sub&gt; measurements
Abstract. We present high spatial resolution (up to 2.2×2.2 km2) simulations focussed over south-west Germany using the online coupled regional atmospheric chemistry model system MECO(n) (MESSy-fied ECHAM and COSMO models nested n times). Numerical simulation of nitrogen dioxide (NO2) surface volume mixing ratios (VMRs) are compared to in situ measurements from a network with 193 locations including background, traffic-adjacent and industrial stations to investigate the model's performance in simulating the spatial and temporal variability of short-lived chemical species. We show that the use of a high-resolution and up-to-date emission inventory is crucial for reproducing the spatial varia…
Sensitivity of aerosol radiative effects to different mixing assumptions in the AEROPT 1.0 submodel of the EMAC atmospheric-chemistry–climate model
Abstract. The modelling of aerosol radiative forcing is a major cause of uncertainty in the assessment of global and regional atmospheric energy budgets and climate change. One reason is the strong dependence of the aerosol optical properties on the mixing state of aerosol components, such as absorbing black carbon and, predominantly scattering sulfates. Using a new column version of the aerosol optical properties and radiative-transfer code of the ECHAM/MESSy atmospheric-chemistry–climate model (EMAC), we study the radiative transfer applying various mixing states. The aerosol optics code builds on the AEROPT (AERosol OPTical properties) submodel, which assumes homogeneous internal mixing …
Chemical aging of atmospheric mineral dust during transatlantic transport
Abstract. Transatlantic dust transport has many implications for the atmosphere, ocean and climate. We present a modeling study on the impact of the key processes (dust emissions flux, convection and dust aging parameterizations) that control the transatlantic dust transport. Typically, the Inter-Tropical Convergence Zone (ITCZ) acts as a barrier for the meridional dust transport. To characterize the dust outflow over the Atlantic Ocean, we address two regional phenomena: (i) dust interactions with the ITCZ (DIZ) and (ii) the adjacent dust transport over the Atlantic Ocean (DTA). In the DTA zone, the dust loading shows a steep and linear gradient westward over the Atlantic Ocean where parti…