Context. The variable Sun is the most likely candidate for the natural forcing of past climate changes on time scales of 50 to 1000 years. Evidence for this understanding is that the terrestrial climate correlates positively with the solar activity. During the past 10 000 years, the Sun has experienced the substantial variations in activity and there have been numerous attempts to reconstruct solar irradiance. While there is general agreement on how solar forcing varied during the last several hundred years -all reconstructions are proportional to the solar activity -there is scientific controversy on the magnitude of solar forcing. Aims. We present a reconstruction of the total and spectral solar irradiance covering 130 nm-10 μm from 1610 to the present with an annual resolution and for the Holocene with a 22-year resolution. Methods. We assume that the minimum state of the quiet Sun in time corresponds to the observed quietest area on the present Sun. Then we use available long-term proxies of the solar activity, which are 10 Be isotope concentrations in ice cores and 22-year smoothed neutron monitor data, to interpolate between the present quiet Sun and the minimum state of the quiet Sun. This determines the longterm trend in the solar variability, which is then superposed with the 11-year activity cycle calculated from the sunspot number. The time-dependent solar spectral irradiance from about 7000 BC to the present is then derived using a state-of-the-art radiation code. Results. We derive a total and spectral solar irradiance that was substantially lower during the Maunder minimum than the one observed today. The difference is remarkably larger than other estimations published in the recent literature. The magnitude of the solar UV variability, which indirectly affects the climate, is also found to exceed previous estimates. We discuss in detail the assumptions that lead us to this conclusion.

respectively, is mainly due to transport of planetary boundary layer air to the station. In contrast, new particle formation is responsible for the high concentrations of nucleation mode particles (D < 20 nm) which exhibited a maximum during the winter months. The relatively low seasonality found for SAi t (summer, winter values: --530, -310 cm -3) is due to gas-to-particle conversion as well as transport processes. An analysis showed that a significant fraction of nucleation mode particles were formed by photochemical reactions.

Abstract. Ambient continental-rural fine aerosol (K-puszta, Hungary, PM 1.5 ) was sampled on quartz fibre filters in winter and summer 2001. Water-soluble matter (WSM) was extracted in MilliQ-water, and, in a second step, solid phase extraction was used to isolate the less hydrophilic fraction (ISOM) of the water-soluble organic matter (WSOM) from remaining inorganic salts and "most" hydrophilic organic matter (MHOM). This approach allowed ISOM, which constitutes the major fraction of WSOM, to be isolated from ambient aerosols and investigated in pure form. Hygroscopic properties of both WSM and ISOM extracts as well as of aquatic reference fulvic and humic acids were investigated using a Hygroscopicity Tandem Differential Mobility Analyser (H-TDMA). ISOM deliquesced between 30% and 60% relative humidity (RH), and hygroscopic growth factors at 90% RH ranged from 1.08 to 1.17. The hygroscopicity of ISOM is comparable to secondary organic aerosols obtained in smog chamber experiments, but lower than the hygroscopicity of highly soluble organic acids. The hygroscopic behaviour of investigated fulvic and humic acids had similarities to ISOM, but hygroscopic growth factors were slightly smaller and deliquescence was observed at higher RH (75-85% and 85-95% RH for fulvic acid and humic acid, respectively). These differences probably originate from larger average molecular mass and lower solubility of fulvic and humic acids.Inorganic composition data, measured ISOM hygroscopicity, and a presumed value for the hygroscopicity of the small remaining MHOM fraction were used to predict hygroscopic growth of WSM extracts. Good agreement between model prediction and measured water uptake was observed with differences (by volume) ranging from +1% to −18%. While deliquescence properties of WSM extracts were mainly determined by the inorganic salts (42-53 wt % Correspondence to: E. Weingartner (ernest.weingartner@psi.ch) of WSM), the WSOM accounted for a significant fraction of particulate water. At 90% RH, according to model predictions and measurements, about 80-62% of particulate water in the samples are associated with inorganic salts and about 20-38% with WSOM. The relative contributions of both distinguished WSOM fractions, ISOM and MHOM, remains uncertain since MHOM was not available in isolated form, but the results suggest that the less abundant MHOM is also important due to its presumably larger hygroscopicity.

[1] The rapid temperature increase of 1°C over mainland Europe since 1980 is considerably larger than the temperature rise expected from anthropogenic greenhouse gas increases. Here we present aerosol optical depth measurements from six specific locations and surface irradiance measurements from a large number of radiation sites in Northern Germany and Switzerland. The measurements show a decline in aerosol concentration of up to 60%, which have led to a statistically significant increase of solar irradiance under cloud-free skies since the 1980s. The measurements confirm solar brightening and show that the direct aerosol effect had an approximately five times larger impact on climate forcing than the indirect aerosol and other cloud effects. The overall aerosol and cloud induced surface climate forcing is $+1 W m À2 dec À1 and has most probably strongly contributed to the recent rapid warming in Europe. Citation: Ruckstuhl, C., et al.

[1] An aerosol black carbon (BC) data set from ongoing measurements at Zeppelin station (474 m asl), near Ny-Å lesund (10 m asl), Svalbard is reported for the period 1998 -2007. Annual average and median BC concentrations were 39 and 27 ng m À3, respectively, while monthly averages ranged from a maximum $80 ng m À3 in February/ March to a minimum 0 -10 ng m À3 from June to September. BC concentrations were calibrated by elemental carbon thermo-optical analysis. PSCF trajectory analysis indicated that BC concentrations at Zeppelin were mainly influenced by source regions in northern and central Russia. Since 2001, a small decreasing trend in BC concentration (À9.5 ng m À3 per decade) for the period to 2007 has been observed which is, however, similar to the detection limit.

Secondary organic aerosol (SOA) formation from the photooxidation of an anthropogenic (1,3,5-trimethylbenzene) and a biogenic (alpha-pinene) precursor was investigated at the new PSI smog chamber. The chemistry of the gas phase was followed by proton transfer reaction mass spectrometry, while the aerosol chemistry was investigated with aerosol mass spectrometry, ion chromatography, laser desorption ionization mass spectrometry, and infrared spectroscopy, along with volatility and hygroscopicity studies. Evidence for oligomer formation for SOA from both precursors was given by an increasing abundance of compounds with a high molecular weight (up to 1000 Da) and by an increasing thermal stability with increasing aging time. The results were compared to data obtained from ambient aerosol samples, revealing a number of similar features.

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Abstract.Results of continuous nitrogen oxide (NO), nitrogen dioxide (NO 2 ), peroxyacetyl nitrate (PAN) and total reactive nitrogen (NO y ) measurements along with seasonal field campaigns of nitric acid (HNO 3 ) and particulate nitrate (NO − 3 ) measurements are presented for a two-year period at the high-alpine research station Jungfraujoch (JFJ), 3580 m asl. The NO y mixing ratio and partitioning is shown to strongly depend on meteorological conditions. Knowledge of these meteorological transport processes allows discrimination between undisturbed (i.e. clean) and disturbed (i.e. influenced by regional pollution sources) free tropospheric (FT) conditions at the JFJ. Median NO y concentrations during undisturbed FT periods ranged from 350 pptv (winter, December to February) to 581 pptv (spring, March to May). PAN was found to be the dominant NO y species during spring and summer, whereas NO 2 was most abundant during autumn and winter. Particulate nitrate was found to contribute significantly to total NO y during thermally induced vertical transport. Föhn events, synoptical lifting (e.g. fronts) and thermally induced vertical transport resulted in mixing ratios up to 10 times higher at the JFJ compared to undisturbed FT conditions. Furthermore this meteorological variability of the NO y concentration and partitioning often dominated the seasonal variability. As a consequence the use of filters at the JFJ (and other mountainous sites) is crucial for the interpretation of data from such measurement sites. This study presents a further development of meteorological filters for the high-alpine site Jungfraujoch, which also could be modified and adapted to other mountainous measurement sites.