Not all types of secondary organic aerosol mix: two phases observed when mixing different secondary organic aerosol types
Bibliographic record
Abstract
Atmospheric aerosol particles play an important role for air quality and climate. Secondary organic aerosol (SOA) make up a significant mass fraction of these particles. SOA particles mostly forms from oxidation of gases, followed by gas-particle conversion of the oxidation products. Due to the variety of precursors and oxidation pathways involved in SOA formation, atmospheric SOA rank among the least understood aerosol types. To assess the impacts of SOA particles on air pollution and climate, knowledge of the number of phases in internal mixtures of different SOA types is critical. For example, gas-particle partitioning of organic species, and thus ultimately ambient SOA mass concentration, strongly depend on the number of phases in SOA particles. Atmospheric models traditionally assumed that different SOA types form a single condensed organic phase when internally mixed in individual particles. In case of mixed SOA particles with a single condensed phase uptake of semi-volatile vapors are enhanced, due to a lowering of the activities in the organic aerosol phase, and hence a lowering of the equilibrium partial pressure. By contrast, the equilibrium partial pressure is greater if the different SOA types form separate phases due to repulsive intermolecular forces between immiscible organic molecules. Consequently, enhancement of vapor uptake and ambient SOA mass concentrations will be smaller or absent in the case of phase-separated SOA particles.Here, using fluorescence microscopy, we directly observed the number of phase in individual particles containing mixtures of different SOA types. A total of 6 different SOA types were generated in environmental chambers from oxidation of single precursors. This included both biogenic and anthropogenic SOA types, having elemental oxygen-to-carbon (O/C) ratios between 0.34 and 1.05, covering values characteristic for aged and fresh atmospheric SOA. The number of phases of all possible internal mixtures of two different SOA types, termed SOA+SOA particles, was investigated as a function of humidity between 90% and 0% relative humidity (RH). We found that the number of phases was independent of RH within the range investigated and that 6 out of 15 SOA+SOA mixtures resulted in particles with two condensed organic phases. The observation of phase separated SOA+SOA particles challenges the approach of assuming a single condensed organic phase when representing SOA formation in atmospheric models. Specifically, we demonstrate that the difference in the average O/C ratio between the two SOA types of a mixture (ΔO/C) is a good predictor of the number of phases in particles that are internal mixtures of different SOA types: two-phase SOA+SOA particles formed for ΔO/C ≥ 0.47, while one-phase SOA+SOA particles formed for ΔO/C < 0.47. This threshold ΔO/C provides a simple, yet powerful parameter to predict whether mixtures of fresh and aged SOA particles form one- or two-phase particles in models.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.001 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.001 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".