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Sulfuric acid is an important gas influencing atmospheric new particleformation (NPF). Both the binary (H2SO4–H2O) system and theternary system involving ammonia (H2SO4–H2O–NH3) may beimportant in the free troposphere. An essential step in the nucleation ofaerosol particles from gas-phase precursors is the formation of a dimer, soan understanding of the thermodynamics of dimer formation over a wide rangeof atmospheric conditions is essential to describe NPF. We have used theCLOUD chamber to conduct nucleation experiments for these systems attemperatures from 208 to 248 K. Neutral monomer and dimer concentrations ofsulfuric acid were measured using a chemical ionization mass spectrometer(CIMS). From these measurements, dimer evaporation rates in the binary systemwere derived for temperatures of 208 and 223 K. We compare these results toliterature data from a previous study that was conducted at highertemperatures but is in good agreement with the present study. For theternary system the formation of H2SO4·NH3 is verylikely an essential step in the formation of sulfuric acid dimers, whichwere measured at 210, 223, and 248 K. We estimate the thermodynamicproperties (dH and dS) of the H2SO4·NH3 clusterusing a simple heuristic model and the measured data. Furthermore, we reportthe first measurements of large neutral sulfuric acid clusters containing asmany as 10 sulfuric acid molecules for the binary system using chemicalionization–atmospheric pressure interface time-of-flight (CI-APi-TOF) massspectrometry

atmospheric chemistry and physics

Thermodynamics of the formation of sulfuric acid dimers in the binary (H&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;SO&amp;lt;sub&amp;gt;4&amp;lt;/sub&amp;gt;–H&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;O) and ternary (H&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;SO&amp;lt;sub&amp;gt;4&amp;lt;/sub&amp;gt;–H&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;O–NH&amp;lt;sub&amp;gt;3&amp;lt;/sub&amp;gt;) system