Abstract
In the present study, time-resolved aerosol particle formation from sulfuric acid vapor is examined with special attention to the stabilization of molecular clusters in the early phase of unary nucleation. An important factor governing this process is the amount of condensable acid vapor. Here it is produced from fast gas-phase reactions in a batch-type reaction cell for which we introduce modifications enabling real-time monitoring. The key component for size- and time-resolved detection of ultrafine particles is a new 1 nm-SMPS. With this new tool at hand, the effect of varying the precursor concentration over two orders of magnitude is investigated. We demonstrate the ability to tune between different growth scenarios as indicated by the size-resolved particle traces which exhibit a transition from sigmoidal over quasi-stationary to peak-like shape. The second key parameter relevant for nucleation studies is the temperature-dependent cluster evaporation. Due to a temperature rise during the mixing stage of the experiment, evaporation is strongly promoted in the early phase. Therefore, the present study extends the T-range used in, e.g., smog chambers. We investigate this temperature effect in a kinetic simulation and can successfully combine simulated and measured data for validating theoretical evaporation rates obtained from DLPNO-CCSD(T-0)-calculations.
| Original language | English |
|---|---|
| Journal | Physical Chemistry Chemical Physics |
| Volume | 24 |
| Issue | 8 |
| Pages (from-to) | 5001-5013 |
| Number of pages | 13 |
| ISSN | 1463-9076 |
| DOIs | |
| Publication status | Published - Feb 2022 |
Keywords
- AMMONIA
- CLUSTER FORMATION
- GROWTH
- HYDRATION
- METHANESULFONIC-ACID
- NUCLEATION
- OZONE
- RATES
- THERMODYNAMICS
- TROPOSPHERE