Decreasing particle number concentrations in a warming atmosphere and implications
1Atmospheric Sciences Research Center, State University of New York at Albany, USA
2Department of Atmospheric and Oceanic Sciences, University of California at Los Angeles, USA
3Global Monitoring Division (GMD), Earth System Research Laboratory (ESRL), NOAA, USA
4School of Engineering and Applied Sciences, Harvard University, USA
Abstract. New particle formation contributes significantly to the number concentration of condensation nuclei (CN) as well as cloud CN (CCN), a key factor determining aerosol indirect radiative forcing of the climate system. Using a physics-based nucleation mechanism that is consistent with a range of field observations of aerosol formation, it is shown that projected increases in global temperatures could significantly inhibit new particle, and CCN, formation rates worldwide. An analysis of CN concentrations observed at four NOAA ESRL/GMD baseline stations since the 1970s and two other sites since 1990s reveals long-term decreasing trends consistent with these predictions. The analysis also suggests, owing to larger observed CN reductions at remote sites than can be explained by the basic nucleation mechanism, that dimethylsulphide (DMS) emissions may be decreasing worldwide with increasing global temperatures, implying a positive DMS-based cloud feedback forcing of the climate ("CLAW"). The combined effects of rising temperatures on aerosol nucleation rates, and possibly on DMS emissions, may imply substantial decreases in future tropospheric particle abundances associated with global warming, delineating a potentially significant feedback mechanism that increases Earth's climate sensitivity to greenhouse gas emissions. Further research is needed to quantify the magnitude of such a feedback process.