Abstract. The climate in the Arctic is changing faster than anywhere else on earth. Poorly understood feedback processes relating to Arctic clouds and aerosol-cloud interactions contribute to a poor understanding of the present changes in the Arctic climate system, and also to a large spread in projections of future climate in the Arctic. The problem is exacerbated by the paucity of research-quality observations in the central Arctic. Improved formulations in climate models require such observations, which can only come from measurements in situ in this difficult-to-reach region with logistically demanding environmental conditions.The Arctic Summer Cloud Ocean Study (ASCOS) was the most extensive central Arctic Ocean expedition with an atmospheric focus during the International Polar Year (IPY) [2007][2008]. ASCOS focused on the study of the formation and life cycle of low-level Arctic clouds. ASCOS departed from Longyearbyen on Svalbard on 2 August and returned on 9 September 2008. In transit into and out of the pack ice, four short research stations were undertaken in the Fram Strait: two in open water and two in the marginal ice zone. After traversing the pack ice northward, an ice camp was set up on 12 August at 87 • 21 N, 01 • 29 W and remained in operation through 1 September, drifting with the ice. During this time, extensive measurements were taken of atmospheric gas and particle chemistry and physics, mesoscale and boundarylayer meteorology, marine biology and chemistry, and upper ocean physics.ASCOS provides a unique interdisciplinary data set for development and testing of new hypotheses on cloud processes, their interactions with the sea ice and ocean and associated physical, chemical, and biological processes and interactions. For example, the first-ever quantitative observation of bubbles in Arctic leads, combined with the unique discovery of marine organic material, polymer gels with an origin in the ocean, inside cloud droplets suggests the possibility of primary marine organically derived cloud condensation nuclei in Arctic stratocumulus clouds. Direct observations of surface fluxes of aerosols could, however, not explain observed variability in aerosol concentrations, and the balance between local and remote aerosols sources remains open. Lack of cloud condensation nuclei (CCN) was at times a controlling factor in low-level cloud formation, and hence for the impact of clouds on the surface energy budget. AS-COS provided detailed measurements of the surface energy balance from late summer melt into the initial autumn freezeup, and documented the effects of clouds and storms on the surface energy balance during this transition. In addition to such process-level studies, the unique, independent ASCOS data set can and is being used for validation of satellite retrievals, operational models, and reanalysis data sets.

Abstract.We have combined chemical and micrometeorological measurements to investigate the formation and distribution of HONO throughout a forest canopy. HONO was measured simultaneously at two heights, close to the forest floor and just above canopy. The turbulent exchange between the forest and the atmosphere above was studied using vertical profiles of eddy covariance measurements of wind velocity, sonic temperature, water vapour and CO 2 . HONO mixing ratios at both heights showed typical diel cycles with low daytime values (∼80 ppt) and high nighttime values (up to 500 ppt), but were influenced by various sources and sinks leading to mixing ratio differences (above canopy minus below) of up to +240 ppt at nighttime. In the late afternoon and early night mixing ratios increased at higher rates near the forest floor, indicating a possible ground source. Due to the simultaneous decoupling of the forest from the air layer above the canopy, mixing ratio differences reached about −170 ppt. From the late night until the early morning mixing ratios above the forest were typically higher than close to the forest floor. For some cases, this could be attributed to advection above the forest, which only partly penetrated the canopy. Measured photolysis frequencies above and below the forest canopy differed by a factor of 10-25 resulting in HONO lifetimes of about 10 min above and 100-250 min below the canopy at noontime. However, these differences of the main daytime HONO sink were not evident in the mixing ratio differences, which were close to zero during the morning hours. Effective turbulent exchange due to a complete coupling of the forest to the air layer above the canopy in Correspondence to: M. Sörgel (matthias.soergel@uni-bayreuth.de) the morning has offset the differences caused by the daytime photolytic sink and added to the interplay between different HONO production and loss processes.

Abstract. New particle formation is of interest because of its influence on the properties of aerosol population, and due to the possible contribution of newly formed particles to cloud condensation nuclei. Currently no conclusive evidence exists as to the mechanism or mechanisms of nucleation and subsequent particle growth. However, nucleation rates exhibit a clear dependence on ambient sulphuric acid concentrations and particle growth is often attributed to the condensation of organic vapours. A detailed study of new particle formation in the Front Range of the Colorado Rocky Mountains is presented here. Gas and particle measurement data for 32 days was analyzed to identify event days, possible event days, and non-event days. A detailed analysis of nucleation and growth is provided for four days on which new particle formation was clearly observed. Evidence for the role of sesquiterpenes in new particle formation is presented.

Gaseous nitrogen dioxide (NO2) represents an oxidant that is present in relatively high concentrations in various indoor settings. Remarkably increased NO2 levels up to 1.5 ppm are associated with homes using gas stoves. The heterogeneous reactions of NO2 with adsorbed water on surfaces lead to the generation of nitrous acid (HONO). Here, we present a HONO source induced by heterogeneous reactions of NO2 with selected indoor paint surfaces in the presence of light (300 nm<λ<400 nm). We demonstrate that the formation of HONO is much more pronounced at elevated relative humidity. In the presence of light (5.5 W m(-2)), an increase of HONO production rate of up to 8.6·10(9) molecules cm(-2) s(-1) was observed at [NO2]=60 ppb and 50% relative humidity (RH). At higher light intensity of 10.6 (W m(-2)), the HONO production rate increased to 2.1·10(10) molecules cm(-2) s(-1). A high NO2 to HONO conversion yield of up to 84% was observed. This result strongly suggests that a light-driven process of indoor HONO production is operational. This work highlights the potential of paint surfaces to generate HONO within indoor environments by light-induced NO2 heterogeneous reactions.

During the DOMINO (Diel Oxidant Mechanism In relation to Nitrogen Oxides) campaign in southwest Spain we measured simultaneously all quantities necessary to calculate a photostationary state for HONO in the gas phase. These quantities comprise the concentrations of OH, NO, and HONO and the photolysis frequency of NO₂, j(NO₂) as a proxy for j(HONO). This allowed us to calculate values of the unknown HONO daytime source. This unknown HONO source, normalized by NO₂ mixing ratios and expressed as a conversion frequency (% h⁻¹), showed a clear dependence on j(NO₂) with values up to 43 % h⁻¹ at noon. We compared our unknown HONO source with values calculated from the measured field data for two recently proposed processes, the light-induced NO₂ conversion on soot surfaces and the reaction of electronically excited NO₂* with water vapour, with the result that these two reactions normally contributed less than 10 % (<1 % NO₂ + soot + hν; and <10 % NO₂* + H₂O) to our unknown HONO daytime source. OH production from HONO photolysis was found to be larger (by 20 %) than the "classical" OH formation from ozone photolysis (O(¹D)) integrated over the day

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The climate in the Arctic is changing faster than anywhere else on Earth. Poorly understood feedback processes relating to Arctic clouds and aerosol-cloud interactions contribute to a poor understanding of the present changes in the Arctic climate system, and also to a large spread in projections of future climate in the Arctic. The problem is exacerbated by the paucity of research-quality observations in the central Arctic. Improved formulations in climate models require such observations, which can only come from measurements in-situ in this difficult to reach region with logistically demanding environmental conditions.

The Arctic Summer Cloud-Ocean Study (ASCOS) was the most extensive central Arctic Ocean expedition with an atmospheric focus during the International Polar Year (IPY) 2007–2008. ASCOS focused on the study of the formation and life cycle of low-level Arctic clouds. ASCOS departed from Longyearbyen on Svalbard on 2 August and returned on 9 September 2008. In transit into and out of the pack ice, four short research stations were undertaken in the Fram Strait; two in open water and two in the marginal ice zone. After traversing the pack-ice northward an ice camp was set up on 12 August at 87°21' N 01°29' W and remained in operation through 1 September, drifting with the ice. During this time extensive measurements were taken of atmospheric gas and particle chemistry and physics, mesoscale and boundary-layer meteorology, marine biology and chemistry, and upper ocean physics.

ASCOS provides a unique interdisciplinary data set for development and testing of new hypotheses on cloud processes, their interactions with the sea ice and ocean and associated physical, chemical, and biological processes and interactions. For example, the first ever quantitative observation of bubbles in Arctic leads, combined with the unique discovery of marine organic material, polymer gels with an origin in the ocean, inside cloud droplets suggest the possibility of primary marine organically derived cloud condensation nuclei in Arctic stratocumulus clouds. Direct observations of surface fluxes of aerosols could, however, not explain observed variability in aerosol concentrations and the balance between local and remote aerosols sources remains open. Lack of CCN was at times a controlling factor in low-level cloud formation, and hence for the impact of clouds on the surface energy budget. ASCOS provided detailed measurements of the surface energy balance from late summer melt into the initial autumn freeze-up, and documented the effects of clouds and storms on the surface energy balance during this transition. In addition to such process-level studies, the unique, independent ASCOS data set can and is being used for validation of satellite retrievals, operational models, and reanalysis data sets

The Canopy Horizontal Array Turbulence Study (CHATS) took place in spring 2007 and is the third in the series of Horizontal Array Turbulence Study (HATS) experiments. The HATS experiments have been instrumental in testing and developing subfilterscale (SFS) models for large-eddy simulation (LES) of planetary boundary layer (PBL) turbulence. The CHATS campaign took place in a deciduous walnut orchard near Dixon, California, and was designed to examine the impacts of vegetation on SFS turbulence. Measurements were collected both prior to and following leafout to capture the impact of leaves on the turbulence, stratification, and scalar source/sink distribution. CHATS utilized crosswind arrays of fast-response instrumentation to investigate the impact of the canopy-imposed distribution of momentum extraction and scalar sources on SFS transport of momentum, energy, and three scalars. To directly test and link with PBL parameterizations of canopy-modified turbulent exchange, CHATS also included a 30-m profile tower instrumented with turbulence instrumentation, fast and slow chemical sensors, aerosol samplers, and radiation instrumentation. A highresolution scanning backscatter lidar characterized the turbulence structure above and within the canopy; a scanning Doppler lidar, mini sodar/radio acoustic sounding system (RASS), and a new helicopter-observing platform provided details of the PBL-scale flow. Ultimately, the CHATS dataset will lead to improved parameterizations of energy and scalar transport to and from vegetation, which are a critical component of global and regional land, atmosphere, and chemical models. This manuscript presents an overview of the experiment, documents the regime sampled, and highlights some preliminary key findings.