Nitrogen compounds and ozone in the stratosphere: comparison of MIPAS satellite data with the Chemistry Climate Model ECHAM5/MESSy1

International audienceThe chemistry climate model ECHAM5/MESSy1 (E5/M1) in a setup extending from the surface to 80 km with a vertical resolution of about 600 m near the tropopause with nudged tropospheric meteorology allows a direct comparison with satellite data of chemical species at the same time and location. Here we present results out of a transient 10 years simulation for the period of the Antarctic vortex split in September 2002, where data of MIPAS on the ENVISAT-satellite are available. For the first time this satellite instrument opens the opportunity, to evaluate all stratospheric nitrogen containing species simultaneously with a good global coverage, including the source gas N2O which allows an estimate for NOx-production in the stratosphere. We show correlations between simulated and observed species in the altitude region between 10 and 50 hpa for different latitude belts, together with the Probability Density Functions (PDFs) of model results and observations. This is supplemented by global charts on pressure levels showing the satellite data and the simulated data sampled at the same time and location. We demonstrate that the model in most cases captures the partitioning in the nitrogen family, the diurnal cycles and the spatial distribution within experimental uncertainty. There appears to be, however, a problem to reproduce the observed nighttime partitioning between N2O5 and NO2 in the middle stratosphere

New representation of water activity based on a single solute specific constant to parameterize the hygroscopic growth of aerosols in atmospheric models

Water activity is a key factor in aerosol thermodynamics and hygroscopic growth. We introduce a new representation of water activity (<i>a</i><sub>w</sub>), which is empirically related to the solute molality (μ<sub>s</sub>) through a single solute specific constant, ν<sub><i>i</i></sub>. Our approach is widely applicable, considers the Kelvin effect and covers ideal solutions at high relative humidity (RH), including cloud condensation nuclei (CCN) activation. It also encompasses concentrated solutions with high ionic strength at low RH such as the relative humidity of deliquescence (RHD). The constant ν<sub><i>i</i></sub> can thus be used to parameterize the aerosol hygroscopic growth over a wide range of particle sizes, from nanometer nucleation mode to micrometer coarse mode particles. In contrast to other <i>a</i><sub>w</sub>-representations, our ν<sub><i>i</i></sub> factor corrects the solute molality both linearly and in exponent form <i>x · a<sup>x</sup></i>. We present four representations of our basic <i>a</i><sub>w</sub>-parameterization at different levels of complexity for different <i>a</i><sub>w</sub>-ranges, e.g. up to 0.95, 0.98 or 1. ν<sub><i>i</i></sub> is constant over the selected <i>a</i><sub>w</sub>-range, and in its most comprehensive form, the parameterization describes the entire <i>a</i><sub>w</sub> range (0–1). In this work we focus on single solute solutions. ν<sub><i>i</i></sub> can be pre-determined with a root-finding method from our water activity representation using an <i>a</i><sub>w</sub>−μ<sub>s</sub> data pair, e.g. at solute saturation using RHD and solubility measurements. Our <i>a</i><sub>w</sub> and supersaturation (Köhler-theory) results compare well with the thermodynamic reference model E-AIM for the key compounds NaCl and (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> relevant for CCN modeling and calibration studies. Envisaged applications include regional and global atmospheric chemistry and climate modeling

Viabilidade de pupas de Thelosia camina schaus coletadas em plantios de erva-mate.

Resumo

Simulation of polar stratospheric clouds in the chemistry-climate-model EMAC via the submodel PSC

The submodel PSC of the ECHAM5/MESSy Atmospheric Chemistry model (EMAC) has been developed to simulate the main types of polar stratospheric clouds (PSC). The parameterisation of the supercooled ternary solutions (STS, type 1b PSC) in the submodel is based on Carslaw et al. (1995b), the thermodynamic approach to simulate ice particles (type 2 PSC) on Marti and Mauersberger (1993). For the formation of nitric acid trihydrate (NAT) particles (type 1a PSC) two different parameterisations exist. The first is based on an instantaneous thermodynamic approach from Hanson and Mauersberger (1988), the second is new implemented and considers the growth of the NAT particles with the aid of a surface growth factor based on Carslaw et al. (2002). It is possible to choose one of this NAT parameterisation in the submodel. This publication explains the background of the submodel PSC and the use of the submodel with the goal of simulating realistic PSC in EMAC

Interannual variation patterns of total ozone and lower stratospheric temperature in observations and model simulations

We report results from a multiple linear regression analysis of long-term total ozone observations (1979 to 2000, by TOMS/SBUV), of temperature reanalyses (1958 to 2000, NCEP), and of two chemistry-climate model simulations (1960 to 1999, by ECHAM4.L39(DLR)/CHEM (=E39/C), and MAECHAM4-CHEM). The model runs are transient experiments, where observed sea surface temperatures, increasing source gas concentrations (CO2, CFCs, CH4, N2O, NOx), 11-year solar cycle, volcanic aerosols and the quasi-biennial oscillation (QBO) are all accounted for. MAECHAM4-CHEM covers the atmosphere from the surface up to 0.01 hPa ( 80 km). For a proper representation of middle atmosphere (MA) dynamics, it includes a parametrization for momentum deposition by dissipating gravity wave spectra. E39/C, on the other hand, has its top layer centered at 10 hPa ( 30 km). It is targeted on processes near the tropopause, and has more levels in this region. Despite some problems, both models generally reproduce the observed amplitudes and much of the observed lowlatitude patterns of the various modes of interannual variability in total ozone and lower stratospheric temperature. In most aspects MAECHAM4-CHEM performs slightly better than E39/C. MAECHAM4-CHEM overestimates the longterm decline of total ozone, whereas E39/C underestimates the decline over Antarctica and at northern mid-latitudes. The true long-term decline in winter and spring above the Correspondence to: W. Steinbrecht ([email protected]) Arctic may be underestimated by a lack of TOMS/SBUV observations in winter, particularly in the cold 1990s. Main contributions to the observed interannual variations of total ozone and lower stratospheric temperature at 50 hPa come from a linear trend (up to −10 DU/decade at high northern latitudes, up to −40 DU/decade at high southern latitudes, and around −0.7 K/decade over much of the globe), from the intensity of the polar vortices (more than 40 DU, or 8 K peak to peak), the QBO (up to 20 DU, or 2 K peak to peak), and from tropospheric weather (up to 20 DU, or 2 K peak to peak). Smaller variations are related to the 11-year solar cycle (generally less than 15 DU, or 1 K), or to ENSO (up to 10 DU, or 1 K). These observed variations are replicated well in the simulations. Volcanic eruptions have resulted in sporadic changes (up to −30 DU, or +3 K). At low latitudes, patterns are zonally symmetric. At higher latitudes, however, strong, zonally non-symmetric signals are found close to the Aleutian Islands or south of Australia. Such asymmetric features appear in the model runs as well, but often at different longitudes than in the observations. The results point to a key role of the zonally asymmetric Aleutian (or Australian) stratospheric anti-cyclones for interannual variations at high-latitudes, and for coupling between polar vortex strength, QBO, 11-year solar cycle and ENSO

Interannual variation patterns of total ozone and temperature in observations and model simulations

International audienceWe report results from a multiple linear regression analysis of long-term total ozone observations (1979 to 2002, by TOMS/SBUV), of temperature reanalyses (1958 to 2002, NCEP), and of two chemistry-climate model simulations (1960 to 1999, by ECHAM4.L39(DLR)/CHEM (=E39/C), and MAECHAM4-CHEM). The model runs are transient experiments, where observed sea surface temperatures, increasing source gas concentrations (CO2, CFCs, CH4, N2O, NOx), 11-year solar cycle, volcanic aerosols and the quasi-biennial oscillation (QBO) are all accounted for. MAECHAM4-CHEM covers the atmosphere from the surface up to 0.01 hPa (?80 km). For a proper representation of middle atmosphere (MA) dynamics, it includes a parametrization for momentum deposition by dissipating gravity wave spectra. E39/C, on the other hand, has its top layer centered at 10 hPa (?30 km). It is targeted on processes near the tropopause, and has more levels in this region. Both models reproduce the observed amplitudes and much of the observed low-latitude patterns of the various modes of interannual variability, MAECHAM4-CHEM somewhat better than E39/C. Total ozone and lower stratospheric temperature show similar patterns. Main contributions to the interannual variations of total ozone and lower stratospheric temperature at 50 hPa come from a linear trend (up to ?30 Dobson Units (DU) per decade, or ?1.5 K/decade), the QBO (up to 25 DU, or 2.5 K peak to peak), the intensity of the polar vortices (up to 50 DU, or 5 K peak to peak), and from tropospheric weather (up to 30 DU, or 3 K peak to peak). Smaller variations are related to the 11-year solar cycle (generally less than 25 DU, or 2.5 K), and to ENSO (up to 15 DU, or 1.5 K). Volcanic eruptions have resulted in sporadic changes (up to ?40 DU, or +3 K). Most stratospheric variations are connected to the troposphere, both in observations and simulations. At low latitudes, patterns are zonally symmetric. At higher latitudes, however, strong, zonally non-symmetric signals are found close to the Aleutian Islands or south of Australia. Such asymmetric features appear in the model runs as well, but often at different longitudes than in the observations. The results point to a key role of the zonally asymmetric Aleutian (or Australian) stratospheric anti-cyclones for interannual variations at high- latitudes, and for coupling between polar vortex strength, QBO, 11-year solar cycle and ENSO

Interannual variation patterns of total ozone and temperature in observations and model simulations

We report results from a multiple linear regression analysis of long-term total ozone observations (1979 to 2000, by TOMS/SBUV), of temperature reanalyses (1958 to 2000, NCEP), and of two chemistry-climate model simulations (1960 to 1999, by ECHAM4.L39(DLR)/CHEM (=E39/C), and MAECHAM4-CHEM). The model runs are transient experiments, where observed sea surface temperatures, increasing source gas concentrations (CO2, CFCs, CH4, N2O, NOx), 11-year solar cycle, volcanic aerosols and the quasi-biennial oscillation (QBO) are all accounted for. MAECHAM4-CHEM covers the atmosphere from the surface up to 0.01 hPa (≈80 km). For a proper representation of middle atmosphere (MA) dynamics, it includes a parametrization for momentum deposition by dissipating gravity wave spectra. E39/C, on the other hand, has its top layer centered at 10 hPa (≈30 km). It is targeted on processes near the tropopause, and has more levels in this region. Despite some problems, both models generally reproduce the observed amplitudes and much of the observed low-latitude patterns of the various modes of interannual variability in total ozone and lower stratospheric temperature. In most aspects MAECHAM4-CHEM performs slightly better than E39/C. MAECHAM4-CHEM overestimates the long-term decline of total ozone, whereas underestimates the decline over Antarctica and at northern mid-latitudes. The true long-term decline in winter and spring above the Arctic may be underestimated by a lack of TOMS/SBUV observations in winter, particularly in the cold 1990s. Main contributions to the observed interannual variations of total ozone and lower stratospheric temperature at 50 hPa come from a linear trend (up to -10 DU/decade at high northern latitudes, up to -40 DU/decade at high southern latitudes, and around -0.7 K/decade over much of the globe), from the intensity of the polar vortices (more than 40 DU, or 8 K peak to peak), the QBO (up to 20 DU, or 2 K peak to peak), and from tropospheric weather (up to 20 DU, or 2 K peak to peak). Smaller variations are related to the 11-year solar cycle (generally less than 15 DU, or 1 K), or to ENSO (up to 10 DU, or 1 K). These observed variations are replicated well in the simulations. Volcanic eruptions have resulted in sporadic changes (up to -30 DU, or +3 K). At low latitudes, patterns are zonally symmetric. At higher latitudes, however, strong, zonally non-symmetric signals are found close to the Aleutian Islands or south of Australia. Such asymmetric features appear in the model runs as well, but often at different longitudes than in the observations. The results point to a key role of the zonally asymmetric Aleutian (or Australian) stratospheric anti-cyclones for interannual variations at high-latitudes, and for coupling between polar vortex strength, QBO, 11-year solar cycle and ENSO

Interannual variation patterns of total ozone and lower stratospheric temperature in observations and model simulations

We report results from a multiple linear regression analysis of long-term total ozone observations (1979 to 2000, by TOMS/SBUV), of temperature reanalyses (1958 to 2000, NCEP), and of two chemistry-climate model simulations (1960 to 1999, by ECHAM4.L39(DLR)/CHEM (=E39/C), and MAECHAM4-CHEM). The model runs are transient experiments, where observed sea surface temperatures, increasing source gas concentrations (CO₂, <i>CFC</i>s, CH₄, N₂O, NO_x), 11-year solar cycle, volcanic aerosols and the quasi-biennial oscillation (QBO) are all accounted for. MAECHAM4-CHEM covers the atmosphere from the surface up to 0.01&nbsp;hPa (&asymp;80&nbsp;km). For a proper representation of middle atmosphere (MA) dynamics, it includes a parametrization for momentum deposition by dissipating gravity wave spectra. E39/C, on the other hand, has its top layer centered at 10&nbsp;hPa (&asymp;30&nbsp;km). It is targeted on processes near the tropopause, and has more levels in this region. Despite some problems, both models generally reproduce the observed amplitudes and much of the observed low-latitude patterns of the various modes of interannual variability in total ozone and lower stratospheric temperature. In most aspects MAECHAM4-CHEM performs slightly better than E39/C. MAECHAM4-CHEM overestimates the long-term decline of total ozone, whereas underestimates the decline over Antarctica and at northern mid-latitudes. The true long-term decline in winter and spring above the Arctic may be underestimated by a lack of TOMS/SBUV observations in winter, particularly in the cold 1990s. Main contributions to the observed interannual variations of total ozone and lower stratospheric temperature at 50&nbsp;hPa come from a linear trend (up to -10&nbsp;DU/decade at high northern latitudes, up to -40&nbsp;DU/decade at high southern latitudes, and around -0.7&nbsp;K/decade over much of the globe), from the intensity of the polar vortices (more than 40&nbsp;DU, or 8&nbsp;K peak to peak), the QBO (up to 20&nbsp;DU, or 2&nbsp;K peak to peak), and from tropospheric weather (up to 20&nbsp;DU, or 2&nbsp;K peak to peak). Smaller variations are related to the 11-year solar cycle (generally less than 15&nbsp;DU, or 1&nbsp;K), or to ENSO (up to 10&nbsp;DU, or 1&nbsp;K). These observed variations are replicated well in the simulations. Volcanic eruptions have resulted in sporadic changes (up to -30&nbsp;DU, or +3&nbsp;K). At low latitudes, patterns are zonally symmetric. At higher latitudes, however, strong, zonally non-symmetric signals are found close to the Aleutian Islands or south of Australia. Such asymmetric features appear in the model runs as well, but often at different longitudes than in the observations. The results point to a key role of the zonally asymmetric Aleutian (or Australian) stratospheric anti-cyclones for interannual variations at high-latitudes, and for coupling between polar vortex strength, QBO, 11-year solar cycle and ENSO

Description and evaluation of GMXe: a new aerosol submodel for global simulations (v1)

We present a new aerosol microphysics and gas aerosol partitioning submodel (Global Modal-aerosol eXtension, GMXe) implemented within the ECHAM/MESSy Atmospheric Chemistry model (EMAC, version 1.8). The submodel is computationally efficient and is suitable for medium to long term simulations with global and regional models. The aerosol size distribution is treated using 7 log-normal modes and has the same microphysical core as the M7 submodel (Vignati et al., 2004). &lt;br&gt;&lt;br&gt; The main developments in this work are: (i) the extension of the aerosol emission routines and the M7 microphysics, so that an increased (and variable) number of aerosol species can be treated (new species include sodium and chloride, and potentially magnesium, calcium, and potassium), (ii) the coupling of the aerosol microphysics to a choice of treatments of gas/aerosol partitioning to allow the treatment of semi-volatile aerosol, and, (iii) the implementation and evaluation of the developed submodel within the EMAC model of atmospheric chemistry. &lt;br&gt;&lt;br&gt; Simulated concentrations of black carbon, particulate organic matter, dust, sea spray, sulfate and ammonium aerosol are shown to be in good agreement with observations (for all species at least 40% of modeled values are within a factor of 2 of the observations). The distribution of nitrate aerosol is compared to observations in both clean and polluted regions. Concentrations in polluted continental regions are simulated quite well, but there is a general tendency to overestimate nitrate, particularly in coastal regions (geometric mean of modelled values/geometric mean of observed data ≈2). In all regions considered more than 40% of nitrate concentrations are within a factor of two of the observations. Marine nitrate concentrations are well captured with 96% of modeled values within a factor of 2 of the observations