Black carbon (BC) is now mainly of anthropogenic origin. It is the dominant light absorbing component of atmospheric aerosols, playing an important role in the earth's radiative balance and therefore relevant to climate change studies. In addition, BC is known to be harmful to human beings making it relevant to policy makers. Nevertheless, the measurement of BC remains biased by the instrument-based definition of BC. The Single Particle Soot Photometer (SP2), allows the measurement of the refractory BC (rBC) mass of individual particles using laser-induced incandescence. However, the SP2 needs an empirical calibration to retrieve the rBC mass from the incandescence signal and the sensitivity of the SP2 differs between different BC types. Ideally, for atmospheric studies, the SP2 should be calibrated using ambient particles containing a known mass of ambient rBC. However, such "ambient BC" calibration particles cannot easily be obtained and thus commercially available BC particles are commonly used for SP2 calibration instead. In this study we tested the sensitivity of the SP2 to different BC types in order to characterize the potential error introduced by using non-ambient BC for calibration. The sensitivity of the SP2 was determined, using an aerosol particle mass analyzer, for rBC from thermodenuded diesel exhaust, wood burning exhaust and ambient particles as well as for commercially available products: Aquadag^® and fullerene soot. <br><br> Thermodenuded, fresh diesel exhaust has been found to be ideal for SP2 calibration for two reasons. First, the small amount of non-BC matter upon emission reduces the risk of bias due to incomplete removal of non-BC matter and second, it is considered to represent atmospheric rBC in urban locations where diesel exhaust is the main source of BC. The SP2 was found to be up to 16% less sensitive to rBC from thermodenuded ambient particles (&le;15 fg) than rBC from diesel exhaust, however, at least part of this difference can be explained by incomplete removal of non-refractory components in the thermodenuder. The amount of remaining non-refractory matter was estimated to be below 30% by mass, according to a comparison of the scattering cross sections of the whole particles with that of the pure BC cores. The SP2 sensitivity to rBC from wood burning exhaust agrees with the SP2 sensitivity to rBC from diesel exhaust within an error of less than 14% (&le;40 fg). <br><br> If, due to experimental restrictions, diesel exhaust cannot be used, untreated fullerene soot was found to give an SP2 calibration curve similar to diesel exhaust and ambient rBC (within ±10% for a rBC mass &le;15 fg) and is therefore recommended although two different batches differed by ~14% between themselves. In addition, the SP2 was found to be up to 40% more sensitive to Aquadag^® than to diesel exhaust rBC. Therefore Aquadag^® cannot be recommended for atmospheric application without accounting for the se...

In the central Arctic Ocean the formation of clouds and their properties are sensitive to the availability of cloud condensation nuclei (CCN). The vapors responsible for new particle formation (NPF), potentially leading to CCN, have remained unidentified since the first aerosol measurements in 1991. Here, we report that all the observed NPF events from the Arctic Ocean 2018 expedition are driven by iodic acid with little contribution from sulfuric acid. Iodic acid largely explains the growth of ultrafine particles (UFP) in most events. The iodic acid concentration increases significantly from summer towards autumn, possibly linked to the ocean freeze-up and a seasonal rise in ozone. This leads to a one order of magnitude higher UFP concentration in autumn. Measurements of cloud residuals suggest that particles smaller than 30 nm in diameter can activate as CCN. Therefore, iodine NPF has the potential to influence cloud properties over the Arctic Ocean.

Abstract. The effect of aerosol water uptake on the aerosol particle light scattering coefficient (σ sp ) is described in this study by comparing measurements from five European sites: the Jungfraujoch, located in the Swiss Alps at 3580 m a.s.l.; Ny-Ålesund, located on Spitsbergen in the Arctic; Mace Head, a coastal site in Ireland; Cabauw, a rural site in the Netherlands; and Melpitz, a regional background site in Eastern Germany. These sites were selected according to the aerosol type usually encountered at that location. The scattering enhancement factor f (RH, λ) is the key parameter to describe the effect of water uptake on the particle light scattering. It is defined as the σ sp (RH) at a certain relative humidity (RH) and wavelength λ divided by its dry value. f (RH) at the five sites varied widely, starting at very low values of f (RH = 85 %, λ = 550 nm) around 1.28 for mineral dust, and reaching up to 3.41 for Arctic aerosol. Hysteresis behavior was observed at all sites except at the Jungfraujoch (due to the absence of sea salt). Closure studies and Mie simulations showed that both size and chemical composition determine the magnitude of f (RH). Both parameters are also needed to successfully predict f (RH). Finally, the measurement results were compared to the widely used aerosol model, OPAC (Hess et al., 1998). Significant discrepancies were seen, especially at intermediate RH ranges; these were mainly attributed to inappropriate implementation of hygroscopic growth in the OPAC model. Replacement of the hygroscopic growth with values from the recent literature resulted in a clear improvement of the OPAC model.

Sea spray is one of the largest natural aerosol sources and plays an important role in the Earth’s radiative budget. These particles are inherently hygroscopic, that is, they take-up moisture from the air, which affects the extent to which they interact with solar radiation. We demonstrate that the hygroscopic growth of inorganic sea salt is 8–15% lower than pure sodium chloride, most likely due to the presence of hydrates. We observe an increase in hygroscopic growth with decreasing particle size (for particle diameters <150 nm) that is independent of the particle generation method. We vary the hygroscopic growth of the inorganic sea salt within a general circulation model and show that a reduced hygroscopicity leads to a reduction in aerosol-radiation interactions, manifested by a latitudinal-dependent reduction of the aerosol optical depth by up to 15%, while cloud-related parameters are unaffected. We propose that a value of κs=1.1 (at RH=90%) is used to represent the hygroscopicity of inorganic sea salt particles in numerical models.

Abstract. Aerosol particles experience hygroscopic growth in the ambient atmosphere. Their optical properties -especially the aerosol light scattering -are therefore strongly dependent on the ambient relative humidity (RH). In-situ light scattering measurements of long-term observations are usually performed under dry conditions (RH<30-40%). The knowledge of this RH effect is of eminent importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements. This study combines measurements and model calculations to describe the RH effect on aerosol light scattering for the first time for aerosol particles present in summer and fall in the high Arctic. For this purpose, a field campaign was carried out from July to October 2008 at the Zeppelin station in Ny-Ålesund, Svalbard. The aerosol light scattering coefficient σ sp (λ) was measured at three distinct wavelengths (λ=450, 550, and 700 nm) at dry and at various, predefined RH conditions between 20% and 95% with a recently developed humidified nephelometer (WetNeph) and with a second nephelometer measuring at dry conditions with an average RH<10% (DryNeph). In addition, the aerosol size distribution and the aerosol absorption coefficient were measured. The scattering enhancement factor f (RH, λ) is the key parameter to describe the RH effect on σ sp (λ) and is defined as the RH dependent σ sp (RH, λ) divided by the corresponding dry σ sp (RH dry ,λ). During our campaign the average f (RH=85%, λ=550 nm) was 3.24±0.63 (mean ± standard deviation), and no clear wavelength dependence of f (RH, λ) was observed. This means that the ambient scattering coefficients at RH=85% were on average about three times higher than the dry meaCorrespondence to: E. Weingartner (ernest.weingartner@psi.ch) sured in-situ scattering coefficients. The RH dependency of the recorded f (RH, λ) can be well described by an empirical one-parameter equation. We used a simplified method to retrieve an apparent hygroscopic growth factor g(RH), defined as the aerosol particle diameter at a certain RH divided by the dry diameter, using the WetNeph, the DryNeph, the aerosol size distribution measurements and Mie theory. With this approach we found, on average, g(RH = 85%) values to be 1.61±0.12 (mean±standard deviation). No clear seasonal shift of f (RH, λ) was observed during the 3-month period, while aerosol properties (size and chemical composition) clearly changed with time. While the beginning of the campaign was mainly characterized by smaller and less hygroscopic particles, the end was dominated by larger and more hygroscopic particles. This suggests that compensating effects of hygroscopicity and size determined the temporal stability of f (RH, λ). During sea salt influenced periods, distinct deliquescence transitions were observed. At the end we present a method on how to transfer the dry in-situ measured aerosol scattering coefficients to ambient values for the aerosol measured during summer and fall at this location.

Abstract.We have developed an inorganic sea spray source function that is based upon state-of-the-art measurements of sea spray aerosol production using a temperature-controlled plunging jet sea spray aerosol chamber. The size-resolved particle production was measured between 0.01 and 10 µm dry diameter. Particle production decreased non-linearly with increasing seawater temperature (between −1 and 30 • C) similar to previous findings. In addition, we observed that the particle effective radius, as well as the particle surface, particle volume and particle mass, increased with increasing seawater temperature due to increased production of particles with dry diameters greater than 1 µm. By combining these measurements with the volume of air entrained by the plunging jet we have determined the size-resolved particle flux as a function of air entrainment. Through the use of existing parameterisations of air entrainment as a function of wind speed, we were subsequently able to scale our laboratory measurements of particle production to wind speed. By scaling in this way we avoid some of the difficulties associated with defining the "white area" of the laboratory whitecap -a contentious issue when relating laboratory measurements of particle production to oceanic whitecaps using the more frequently applied whitecap method.The here-derived inorganic sea spray source function was implemented in a Lagrangian particle dispersion model (FLEXPART -FLEXible PARTicle dispersion model). An estimated annual global flux of inorganic sea spray aerosol of 5.9 ± 0.2 Pg yr −1 was derived that is close to the median of estimates from the same model using a wide range of existing sea spray source functions. When using the source function derived here, the model also showed good skill in predicting measurements of Na + concentration at a number of field sites further underlining the validity of our source function.In a final step, the sensitivity of a large-scale model (NorESM -the Norwegian Earth System Model) to our new source function was tested. Compared to the previously implemented parameterisation, a clear decrease of sea spray aerosol number flux and increase in aerosol residence time was observed, especially over the Southern Ocean. At the same time an increase in aerosol optical depth due to an increase in the number of particles with optically relevant sizes was found. That there were noticeable regional differences may have important implications for aerosol optical properties and number concentrations, subsequently also affecting the indirect radiative forcing by non-sea spray anthropogenic aerosols.

Abstract. In the field, aerosol in-situ measurements are often performed under dry conditions (relative humidity RH<30-40%). Since ambient aerosol particles experience hygroscopic growth at enhanced RH, their microphysical and optical properties -especially the aerosol light scatteringare also strongly dependent on RH. The knowledge of this RH effect is of crucial importance for climate forcing calculations or for the comparison of remote sensing with insitu measurements. Here, we will present results from a four-month campaign which took place in summer 2009 in Cabauw, The Netherlands. The aerosol scattering coefficient σ sp (λ) was measured dry and at various, predefined RH conditions between 20 and 95% with a humidified nephelometer. The scattering enhancement factor f (RH,λ) is the key parameter to describe the effect of RH on σ sp (λ) and is defined as σ sp (RH,λ) measured at a certain RH divided by the dry σ sp (dry,λ). The measurement of f (RH,λ) together with the dry absorption measurement (assumed not to change with RH) allows the determination of the actual extinction coefficient σ ep (RH,λ) at ambient RH. In addition, a wide range of other aerosol properties were measured in parallel. The measurements were used to characterize the effects of RH on the Correspondence to: E. Weingartner (ernest.weingartner@psi.ch) aerosol optical properties. A closure study showed the consistency of the aerosol in-situ measurements. Due to the large variability of air mass origin (and thus aerosol composition) a simple parameterization of f (RH,λ) could not be established. If f (RH,λ) needs to be predicted, the chemical composition and size distribution need to be known. Measurements of four MAX-DOAS (multi-axis differential optical absorption spectroscopy) instruments were used to retrieve vertical profiles of σ ep (λ). The values of the lowest layer were compared to the in-situ values after conversion of the latter ones to ambient RH. The comparison showed a good correlation of R 2 = 0.62-0.78, but the extinction coefficients from MAX-DOAS were a factor of 1.5-3.4 larger than the insitu values. Best agreement is achieved for a few cases characterized by low aerosol optical depths and low planetary boundary layer heights. Differences were shown to be dependent on the applied MAX-DOAS retrieval algorithm. The comparison of the in-situ extinction data to a Raman LIDAR (light detection and ranging) showed a good correlation and higher values measured by the LIDAR (R 2 = 0.82 − 0.85, slope of 1.69-1.76) if the Raman retrieved profile was used to extrapolate the directly measured extinction coefficient to the ground. The comparison improved if only nighttime measurements were used in the comparison (R 2 = 0.96, slope of

28Knowledge of the scattering enhancement factor, f(RH), is important for an accurate 29 description of direct aerosol radiative forcing. This factor is defined as the ratio between the 30 scattering coefficient at enhanced relative humidity, RH, to a reference (dry) scattering