Subsecond measurement on deliquescence kinetics of aerosol particles: Observation of partial dissolution and calculation of dissolution rates

The deliquescence behavior of atmospheric aerosols has significant effects on global climate and atmospheric heterogeneous chemistry but remains largely unclear. The deliquescence kinetics data of micron-sized particles are scarce owing to the difficulty on performing the time-resolved dissolution measurements. In view of this technique bottleneck, an applicable and powerful experimental technique, i. e., vacuum FTIR combining pulsed relative humidity (RH) change technique, is introduced for gaining deliquescence kinetics information of three inorganic salts. For NaCl and (NH₄)₂SO₄ aerosols, a solid-liquid mixing state derived from partial dissolution of NaCl and (NH₄)₂SO₄ crystals is present during deliquescence, and the recrystallization will occur once RH decreases. While for NaNO₃ particles, the recrystallization cannot occur as RH decreases owing to the formed amorphous NaNO₃ solids after dying. The dissolution rates of NaCl, (NH₄)₂SO₄ and NaNO₃ solid particles are calculated, as a first attempt, by the upward pulsed RH mode. The measured rates show a significant dependency on ambient RH with three orders of magnitude. For NaCl particles, the measured J values range from 1.41 × 10⁻⁴ to 7.67 × 10⁻¹ s⁻¹ at RH of 73.41–75.15%. The J for (NH₄)₂SO₄ particles is 7.34 × 10⁻³ to 2.46 × 10⁰ s⁻¹ over the RH range of 77.27%–80.13%. The J values for amorphous NaNO₃ solids range from 6.01 × 10⁻³ to 2.63 × 10⁰ s⁻¹ as RH increases from 71.15% to 73.84%. Our results fill in the dataset of atmospheric models describing the kinetics features of deliquescence and provide an insight into dynamic solid-solution transition for PM2.5 particles.