New particle formation in the Arctic atmosphere is an important source of aerosol particles. Understanding the processes of Arctic secondary aerosol formation is crucial due to their significant impact on cloud properties and therefore Arctic amplification. We observed the molecular formation of new particles from low‐volatility vapors at two Arctic sites with differing surroundings. In Svalbard, sulfuric acid (SA) and methane sulfonic acid (MSA) contribute to the formation of secondary aerosol and to some extent to cloud condensation nuclei (CCN). This occurs via ion‐induced nucleation of SA and NH₃ and subsequent growth by mainly SA and MSA condensation during springtime and highly oxygenated organic molecules during summertime. By contrast, in an ice‐covered region around Villum, we observed new particle formation driven by iodic acid but its concentration was insufficient to grow nucleated particles to CCN sizes. Our results provide new insight about sources and precursors of Arctic secondary aerosol particles.

A systematic study of black carbon (BC) vertical profiles measured at high-resolution over three Italian basin valleys (Terni Valley, Po Valley and Passiria Valley) is presented. BC vertical profiles are scarcely available in literature. The campaign lasted 45 days and resulted in 120 measured vertical profiles. Besides the BC mass concentration, measurements along the vertical profiles also included aerosol size distributions in the optical particle counter range, chemical analysis of filter samples and a full set of meteorological parameters. Using the collected experimental data, we performed calculations of aerosol optical properties along the vertical profiles. The results, validated with AERONET data, were used as inputs to a radiative transfer model (libRadtran). The latter allowed an estimation of vertical profiles of the aerosol direct radiative effect, the atmospheric absorption and the heating rate in the lower troposphere. The present measurements revealed some common behaviors over the studied basin valleys. Specifically, at the mixing height, marked concentration drops of both BC (range: from −48.4 ± 5.3 to −69.1 ± 5.5%) and aerosols (range: from −23.9 ± 4.3 to −46.5 ± 7.3%) were found. The measured percentage decrease of BC was higher than that of aerosols: therefore, the BC aerosol fraction decreased upwards. Correspondingly, both the absorption and scattering coefficients decreased strongly across the mixing layer (range: from −47.6 ± 2.5 to −71.3 ± 3.0% and from −23.5 ± 0.8 to −61.2 ± 3.1%, respectively) resulting in a single-scattering albedo increase along height (range: from +4.9 ± 2.2 to +7.4 ± 1.0%). This behavior influenced the vertical distribution of the aerosol direct radiative effect and of the heating rate. In this respect, the highest atmospheric absorption of radiation was predicted below the mixing height (~ 2–3 times larger than above it) resulting in a heating rate characterized by a vertical negative gradient (range: from −2.6 ± 0.2 to −8.3 ± 1.2 K day−1 km−1). In conclusion, the present results suggest that the BC below the mixing height has the potential to promote a negative feedback on the atmospheric stability over basin valleys, weakening the ground-based thermal inversions and increasing the dispersal conditions.

We present results from a systematic study of vertical profiles of aerosol number size distribution and black carbon (BC) concentrations conducted in the Arctic, over Ny-Ålesund (Svalbard). The campaign lasted 2 years (2011–2012) and resulted in 200 vertical profiles measured by means of a tethered balloon (up to 1200 m a.g.l.) during the spring and summer seasons. In addition, chemical analysis of filter samples, aerosol size distribution and a full set of meteorological parameters were determined at ground. The collected experimental data allowed a classification of the vertical profiles into different typologies, which allowed us to describe the seasonal phenomenology of vertical aerosol properties in the Arctic. During spring, four main types of profiles were found and their behavior was related to the main aerosol and atmospheric dynamics occurring at the measuring site. Background conditions generated homogenous profiles. Transport events caused an increase of aerosol concentration with altitude. High Arctic haze pollution trapped below thermal inversions promoted a decrease of aerosol concentration with altitude. Finally, ground-based plumes of locally formed secondary aerosol determined profiles with decreasing aerosol concentration located at different altitude as a function of size. During the summer season, the impact from shipping caused aerosol and BC pollution plumes to be constrained close to the ground, indicating that increasing shipping emissions in the Arctic could bring anthropogenic aerosol and BC in the Arctic summer, affecting the climate.

The atom–bond pairwise additive approach, recently introduced by us to describe the potential energy surface for atom–molecule cases, is extended here for the first time to molecule–molecule systems. The idea is to decompose the van der Waals interaction energy into bond–bond pair contributions. This must be considered an improvement with respect to the familiar atom–atom pairwise additive representation since, still using a simple formulation, it indirectly accounts for three body effects. Such an approach also allows to include, in a straightforward way, the effect of the bond length on the intermolecular interaction energy. Cases of study are the weakly bound complexes involving the H₂ and N₂ molecules, namely N₂–H₂ and N₂–N₂, here described as a single bond–bond pair. For both systems ab initio calculations and experimental molecular beam scattering data, as well as second virial coefficients, have been employed to test the accuracy of the chosen representation of the interaction and to improve the obtained potential energy surfaces. The results of this work are important also for the generalization to the cases involving molecular ions and polyatomic molecules.