Current State of Atmospheric Aerosol Thermodynamics and Mass Transfer Modeling: A Review
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Notice bibliographique
Résumé
A useful aerosol model must be able to adequately resolve the chemical complexity and phase state of the wide particle size range arising from the many different secondary aerosol growth processes to assess their environmental and health impacts. Over the past two decades, significant advances in understanding of gas-aerosol partitioning have occurred, particularly with respect to the role of organic compounds, yet aerosol representations have changed little in air quality and climate models since the late 1990s and early 2000s. The gas-aerosol partitioning models which are still commonly used in air quality models are separate inorganics-only thermodynamics and secondary organic aerosol (SOA) formation based on absorptive partitioning theory with an assumption of well-mixed liquid-like particles that continuously maintain equilibrium with the gas phase. These widely used approaches in air quality models for secondary aerosol composition and growth based on separated inorganic and organic processes are inadequate. This review summarizes some of the important developments during the past two decades in understanding of gas aerosol mass transfer processes. Substantial increases in computer performance in the last decade justify increasing the process detail in aerosol models. Organics play a central role during post-nucleation growth into the accumulation mode and change the hygroscopic properties of sulfate aerosol. At present, combined inorganic-organic aerosol thermodynamics models are too computationally expensive to be used online in 3-D simulations without high levels of aggregation of organics into a small number of functional surrogates. However, there has been progress in simplified modeling of liquid-liquid phase separation (LLPS) and distinct chemical regimes within organic-rich and inorganic-rich phases. Additional limitations of commonly used thermodynamics models are related to lack of surface tension data for various aerosol compositions in the small size limit, and lack of a comprehensive representation of surface interaction terms such as disjoining pressure in the Gibbs free energy which become significant in the small size limit and which affect both chemical composition and particle growth. As a result, there are significant errors in modeling of hygroscopic growth and phase transitions for particles in the nucleation and Aitken modes. There is also increasing evidence of reduced bulk diffusivity in viscous organic particles and, therefore, traditional secondary organic aerosol models, which are typically based on the assumption of instantaneous equilibrium gas-particle partitioning and neglect the kinetic effects, are no longer tenable.
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Prédiction distillée sur la base complète
Imitation des enseignantsNi prévalence calibrée, ni vérité terrain. Validation humaine à venir. Apprise à partir de 10 348 étiquettes directes de Codex et de 10 348 étiquettes directes de Gemma. Le mode candidate est l'union des têtes enseignantes seuillées; le consensus est leur intersection. Ces sorties portent le statut machine_predicted_unvalidated et ne sont ni des étiquettes humaines ni des étiquettes directes de modèles de pointe.
Scores Codex et Gemma par catégorie
| Catégorie | Codex | Gemma |
|---|---|---|
| Métarecherche | 0,000 | 0,000 |
| Méta-épidémiologie (sens strict) | 0,001 | 0,001 |
| Méta-épidémiologie (sens large) | 0,003 | 0,001 |
| Bibliométrie | 0,000 | 0,001 |
| Études des sciences et des technologies | 0,000 | 0,000 |
| Communication savante | 0,000 | 0,000 |
| Science ouverte | 0,001 | 0,000 |
| Intégrité de la recherche | 0,000 | 0,001 |
| Charge utile insuffisante (le modèle a refusé de juger) | 0,001 | 0,000 |
Scores machine (provisoires)
Les deux têtes enseignantes du modèle étudiant, lues sur ce travail. Un score ordonne la base pour la relecture; il n'affirme jamais une catégorie, et le statut de validation accompagne chaque rangée tel quel.
Scores de référence d'un modèle non mature (critères de maturité non atteints, 7 itérations). Un score ordonne; il n'affirme jamais une catégorie.
score_only:v0-immature-baseline · tel quel depuis la passe de notation : score_only signifie que le nombre peut ordonner les travaux, et qu'aucune étiquette de catégorie n'en découle