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Particle hygroscopicity during atmospheric new particle formation events: Implications for the chemical species contributing to particle growth
2013, Wu, Z., Birmili, W., Poulain, L., Poulain, L., Merkel, M., Fahlbusch, B., Van Pinxteren, D., Herrmann, H., Wiedensohler, A.
This study examines the hygroscopicity of newly formed particles (diameters range 25-45 nm) during two atmospheric new particle formation (NPF) events in the German mid-level mountains during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) field experiment. At the end of the NPF event involving clear particle growth, we measured an unusually high soluble particle fraction of 58.5% at 45 nm particle size. The particle growth rate contributed through sulfuric acid condensation only accounts for around 6.5% of the observed growth rate. Estimations showed that sulfuric acid condensation explained, however, only around 10% of that soluble particle fraction. Therefore, the formation of additional water-soluble matter appears imperative to explain the missing soluble fraction. Although direct evidence is missing, we consider water-soluble organics as candidates for this mechanism. For the case with clear growth process, the particle growth rate was determined by two alternative methods based on tracking the mode diameter of the nucleation mode. The mean particle growth rate obtained from the inter-site data comparison using Lagrangian consideration is 3.8 (± 2.6) nm h-1. During the same period, the growth rate calculated based on one site data is 5.0 nm h-1 using log-normal distribution function method. In light of the fact that considerable uncertainties could be involved in both methods, we consider both estimated growth rates consistent.
Global annual methane emission rate derived from its current atmospheric mixing ratio and estimated lifetime
2014, Sonnemann, G.R., Grygalashvyly, M.
We use the estimated lifetime of methane (CH4), the current methane concentration, and its annual growth rate to calculate the global methane emission rate. The upper and lower limits of the annual global methane emission rate, depending on loss of CH4 into the stratosphere and methane consuming bacteria, amounts to 648.0 Mt a-1 and 608.0 Mt a-1. These values are in reasonable agreement with satellite and with much more accurate in situ measurements of methane. We estimate a mean tropospheric and mass-weighted temperature related to the reaction rate and employ a mean OH-concentration to calculate a mean methane lifetime. The estimated atmospheric lifetime of methane amounts to 8.28 years and 8.84 years, respectively. In order to improve the analysis a realistic 3D-calculations should be performed.
Zonal asymmetries in middle atmospheric ozone and water vapour derived from Odin satellite data 2001-2010
2011, Gabriel, A., Körnich, H., Lossow, S., Peters, D.H.W., Urban, J., Murtagh, D.
Stationary wave patterns in middle atmospheric ozone (O3) and water vapour (H2O) are an important factor in the atmospheric circulation, but there is a strong gap in diagnosing and understanding their configuration and origin. Based on Odin satellite data from 2001 to 2010 we investigate the stationary wave patterns in O3 and H2O as indicated by the seasonal long-term means of the zonally asymmetric components O3* Combining double low line O3-[O3] and H2O* Combining double low line H2O-[H2O] ([O3], [H2O]: zonal means). At mid-and polar latitudes we find a pronounced wave one pattern in both constituents. In the Northern Hemisphere, the wave patterns increase during autumn, maintain their strength during winter and decay during spring, with maximum amplitudes of about 10-20 % of the zonal mean values. During winter, the wave one in O3* shows a maximum over the North Pacific/Aleutians and a minimum over the North Atlantic/Northern Europe and a double-peak structure with enhanced amplitude in the lower and in the upper stratosphere. The wave one in H2O* extends from the lower stratosphere to the upper mesosphere with a westward shift in phase with increasing height including a jump in phase at upper stratosphere altitudes. In the Southern Hemisphere, similar wave patterns occur mainly during southern spring. By comparing the observed wave patterns in O 3* and H2O3* with a linear solution of a steady-state transport equation for a zonally asymmetric tracer component we find that these wave patterns are primarily due to zonally asymmetric transport by geostrophically balanced winds, which are derived from observed temperature profiles. In addition temperature-dependent photochemistry contributes substantially to the spatial structure of the wave pattern in O 3* . Further influences, e.g., zonal asymmetries in eddy mixing processes, are discussed.
Effective CO2 lifetime and future CO2 levels based on fit function
2013, Sonnemann, G.R., Grygalashvyly, M.
The estimated global CO2 emission rates and the measured atmospheric CO2 concentrations show that only a certain share of the emitted CO2 accumulates in the atmosphere. For given atmospheric emissions of CO2, the effective lifetime determines its accumulation in the atmosphere and, consequently, its impact on the future global warming. We found that on average the inferred effective lifetime of CO2 decreases as its atmospheric concentration increases, reducing the rate of its accumulation in the atmosphere. We derived a power function that fits the varying lifetimes. Based on this fitting function, we calculated the increase of CO2 for different scenarios of future global emission rates.