Over Boreal regions, monoterpenes emitted from the forest are the main precursors for secondary organic aerosol (SOA) formation and the primary driver of the growth of new aerosol particles to climatically important cloud condensation nuclei (CCN). Autoxidation of monoterpenes leads to rapid formation of Highly Oxygenated organic Molecules (HOM). We have developed the first model with near-explicit representation of atmospheric new particle formation (NPF) and HOM formation. The model can reproduce the observed NPF, HOM gas-phase composition and SOA formation over the Boreal forest. During the spring, HOM SOA formation increases the CCN concentration by~10 % and causes a direct aerosol radiative forcing of −0.10 W/m 2. In contrast, NPF reduces the number of CCN at updraft velocities < 0.2 m/s, and causes a direct aerosol radiative forcing of +0.15 W/m 2. Hence, while HOM SOA contributes to climate cooling, NPF can result in climate warming over the Boreal forest.

Abstract. With the present demand on fast and inexpensive aerosol source apportionment methods, the Aethalometer model was evaluated for a full seasonal cycle (June 2014-June 2015 at a rural atmospheric measurement station in southern Sweden by using radiocarbon and levoglucosan measurements. By utilizing differences in absorption of UV and IR, the Aethalometer model apportions carbon mass into wood burning (WB) and fossil fuel combustion (FF) aerosol. In this study, a small modification in the model in conjunction with carbon measurements from thermal-optical analysis allowed apportioned non-light-absorbing biogenic aerosol to vary in time. The absorption differences between WB and FF can be quantified by the absorption Ångström exponent (AAE). In this study AAE WB was set to 1.81 and AAE FF to 1.0. Our observations show that the AAE was elevated during winter (1.36 ± 0.07) compared to summer (1.12 ± 0.07). Quantified WB aerosol showed good agreement with levoglucosan concentrations, both in terms of correlation (R 2 = 0.70) and in comparison to reference emission inventories. WB aerosol showed strong seasonal variation with high concentrations during winter (0.65 µg m −3 , 56 % of total carbon) and low concentrations during summer (0.07 µg m −3 , 6 % of total carbon). FF aerosol showed less seasonal dependence; however, black carbon (BC) FF showed clear diurnal patterns corresponding to traffic rush hour peaks. The presumed non-light-absorbing biogenic carbonaceous aerosol concentration was high during summer (1.04 µg m −3 , 72 % of total carbon) and low during winter (0.13 µg m −3 , 8 % of total carbon). Aethalometer model results were further compared to radiocarbon and levoglucosan source apportionment results. The comparison showed good agreement for apportioned mass of WB and biogenic carbonaceous aerosol, but discrepancies were found for FF aerosol mass. The Aethalometer model overestimated FF aerosol mass by a factor of 1.3 compared to radiocarbon and levoglucosan source apportionment. A performed sensitivity analysis suggests that this discrepancy can be explained by interference of non-light-absorbing biogenic carbon during winter. In summary, the Aethalometer model offers a costeffective yet robust high-time-resolution source apportionment at rural background stations compared to a radiocarbon and levoglucosan alternative.

Abstract. In this study, the processes behind observed new particle formation (NPF) events and subsequent organicdominated particle growth at the Pallas AtmosphereEcosystem Supersite in Northern Finland are explored with the one-dimensional column trajectory model ADCHEM. The modeled sub-micron particle mass is up to ∼ 75 % composed of SOA formed from highly oxidized multifunctional organic molecules (HOMs) with low or extremely low volatility. In the model the newly formed particles with an initial diameter of 1.5 nm reach a diameter of 7 nm about 2 h earlier than what is typically observed at the station. This is an indication that the model tends to overestimate the initial particle growth. In contrast, the modeled particle growth to CCN size ranges (> 50 nm in diameter) seems to be underestimated because the increase in the concentration of particles above 50 nm in diameter typically occurs several hours later compared to the observations. Due to the high fraction of HOMs in the modeled particles, the oxygen-to-carbon (O : C) atomic ratio of the SOA is nearly 1. This unusually high O : C and the discrepancy between the modeled and observed particle growth might be explained by the fact that the model does not consider any particle-phase reactions involving semi-volatile organic compounds with relatively low O : C. In the model simulations where condensation of lowvolatility and extremely low-volatility HOMs explain most of the SOA formation, the phase state of the SOA (assumed either liquid or amorphous solid) has an insignificant impact on the evolution of the particle number size distributions. However, the modeled particle growth rates are sensitive to the method used to estimate the vapor pressures of the HOMs. Future studies should evaluate how heterogeneous reactions involving semi-volatility HOMs and other less-oxidized organic compounds can influence the SOA composition-and size-dependent particle growth.

Fresh and aged diesel soot particles have different impacts on climate and human health. While fresh diesel soot particles are highly aspherical and non-hygroscopic, aged particles are spherical and hygroscopic. Aging and its effect on water uptake also controls the dispersion of diesel soot in the atmosphere. Understanding the timescales on which diesel soot ages in the atmosphere is thus important, yet knowledge thereof is lacking. We show that under cold, dark and humid conditions the atmospheric transformation from fresh to aged soot occurs on a timescale of less than five hours. Under dry conditions in the laboratory, diesel soot transformation is much less efficient. While photochemistry drives soot aging, our data show it is not always a limiting factor. Field observations together with aerosol process model simulations show that the rapid ambient diesel soot aging in urban plumes is caused by coupled ammonium nitrate formation and water uptake.

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