Abstract. Atmospheric aerosol particle concentrations are strongly affected by various
wet processes, including below and in-cloud wet scavenging and in-cloud
aqueous-phase oxidation. We studied how wet scavenging and cloud processes
affect particle concentrations and composition during transport to a rural
boreal forest site in northern Europe. For this investigation, we employed
air mass history analysis and observational data. Long-term particle number
size distribution (∼15 years) and composition measurements
(∼8 years) were combined with air mass trajectories with
relevant variables from reanalysis data. Some such variables were rainfall
rate, relative humidity, and mixing layer height. Additional observational
datasets, such as temperature and trace gases, helped further evaluate wet
processes along trajectories with mixed effects models. All chemical species investigated (sulfate, black carbon, and organics)
exponentially decreased in particle mass concentration as a function of
accumulated precipitation along the air mass route. In sulfate (SO4)
aerosols, clear seasonal differences in wet removal emerged, whereas
organics (Org) and equivalent black carbon (eBC) exhibited only minor differences. The
removal efficiency varied slightly among the different reanalysis datasets
(ERA-Interim and Global Data Assimilation System; GDAS) used for the trajectory calculations due to the
difference in the average occurrence of precipitation events along the
air mass trajectories between the reanalysis datasets. Aqueous-phase processes were investigated by using a proxy for air masses
travelling inside clouds. We compared air masses with no experience of
approximated in-cloud conditions or precipitation during the past 24 h
to air masses recently inside non-precipitating clouds before they entered
SMEAR II (Station for Measuring Ecosystem–Atmosphere Relations). Significant increases in SO4 mass concentration were observed
for the latter air masses (recently experienced non-precipitating clouds). Our mixed effects model considered other contributing factors affecting
particle mass concentrations in SMEAR II: examples were trace gases, local
meteorology, and diurnal variation. This model also indicated in-cloud
SO4 production. Despite the reanalysis dataset used in the trajectory
calculations, aqueous-phase SO4 formation was observed. Particle
number size distribution measurements revealed that most of the in-cloud
SO4 formed can be attributed to particle sizes larger than 200 nm
(electrical mobility diameter). Aqueous-phase secondary organic aerosol
(aqSOA) formation was non-significant.