ALBERT

Description: Highlights: • Oscillations with 2–5 yr periods are found in atmospheric temperatures from 0–100 km. • They show very special amplitude and phase profiles. • They are found to be self-sustained. • They appear to show period and phase synchronization. Abstract: SABER temperature measurements from 2002 to 2012 are analyzed from 18 to 110 km altitude in Middle Europe. Data are complemented by radiosonde measurements in the altitude range from 0 to 30 km. Low frequency oscillations with periods of about 2.4-2.2 yr, 3.4 yr, and 5.5 yr are seen in either data set. Surprising vertical structures in amplitudes and phases are observed with alternating minima and maxima of amplitudes, steep phase changes (180°) at the altitudes of the minima, and constant phase values in between. HAMMONIA CCM simulations driven by boundary conditions for the years 1996 to 2006 are analyzed for corresponding features, and very similar structures are found. Data from another CCM, the CESM-WACCM model, are also analyzed and show comparable results. Similar oscillation periods have been reported in the literature for the ocean. A possible forcing of the atmospheric oscillations from below was therefore tested with a special HAMMONIA run. Here, climatological boundary conditions were used, i.e. the boundaries in all eleven years were the same. Surprisingly also in this data set the same atmospheric oscillations are obtained. We therefore conclude that the oscillations are intrinsically forced, self-sustained in the atmosphere. The oscillations turned out to be quite robust as they are still found in a HAMMONIA run with strongly reduced vertical resolution. Here only the form of the vertical amplitude and phase profile of the 2.2 yr feature is lost but the oscillation itself is still there, and the two other oscillations are essentially unchanged. Similar oscillations are seen in the earth surface temperatures. Global Land Ocean Temperature Index data (GLOTI) reaching back to 1880 show such oscillations during all that time. The oscillations are also seen in parameters other than atmospheric temperature. They are found in surface data such as the North Atlantic Oscillation Index (NAO) and in zonal winds in the troposphere and lower stratosphere. The oscillations found are tentatively discussed in terms (of synchronization) of self-sustained non-linear oscillators, as many of their properties resemble such oscillators described in the literature.

Description: Abstract. It has been claimed for more than a century that atmospheric new particle formation is primarily influenced by the presence of sulfuric acid. However, the activation process of sulfuric acid related clusters into detectable particles is still an unresolved topic. In this study we focus on the PARADE campaign measurements conducted during August/September 2011 at Mt Kleiner Feldberg in central Germany. During this campaign a set of radicals, organic and inorganic compounds and oxidants and aerosol properties were measured or calculated. We compared a range of organic and inorganic nucleation theories, evaluating their ability to simulate measured particle formation rates at 3 nm in diameter (J3) for a variety of different conditions. Nucleation mechanisms involving only sulfuric acid tentatively captured the observed noon-time daily maximum in J3, but displayed an increasing difference to J3 measurements during the rest of the diurnal cycle. Including large organic radicals, i.e. organic peroxy radicals (RO2) deriving from monoterpenes and their oxidation products, in the nucleation mechanism improved the correlation between observed and simulated J3. This supports a recently proposed empirical relationship for new particle formation that has been used in global models. However, the best match between theory and measurements for the site of interest was found for an activation process based on large organic peroxy radicals and stabilised Criegee intermediates (sCI). This novel laboratory-derived algorithm simulated the daily pattern and intensity of J3 observed in the ambient data. In this algorithm organic derived radicals are involved in activation and growth and link the formation rate of smallest aerosol particles with OH during daytime and NO3 during night-time. Because the RO2 lifetime is controlled by HO2 and NO we conclude that peroxy radicals and NO seem to play an important role for ambient radical chemistry not only with respect to oxidation capacity but also for the activation process of new particle formation. This is supposed to have significant impact of atmospheric radical species on aerosol chemistry and should be taken into account when studying the impact of new particles in climate feedback cycles.