Extended Data Fig. 2: Enhancement of H2SO4–HNO3 nucleation by ammonia.
From: Synergistic HNO3–H2SO4–NH3 upper tropospheric particle formation
a, Particle number concentrations versus time at mobility diameters >1.7 nm (magenta) and >2.5 nm (green). The solid magenta trace is measured by a PSM1.7 and the solid green trace is measured by a CPC2.5. The fixed experimental conditions are 223 K and 25% relative humidity. b, Particle formation rate versus time at 1.7 nm (J1.7), measured by a PSM. c, Particle size distribution versus time, measured by an SMPS. d, Gas-phase nitric acid and sulfuric acid versus time, measured by an I− CIMS and a NO3− CIMS, respectively; gas-phase ammonia versus time, calculated with a first-order wall-loss rate. Before the experiment, we cleaned the chamber by rinsing the walls with ultra-pure water, followed by heating to 373 K and flushing at a high rate with humidified synthetic air for 48 h. We started with an almost perfectly clean chamber and only HNO3, SO2 and O3 vapours present at constant levels. Sulfuric acid starts to appear by means of SO2 oxidation soon after switching on the UV lights at time = 0 min, building up to a steady state of 5.0 × 106 cm−3 with the wall-loss timescale of about 10 min. Subsequently, we observe slow formation of 1.7-nm particles, yet they do not reach 2.5 nm during the course of a 2-h period with small growth rates and low survival probability. Then, owing to the injection of ammonia from 0 to around 6.5 × 108 cm−3 into the chamber after 80 min, a sharp increase in the rate of particle formation is observed with a fixed production rate of sulfuric acid and injection rate of nitric acid. The sulfuric acid concentration decreases slightly afterwards, owing to accumulated condensation sink from fast particle growth. The overall systematic scale uncertainties of ±30% on particle formation rate, −33%/50% on sulfuric acid concentration and ±25% on nitric acid concentration are not shown.
