Potential pre-industrial-like new particle formation induced by pure biogenic organic vapors in Finnish peatland.

Pure biogenic new particle formation (NPF) induced by highly oxygenated organic molecules (HOMs) could be an important mechanism for pre-industrial aerosol formation. However, it has not been unambiguously confirmed in the ambient due to the scarcity of truly pristine continental locations in the present-day atmosphere or the lack of chemical characterization of NPF precursors. Here, we report ambient observations of pure biogenic HOM-driven NPF over a peatland in southern Finland. Meteorological decoupling processes formed an "air pocket" (i.e., a very shallow surface layer) at night and favored NPF initiated entirely by biogenic HOM from this peatland, whose atmospheric environment closely resembles that of the pre-industrial era. Our study sheds light on pre-industrial aerosol formation, which represents the baseline for estimating the impact of present and future aerosol on climate, as well as on future NPF, the features of which may revert toward pre-industrial-like conditions due to air pollution mitigation.

Constraining global transport of perfluoroalkyl acids on sea spray aerosol using field measurements.

Perfluoroalkyl acids (PFAAs) are highly persistent anthropogenic pollutants that have been detected in the global oceans. Our previous laboratory studies demonstrated that PFAAs in seawater are remobilized to the air in sea spray aerosols (SSAs). Here, we conducted field experiments along a north-south transect of the Atlantic Ocean to study the enrichment of PFAAs in SSA. We show that in some cases PFAAs were enriched >100,000 times in the SSA relative to seawater concentrations. On the basis of the results of the field experiments, we estimate that the secondary emission of certain PFAAs from the global oceans via SSA emission is comparable to or greater than estimates for the other known global sources of PFAAs to the atmosphere from manufacturing emissions and precursor degradation.

Process-evaluation of forest aerosol-cloud-climate feedback shows clear evidence from observations and large uncertainty in models.

Natural aerosol feedbacks are expected to become more important in the future, as anthropogenic aerosol emissions decrease due to air quality policy. One such feedback is initiated by the increase in biogenic volatile organic compound (BVOC) emissions with higher temperatures, leading to higher secondary organic aerosol (SOA) production and a cooling of the surface via impacts on cloud radiative properties. Motivated by the considerable spread in feedback strength in Earth System Models (ESMs), we here use two long-term observational datasets from boreal and tropical forests, together with satellite data, for a process-based evaluation of the BVOC-aerosol-cloud feedback in four ESMs. The model evaluation shows that the weakest modelled feedback estimates can likely be excluded, but highlights compensating errors making it difficult to draw conclusions of the strongest estimates. Overall, the method of evaluating along process chains shows promise in pin-pointing sources of uncertainty and constraining modelled aerosol feedbacks.