SearcharxivSearch

arXiv · 2109.12737

Enthalpy effect on the kinetics of concurrent nucleation and chemical aging of aqueous organic aerosols. The stage of thermal relaxation

Abstract

The size and composition distribution of an ensemble of aqueous organic droplets, evolving via nucleation and concomitant chemical aging, may be affected by the latent heat of condensation and enthalpy of heterogeneous chemical reactions, so the temperature of the droplet may deviate from the air temperature and thus become an independent variable of its state (additional to its size and composition variables). Using the formalism of the classical nucleation theory, we derive a partial differential equation for the temporal evolution of the distribution of an ensemble of such droplets with respect to all their variables of state via Taylor series expansions of the corresponding multidimensional discrete equation of balance, describing the material and heat exchange between droplets and air. The resulting kinetic equation goes beyond the framework of the Fokker-Planck approximation with respect to the temperature variable. A hierarchy of time scales of nonisothermal nucleation and concomitant chemical aging of aqueous organic aerosols is established and an analytical description of their thermal relaxation stage is developed, allowing one to estimate the characteristic time of the establishment of the equilibrium distribution of aerosol particles with respect to their temperatures. Theoretical results are illustrated with numerical calculations for the concurrent nucleation and chemical aging of model aqueous hydrophilic-hydrophobic organic aerosols in air.

Explore related subjects

Keep this discovery

BibTeXRIS

Yuri S. Djikaev, Batradz I. Djikkaity. 2021-09-27. Enthalpy effect on the kinetics of concurrent nucleation and chemical aging of aqueous organic aerosols. The stage of thermal relaxation. https://arxiv.org/abs/2109.12737

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related papers

Windowed Envelope Statistics for Time-Domain Significant Wave Height Estimation From HF Radar

Significant wave height (SWH) retrieval from high-frequency (HF) radar typically relies on a weak second-order Doppler continuum that is sensitive to noise, interference, and spectral leakage. This letter presents a Windowed Envelope Statistics Estimator (WESE) that operates directly on beam-formed time-domain voltages. A second-order term obtained from a Neumann expansion of the rough-surface field equation motivates quadratic compensation of localized radar features. WESE extracts the mean, standard deviation, or variance from overlapping windows of the in-phase, quadrature, or envelope-magnitude sequence, followed by quadratic compensation, rank ordering, least-squares regression, and causal smoothing. Evaluation used 335 synchronized hourly observations from a 13.385 MHz, 12-element WERA system at Argentia, Newfoundland and Labrador. The optimal configuration used quadrature variance, a 16-sample window, 896 retained chronological samples, and 30-h smoothing, achieving an RMSE of 0.152 m and a Pearson correlation of 0.978. This represents RMSE reductions of 32.1% and 18.7% relative to previously reported linear and second-order compensated ordered-statistics models, respectively. The results demonstrate robust time-domain SWH estimation without explicit Doppler-spectrum construction.

physics.ao-ph

KiloDA: Reconstructing kilometer-scale near-surface wind states from sparse station observations

Accurate kilometer-scale near-surface winds are important for understanding atmospheric processes over complex terrain, yet remain difficult to reconstruct from sparse and unevenly distributed observations. Here we introduce KiloDA, a diffusion framework for hourly kilometer-scale wind reconstruction from surface stations. KiloDA learns the statistical distribution and spatial structure of wind fields from historical 3-km Weather Research and Forecasting (WRF) model forecasts. At each reconstruction time, no contemporaneous WRF field is used. Instead, station observations provide the only constraints on the current atmospheric state and guide posterior sampling from the learned prior. In idealized WRF experiments, KiloDA recovers localized wind structures when only 0.24% of grid cells are observed and shows an overall advantage over conventional interpolation across terrain conditions and wind speed regimes. This capability largely transfers to real observations. In a fully withheld region, KiloDA reduces the median wind speed root mean square error (RMSE) by 19% relative to ERA5 reanalysis, using only observations outside the region, with the largest improvements over high-elevation and high-relief terrain. A random station holdout further confirms that this advantage extends across different complex-terrain locations and holdout configurations. These results show that historical model archives can provide useful structural knowledge for reconstructing kilometer-scale wind fields from sparse observations without requiring an accurate model estimate of the current atmospheric state.

physics.ao-ph