scholarly journals Modelling marine emissions and atmospheric distributions of halocarbons and DMS: the influence of prescribed water concentration vs. prescribed emissions

2015 ◽  
Vol 15 (12) ◽  
pp. 17553-17598
Author(s):  
S. T. Lennartz ◽  
G. Krysztofiak-Tong ◽  
C. A. Marandino ◽  
B.-M. Sinnhuber ◽  
S. Tegtmeier ◽  
...  

Abstract. Marine produced short-lived trace gases such as dibromomethane (CH2Br2), bromoform (CHBr3), methyliodide (CH3I) and dimethylsulfide (DMS) significantly impact tropospheric and stratospheric chemistry. Describing their marine emissions in atmospheric chemistry models as accurately as possible is necessary to quantify their impact on ozone depletion and the Earth's radiative budget. So far, marine emissions of trace gases have mainly been prescribed from emission climatologies, thus lacking the interaction between the actual state of the atmosphere and the ocean. Here we present simulations with the chemistry climate model EMAC with online calculation of emissions based on surface water concentrations, in contrast to directly prescribed emissions. Considering the actual state of the model atmosphere results in a concentration gradient consistent with model real-time conditions at ocean surface and atmosphere, which determine the direction and magnitude of the computed flux. This method has a number of conceptual and practical benefits, as the modelled emission can respond consistently to changes in sea surface temperature, surface wind speed, sea ice cover and especially atmospheric mixing ratio. This online calculation could enhance, dampen or even invert the fluxes (i.e. deposition instead of emissions) of VSLS. We show that differences between prescribing emissions and prescribing concentrations (−28 % for CH2Br2 to +11 % for CHBr3) result mainly from consideration of the actual, time-varying state of the atmosphere. The absolute magnitude of the differences depends mainly on the surface ocean saturation of each particular gas. Comparison to observations from aircraft, ships and ground stations reveals that computing the air–sea flux interactively leads in most of the cases to more accurate atmospheric mixing ratios in the model compared to the computation from prescribed emissions. Calculating emissions online also enables effective testing of different air–sea transfer velocity parameterizations k, which was performed here for eight different parameterizations. The testing of these different k values is of special interest for DMS, as recently published parameterizations derived by direct flux measurements using eddy covariance measurements suggest decreasing k values at high wind speeds or a linear relationship with wind speed. Implementing these parameterizations reduces discrepancies in modelled DMS atmospheric mixing ratios and observations by a factor of 1.5 compared to parameterizations with a quadratic or cubic relationship to wind speed.

2015 ◽  
Vol 15 (20) ◽  
pp. 11753-11772 ◽  
Author(s):  
S. T. Lennartz ◽  
G. Krysztofiak ◽  
C. A. Marandino ◽  
B.-M. Sinnhuber ◽  
S. Tegtmeier ◽  
...  

Abstract. Marine-produced short-lived trace gases such as dibromomethane (CH2Br2), bromoform (CHBr3), methyliodide (CH3I) and dimethyl sulfide (DMS) significantly impact tropospheric and stratospheric chemistry. Describing their marine emissions in atmospheric chemistry models as accurately as possible is necessary to quantify their impact on ozone depletion and Earth's radiative budget. So far, marine emissions of trace gases have mainly been prescribed from emission climatologies, thus lacking the interaction between the actual state of the atmosphere and the ocean. Here we present simulations with the chemistry climate model EMAC (ECHAM5/MESSy Atmospheric Chemistry) with online calculation of emissions based on surface water concentrations, in contrast to directly prescribed emissions. Considering the actual state of the model atmosphere results in a concentration gradient consistent with model real-time conditions at the ocean surface and in the atmosphere, which determine the direction and magnitude of the computed flux. This method has a number of conceptual and practical benefits, as the modelled emission can respond consistently to changes in sea surface temperature, surface wind speed, sea ice cover and especially atmospheric mixing ratio. This online calculation could enhance, dampen or even invert the fluxes (i.e. deposition instead of emissions) of very short-lived substances (VSLS). We show that differences between prescribing emissions and prescribing concentrations (−28 % for CH2Br2 to +11 % for CHBr3) result mainly from consideration of the actual, time-varying state of the atmosphere. The absolute magnitude of the differences depends mainly on the surface ocean saturation of each particular gas. Comparison to observations from aircraft, ships and ground stations reveals that computing the air–sea flux interactively leads in most of the cases to more accurate atmospheric mixing ratios in the model compared to the computation from prescribed emissions. Calculating emissions online also enables effective testing of different air–sea transfer velocity (k) parameterizations, which was performed here for eight different parameterizations. The testing of these different k values is of special interest for DMS, as recently published parameterizations derived by direct flux measurements using eddy covariance measurements suggest decreasing k values at high wind speeds or a linear relationship with wind speed. Implementing these parameterizations reduces discrepancies in modelled DMS atmospheric mixing ratios and observations by a factor of 1.5 compared to parameterizations with a quadratic or cubic relationship to wind speed.


2014 ◽  
Vol 14 (19) ◽  
pp. 10721-10730 ◽  
Author(s):  
L. Ran ◽  
W. L. Lin ◽  
Y. Z. Deji ◽  
B. La ◽  
P. M. Tsering ◽  
...  

Abstract. Through several years of development, the city of Lhasa has become one of the most populated and urbanized areas on the highest plateau in the world. In the process of urbanization, current and potential air quality issues have been gradually concerned. To investigate the current status of air pollution in Lhasa, various gas pollutants including NOx, CO, SO2, and O3, were continuously measured from June 2012 to May 2013 at an urban site (29.40° N, 91.08° E, 3650 m a.s.l.). The seasonal variations of primary gas pollutants exhibited a peak from November to January with a large variability. High mixing ratios of primary trace gases almost exclusively occurred under low wind speed and showed no distinct dependence on wind direction, implying local urban emissions to be predominant. A comparison of NO2, CO, and SO2 mixing ratios in summer between 1998 and 2012 indicated a significant increase in emissions of these gas pollutants and a change in their intercorrelations, as a result of a substantial growth in the demand of energy consumption using fossil fuels instead of previously widely used biomass. The pronounced diurnal double peaks of primary trace gases in all seasons suggested automobile exhaust to be a major emission source in Lhasa. The secondary gas pollutant O3 displayed an average diurnal cycle of a shallow flat peak for about 4–5 h in the afternoon and a minimum in the early morning. Nighttime O3 was sometimes completely consumed by the high level of NOx. Seasonally, the variations of O3 mixing ratios displayed a low valley in winter and a peak in spring. In autumn and winter, transport largely contributed to the observed O3 mixing ratios, given its dependence on wind speed and wind direction, while in spring and summer photochemistry played an important role. A more efficient buildup of O3 mixing ratios in the morning and a higher peak in the afternoon was found in summer 2012 than in 1998. An enhancement in O3 mixing ratios would be expected in the future and more attention should be given to O3 photochemistry in response to increasing precursor emissions in this area.


2015 ◽  
Vol 8 (8) ◽  
pp. 2435-2445 ◽  
Author(s):  
H. G. Ouwersloot ◽  
A. Pozzer ◽  
B. Steil ◽  
H. Tost ◽  
J. Lelieveld

Abstract. The convective transport module, CVTRANS, of the ECHAM/MESSy Atmospheric Chemistry (EMAC) model has been revised to better represent the physical flows and incorporate recent findings on the properties of the convective plumes. The modifications involve (i) applying intermediate time stepping based on a settable criterion, (ii) using an analytic expression to account for the intra-time-step mixing ratio evolution below cloud base, and (iii) implementing a novel expression for the mixing ratios of atmospheric compounds at the base of an updraft. Even when averaged over a year, the predicted mixing ratios of atmospheric compounds are affected considerably by the intermediate time stepping. For example, for an exponentially decaying atmospheric tracer with a lifetime of 1 day, the zonal averages can locally differ by more than a factor of 6 and the induced root mean square deviation from the original code is, weighted by the air mass, higher than 40 % of the average mixing ratio. The other modifications result in smaller differences. However, since they do not require additional computational time, their application is also recommended.


2020 ◽  
Author(s):  
Franziska Winterstein ◽  
Patrick Jöckel ◽  
Martin Dameris ◽  
Michael Ponater ◽  
Fabian Tanalski ◽  
...  

<p>Methane (CH<sub>4</sub>) is the second most important greenhouse gas, which atmospheric concentration is influenced by human activities and currently on a sharp rise. We present a study with numerical simulations using a Chemistry-Climate-Model (CCM), which are performed to assess possible consequences of strongly enhanced CH<sub>4</sub> concentrations in the Earth's atmosphere for the climate.</p><p>Our analysis includes experiments with 2xCH<sub>4</sub> and 5xCH<sub>4</sub> present day (2010) lower boundary mixing ratios using the CCM EMAC. The simulations are conducted with prescribed oceanic conditions, mimicking present day tropospheric temperatures as its changes are largely suppressed. By doing so we are able to investigate the quasi-instantaneous chemical impact on the atmosphere. We find that the massive increase in CH<sub>4</sub> strongly influences the tropospheric chemistry by reducing the OH abundance and thereby extending the tropospheric CH<sub>4</sub> lifetime as well as the residence time of other chemical pollutants. The region above the tropopause is impacted by a substantial rise in stratospheric water vapor (SWV). The stratospheric ozone (O<sub>3</sub>) column increases overall, but SWV induced stratospheric cooling also leads to enhanced ozone depletion in the Antarctic lower stratosphere. Regional  patterns of ozone change are affected by modification of stratospheric dynamics, i.e. increased tropical up-welling and stronger meridional transport  towards the polar regions. We calculate the net radiative impact (RI) of the 2xCH<sub>4</sub> experiment to be 0.69 W m<sup>-2</sup> and for the 5xCH<sub>4</sub> experiment to be 1.79 W m<sup>-2</sup>. A substantial part of the RI is contributed by chemically induced O<sub>3</sub> and SWV changes, in line with previous radiative forcing estimates and is for the first time splitted and spatially asigned to its chemical contributors.</p><p>This numerical study using a CCM with prescibed oceanic conditions shows the rapid responses to significantly enhanced CH<sub>4</sub> mixing ratios, which is the first step towards investigating the impact of possible strong future CH<sub>4</sub> emissions on atmospheric chemistry and its feedback on climate.</p>


2019 ◽  
Author(s):  
Xiaoyong Yu ◽  
Annette Rinke ◽  
Wolfgang Dorn ◽  
Gunnar Spreen ◽  
Christof Lüpkes ◽  
...  

Abstract. We examine the simulated Arctic sea-ice drift speed for the period 2003–2014 in the coupled Arctic regional climate model HIRHAM-NAOSIM 2.0. In particular, we evaluate the dependency of the drift speed on the near-surface wind speed and sea-ice conditions. Considering the seasonal cycle of Arctic basin averaged drift speed, the model reproduces the summer-autumn drift speed well, but significantly overestimates the winter-spring drift speed, compared to satellite-derived observations. Also, the model does not capture the observed seasonal phase lag between drift and wind speed, but the simulated drift speed is more in phase with near-surface wind. The model calculates a realistic negative relationship between drift speed and ice thickness and between drift speed and ice concentration during summer-autumn when concentration is relatively low, but the correlation is weaker than observed. A daily grid-scale diagnostic indicates that the model reproduces the observed positive relationship between drift and wind speed. The strongest impact of wind changes on drift speed occurs for high and moderate wind speeds, with a low impact for calm conditions. The correlation under low-wind conditions is overestimated in the simulations, compared to observation/reanalysis. A sensitivity experiment demonstrates the significant effects of sea-ice form drag included by an improved parameterization of the transfer coefficients for momentum and heat over sea ice. However, this does not improve the agreement of the modelled drift speed/wind speed ratio with observations based on reanalysis for wind and remote sensing for sea ice drift. An improvement might be possible, among others, by tuning the open parameters of the parameterization in future.


2020 ◽  
Author(s):  
Markus Kunze ◽  
Tim Kruschke ◽  
Ulrike Langematz ◽  
Miriam Sinnhuber ◽  
Thomas Reddmann ◽  
...  

Abstract. Variations of the solar spectral irradiance (SSI) with the 11-year sunspot cycle have been shown to have a significant impact on temperatures and the mixing ratios of atmospheric constituents in the stratosphere and mesosphere. Uncertainties in modelling the effects of SSI variations arise from uncertainties in the empirical models reconstructing the prescribed SSI data set as well as from uncertainties in the chemistry-climate model (CCM) formulation. In this study CCM simulations with the ECHAM MESSy Atmospheric Chemistry (EMAC) model and the Community Earth System Model 1 (CESM1) – Whole Atmosphere Chemistry Climate Model (WACCM) have been performed to quantify the uncertainties of the solar responses in chemistry and dynamics that are due to the usage of five different SSI data sets or the two CCMs. We apply a two-way analysis of variance (ANOVA) to separate the influence of the SSI data sets and the CCMs on the variability of the solar response in shortwave heating rates, temperature and ozone. The ANOVA identifies the SSI data set with the strongest influence on the variability of the solar signal in shortwave heating rates in the upper mesosphere and in the upper stratosphere/lower mesosphere. The strongest influence on the variability of the solar signal in ozone and temperature is identified in the upper stratosphere/lower mesosphere. The largest influence of the CCMs on variability of the solar responses can be identified in the upper mesosphere. The solar response in the lower stratosphere also depends on the CCM used, especially in the tropics and northern hemispheric subtropics and mid latitudes, where the model dynamics modulate the solar responses.


2012 ◽  
Vol 12 (14) ◽  
pp. 6581-6592 ◽  
Author(s):  
G. Wetzel ◽  
H. Oelhaf ◽  
O. Kirner ◽  
F. Friedl-Vallon ◽  
R. Ruhnke ◽  
...  

Abstract. The winter 2009/2010 was characterized by a strong Arctic vortex with extremely cold mid-winter temperatures in the lower stratosphere associated with an intense activation of reactive chlorine compounds (ClOx) from reservoir species. Stratospheric limb emission spectra were recorded during a flight of the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) from Kiruna (Sweden) on 24 January 2010 inside the Arctic vortex. Several fast limb sequences of spectra (in time steps of about 10 min) were measured from nighttime photochemical equilibrium to local noon allowing the retrieval of chlorine- and nitrogen-containing species which change rapidly their concentration around the terminator between night and day. Mixing ratios of species like ClO, NO2, and N2O5 show significant changes around sunrise, which are temporally delayed due to polar stratospheric clouds reducing the direct radiative flux from the sun. ClO variations were derived for the first time from MIPAS-B spectra. Daytime ClO values of up to 1.6 ppbv are visible in a broad chlorine activated layer below 26 km correlated with low values (below 0.1 ppbv) of the chlorine reservoir species ClONO2. Observations are compared and discussed with calculations performed with the 3-dimensional Chemistry Climate Model EMAC (ECHAM5/MESSy Atmospheric Chemistry). Mixing ratios of the species ClO, NO2, and N2O5 are well reproduced by the model during night and noon. However, the onset of ClO production and NO2 loss around the terminator in the model is not consistent with the measurements. The MIPAS-B observations along with Tropospheric Ultraviolet-Visible (TUV) radiation model calculations suggest that polar stratospheric clouds lead to a delayed start followed by a faster increase of the photodissoziation of ClOOCl and NO2 near the morning terminator since stratospheric clouds alter the direct and the diffuse flux of solar radiation. These effects are not considered in the EMAC model simulations which assume a cloudless atmosphere.


2021 ◽  
Vol 2145 (1) ◽  
pp. 012048
Author(s):  
Pakpoom Ratjiranukool ◽  
Sujittra Ratjiranukool

Abstract One of the alternative energy sources which have globally pay more attention is wind power. In this research, the Weibull wind speed distribution was applied to evaluate wind energy potential during the period of 2081-2090. The projected wind datasets in this study were simulated by the Non hydrostatic Regional Climate Model (NHRCM). The boundary condition was the 20 km resolution MRI Atmospheric General Circulation Model (AGCM20) under the RCP8.5 scenario. The surface wind datasets in Chiang Mai were analyzed to 3-time intervals, i.e., May-August, September-December and January-April. Two averaged Weibull distribution parameters, i.e., k, shape parameter, and c, scale parameter were determined. The shape and scale parameters fluctuated 1.15 to 1.34 and 0.38 m/s to 0.74 m/s, respectively. It was found that the surface mean wind speed from May through August was stronger than from September through December.


2013 ◽  
Vol 13 (3) ◽  
pp. 6067-6129 ◽  
Author(s):  
M. S. Long ◽  
W.C. Keene ◽  
R. C. Easter ◽  
R. Sander ◽  
X. Liu ◽  
...  

Abstract. Observations and model studies suggest a significant but highly non-linear role for halogens, primarily Cl and Br, in multiphase atmospheric processes relevant to tropospheric chemistry and composition, aerosol evolution, radiative transfer, weather, and climate. The sensitivity of global atmospheric chemistry to the production of marine aerosol and the associated activation and cycling of inorganic Cl and Br was tested using a size-resolved multiphase coupled chemistry/global climate model (National Center for Atmospheric Research's Community Atmosphere Model (CAM); v3.6.33). Simulation results showed strong meridional and vertical gradients in Cl and Br species. The simulation reproduced most available observations with reasonable confidence permitting the formulation of potential mechanisms for several previously unexplained halogen phenomena including the enrichment of Br− in submicron aerosol, and the presence of a BrO maximum in the polar free troposphere. However, simulated total volatile Br mixing ratios were generally high in the troposphere. Br in the stratosphere was lower than observed due to the lack of long-lived organobromine species in the simulation. Comparing simulations using chemical mechanisms with and without reactive Cl and Br species demonstrated a significant temporal and spatial sensitivity of primary atmospheric oxidants (O3, HOx, NOx), CH4, and non-methane hydrocarbons (NMHC's) to halogen cycling. Simulated O3 and NOx were globally lower (65% and 35%, respectively, less in the planetary boundary layer based on median values) in simulations that included halogens. Globally, little impact was seen in SO2 and non-sea-salt SO42− processing due to halogens. Significant regional differences were evident: the lifetime of nss-SO42− was extended downwind of large sources of SO2. The burden and lifetime of DMS (and its oxidation products) were lower by a factor of 5 in simulations that included halogens, versus those without, leading to a 20% reduction in nss-SO42− in the Southern Hemisphere planetary boundary layer based on median values.


Climate ◽  
2021 ◽  
Vol 9 (10) ◽  
pp. 150
Author(s):  
Mohamed ElBessa ◽  
Saad Mesbah Abdelrahman ◽  
Kareem Tonbol ◽  
Mohamed Shaltout

The characteristics of near surface air temperature and wind field over the Southeastern Levantine (SEL) sub-basin during the period 1979–2018 were simulated. The simulation was carried out using a dynamical downscaling approach, which requires running a regional climate model system (RegCM-SVN6994) on the study domain, using lower-resolution climate data (i.e., the fifth generation of ECMWF atmospheric reanalysis of the global climate ERA5 datasets) as boundary conditions. The quality of the RegCM-SVN simulation was first verified by comparing its simulations with ERA5 for the studied region from 1979 to 2018, and then with the available five WMO weather stations from 2007 to 2018. The dynamical downscaling results proved that RegCM-SVN in its current configuration successfully simulated the observed surface air temperature and wind field. Moreover, RegCM-SVN was proved to provide similar or even better accuracy (during extreme events) than ERA5 in simulating both surface air temperature and wind speed. The simulated annual mean T2m by RegCM-SVN (from 1979 to 2018) was 20.9 °C, with a positive warming trend of 0.44 °C/decade over the study area. Moreover, the annual mean wind speed by RegCM-SVN was 4.17 m/s, demonstrating an annual negative trend of wind speed over 92% of the study area. Surface air temperatures over SEL mostly occurred within the range of 4–31 °C; however, surface wind speed rarely exceeded 10 m/s. During the study period, the seasonal features of T2m showed a general warming trend along the four seasons and showed a wind speed decreasing trend during spring and summer. The results of the RegCM-SVN simulation constitute useful information that could be utilized to fully describe the study area in terms of other atmospheric parameters.


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