Abstract. One of the major uncertainties in the understanding of Earth's climate system is the interaction between solar radiation and aerosols in the atmosphere. Aerosols exposed to high humidity will change their chemical, physical, and optical properties due to their increased water content. To model hydrated aerosols, atmospheric chemistry and climate models often use the volume weighted mixing rule to predict the complex refractive index (RI) of aerosols when they interact with high relative humidity, and, in general, assume homogeneous mixing. This study explores the validity of these assumptions. A humidified cavity ring down aerosol spectrometer (CRD-AS) and a tandem hygroscopic DMA (differential mobility analyzer) are used to measure the extinction coefficient and hygroscopic growth factors of humidified aerosols, respectively. The measurements are performed at 80 % and 90 %RH at wavelengths of 532 nm and 355 nm using size-selected aerosols with different degrees of absorption; from purely scattering to highly absorbing particles. The ratio of the humidified to the dry extinction coefficients (f RH ext (%RH, Dry)) is measured and compared to theoretical calculations based on Mie theory. Using the measured hygroscopic growth factors and assuming homogeneous mixing, the expected RIs using the volume weighted mixing rule are compared to the RIs derived from the extinction measurements.We found a weak linear dependence or no dependence of f RH(%RH, Dry) with size for hydrated absorbing aerosols in contrast to the non-monotonically decreasing behavior with size for purely scattering aerosols. No discernible difference could be made between the two wavelengths used. Less than 7 % differences were found between the real parts of the complex refractive indices derived and those calculated using the volume weighted mixing rule, and the imaginary parts had up to a 20 % difference. However, for substances with growth factor less than 1.15 the volume weighted mixing rule assumption needs to be taken with caution as the imaginary part of the complex RI can be underestimated.

Abstract. Fires including peatland burning in Southeast Asia have become a major concern to the general public as well as governments in the region. This is because aerosols emitted from such fires can cause persistent haze events under certain weather conditions in downwind locations, degrading visibility and causing human health issues. In order to improve our understanding of the spatiotemporal coverage and influence of biomass burning aerosols in Southeast Asia, we have used surface visibility and particulate matter concentration observations, supplemented by decade-long (2003 to 2014) simulations using the Weather Research and Forecasting (WRF) model with a fire aerosol module, driven by high-resolution biomass burning emission inventories. We find that in the past decade, fire aerosols are responsible for nearly all events with very low visibility (< 7 km). Fire aerosols alone are also responsible for a substantial fraction of low-visibility events (visibility  < 10 km) in the major metropolitan areas of Southeast Asia: up to 39 % in Bangkok, 36 % in Kuala Lumpur, and 34 % in Singapore. Biomass burning in mainland Southeast Asia accounts for the largest contribution to total fire-produced PM2.5 in Bangkok (99 %), while biomass burning in Sumatra is a major contributor to fire-produced PM2.5 in Kuala Lumpur (50 %) and Singapore (41 %). To examine the general situation across the region, we have further defined and derived a new integrated metric for 50 cities of the Association of Southeast Asian Nations (ASEAN): the haze exposure day (HED), which measures the annual exposure days of these cities to low visibility (< 10 km) caused by particulate matter pollution. It is shown that HEDs have increased steadily in the past decade across cities with both high and low populations. Fire events alone are found to be responsible for up to about half of the total HEDs. Our results suggest that in order to improve the overall air quality in Southeast Asia, mitigation policies targeting both biomass burning and fossil fuel burning sources need to be implemented.

The hygroscopic growth of aerosols is controlled by the relative humidity (RH) and changes the aerosols' physical and hence optical properties. Observational studies of aerosol-cloud interactions evaluate the aerosol concentration using optical parameters, such as the aerosol optical depth (AOD), which can be affected by aerosol humidification. In this study we evaluate the RH background and variance values, in the lower cloudy atmosphere, an additional source of variance in AOD values beside the natural changes in aerosol concentration. In addition, we estimate the bias in RH and AOD, related to cloud thickness. This provides the much needed range of RH-related biases in studies of aerosol-cloud interaction.Twelve years of radiosonde measurements (June-August) in thirteen globally distributed stations are analyzed. The estimated non-biased AOD variance due to day-to-day changes in RH is found to be around 20% and the biases linked to cloud development around 10%. Such an effect is important and should be considered in direct and indirect aerosol effect estimations but it is inadequate to account for most of the AOD trend found in observational studies of aerosol-cloud interactions.

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