The composition of atmospheric aerosols varies with time,
season,
location, and environment. This affects key aerosol properties such
as hygroscopicity and reactivity, influencing the aerosol’s
impact on the climate and air quality. The organic fraction of atmospheric
aerosol emissions often contains surfactant material, such as fatty
acids. These molecules are known to form three-dimensional nanostructures
in contact with water. Different nanostructures have marked differences
in viscosity and diffusivity that are properties whose understanding
is essential when considering an aerosol’s atmospheric impact.
We have explored a range of nanostructures accessible to the organic
surfactant oleic acid (commonly found in cooking emissions), simulating
variation that is likely to happen in the atmosphere. This was achieved
by changing the amount of water, aqueous phase salinity and by addition
of other commonly coemitted compounds: sugars and stearic acid (the
saturated analogue of oleic acid). The nanostructure was observed
by both synchrotron and laboratory small/wide angle X-ray scattering
(SAXS/WAXS) and found to be sensitive to the proxy composition. Additionally,
the spacing between repeat units in these nanostructures was water
content dependent (i.e., an increase from 41 to 54 Å in inverse
hexagonal phase d-spacing when increasing the water
content from 30 to 50 wt %), suggesting incorporation of water within
the nanostructure. A significant decrease in mixture viscosity was
also observed with increasing water content from ∼104 to ∼102 Pa s when increasing the water content
from 30 to 60 wt %. Time-resolved SAXS experiments on levitated droplets
of this proxy confirm the phase changes observed in bulk phase mixtures
and demonstrate that coexistent nanostructures can form in droplets.
Aerosol compositional and subsequent nanostructural changes could
affect aerosol processes, leading to an impact on the climate and
urban air pollution.