Global aerosol formation and revised radiative forcing based on CERN CLOUD data

Abstract:

New particle formation in the atmosphere accounts for 40-70% of global cloud condensation nuclei (CCN). It is a complex process involving many precursors: sulphuric acid, ions, ammonia, and a wide range of natural and anthropogenic organic molecules. The CLOUD laboratory chamber experiment at CERN allows the contributions of different compounds to be disentangled in a uniquely well-controlled environment. To date, CLOUD has measured over 500 formation rates (Riccobono 2014, Kirkby 2015, Dunne 2015), under conditions representative of the planetary boundary layer and free troposphere.

To understand the sensitivity of the climate to anthropogenic atmospheric aerosols, we must quantify historical aerosol radiative forcing. This requires an understanding of pre-industrial aerosol sources. Here we show pre-industrial nucleation over land usually involves organic molecules in the very first steps of cluster formation. The complexity of the organic vapors is a major challenge for theoretical approaches. Furthermore, with fewer sulphuric acid and ammonia molecules available to stabilize nucleating clusters in the pre-industrial atmosphere, ions from radon or galactic cosmic rays were probably more important than they are today.

Parameterizations of particle formation rates determined in CLOUD as a function of precursor concentrations, temperature and ions are being used to refine the GLOMAP aerosol model (Spracklen 2005). The model simulates the growth, transport and loss of particles, translating nucleation rates to CCN concentrations. This allows us to better understand the effects of pre-industrial and present-day particle formation. I will present new results on global CCN based on CLOUD data, including estimates of anthropogenic aerosol radiative forcing, currently the most uncertain driver of climate change (IPCC 2013).

References: Riccobono, F. et al, Science 344 717 (2014); Kirkby, J. et al, in review; Dunne, E. et al, in preparation; Spracklen, D. et al, Atmos. Chem. Phys. 5 2227 (2005); IPCC AR5 (2013).

The figure shows annual mean mixing ratios of sulphuric acid (A) and condensable secondary organic vapours `SecOrg' formed from biogenic monoterpenes (B) from a GLOMAP simulation for 2008. Most new particles are formed below 2km altitude.