Aerosols and clouds contribute to atmospheric variability and Earth’s radiative balance across local, regional, and global scales. Originating from both natural and anthropogenic sources, aerosols can cause adverse health effects and can interact directly with solar radiation as well as indirectly through complex interactions with clouds. Aerosol optical depth (AOD) has been observed from satellite platforms for over 30 years. During this time, regional changes in emissions, arising from air quality policies and socioeconomic factors, have been suggested as causes for some observed AOD trends. In the United States, the Clean Air Act and amendments have produced improvements in air quality. In this work the impacts of improved air quality on the aerosol loading and aerosol direct and indirect effects over the North Atlantic Ocean are explored using satellite, ground, and model datasets on the monthly timescale during 2002 to 2012.

It is established that two trends exist in the total AOD observed by MODIS over the North Atlantic.  A decreasing AOD trend between −0.02 and −0.04 per decade is observed over the mid-latitude region.  Using the GOCART aerosol model it is shown that this trend results from decreases in anthropogenic species.  Ground based aerosol networks (AERONET and IMPROVE) support a decreasing trend in AOD and further strengthen links to anthropogenic aerosol species, particularly sulfate species.  This anthropogenic decrease occurs primarily during spring and summer.  During the same time period, MODIS also observes an increasing AOD trend of 0.02 per decade located in the sub-tropical region.  This trend is shown to occur during summer and is the result of natural dust aerosol.  Changes in the North African environment seen in the MERRA reanalysis suggest an accelerated warming over the Saharan Desert leads to changes in the African Easterly Jet, related Easterly Waves, and baroclinicity playing a role in an increase and northward shift in African dust.

Both the direct and indirect impacts of the aerosol trends are investigated.  Using the SBDART radiative transfer model, estimates of the shortwave direct radiative forcing are calculated.  The decrease in anthropogenic AOD produces an increase of 2.0 ± 0.3 W/m2 per decade in the Earth-system absorbance over the mid-latitude site (37.5ºN, −68.5ºE).  The increase in natural AOD results in a decrease of −1.1 ± 0.2 W/m2 per decade in the Earth-system absorbance over the sub-tropical site (23.5ºN, −55.5ºE).  Evaluation of the first indirect effect demonstrates agreement with Twomey theory when considering the North Atlantic domain on the whole.  A regional analysis reveals the existence of counter-Twomey behavior along the U.S. Atlantic coast.  Using a daily dataset during summertime with focus on warm, non-precipitating clouds, it is found that aerosol-cloud interaction in this coastal region is sensitive to vertical velocity and aerosol size.  Cases experiencing updrafts (ω < 0 Pa/s) and cases of mainly coarse-mode aerosol demonstrate good agreement with Twomey theory.  Additionally, cases with low specific humidity near the cloud base show non-Twomey behavior for clouds with low liquid water path.