Statistico-probabilistic approach to taking account of the vapor depletion in the kinetics of homogeneous nucleation: A free-molecular regime of droplet growth

2004 ◽  
Vol 120 (4) ◽  
pp. 1846-1854 ◽  
Author(s):  
A. P. Grinin ◽  
F. M. Kuni ◽  
Y. S. Djikaev
2012 ◽  
Vol 12 (21) ◽  
pp. 10239-10255 ◽  
Author(s):  
L. T. Padró ◽  
R. H. Moore ◽  
X. Zhang ◽  
N. Rastogi ◽  
R. J. Weber ◽  
...  

Abstract. Aerosol composition and mixing state near anthropogenic sources can be highly variable and can challenge predictions of cloud condensation nuclei (CCN). The impacts of chemical composition on CCN activation kinetics is also an important, but largely unknown, aspect of cloud droplet formation. Towards this, we present in-situ size-resolved CCN measurements carried out during the 2008 summertime August Mini Intensive Gas and Aerosol Study (AMIGAS) campaign in Atlanta, GA. Aerosol chemical composition was measured by two particle-into-liquid samplers measuring water-soluble inorganic ions and total water-soluble organic carbon. Size-resolved CCN data were collected using the Scanning Mobility CCN Analysis (SMCA) method and were used to obtain characteristic aerosol hygroscopicity distributions, whose breadth reflects the aerosol compositional variability and mixing state. Knowledge of aerosol mixing state is important for accurate predictions of CCN concentrations and that the influence of an externally-mixed, CCN-active aerosol fraction varies with size from 31% for particle diameters less than 40 nm to 93% for accumulation mode aerosol during the day. Assuming size-dependent aerosol mixing state and size-invariant chemical composition decreases the average CCN concentration overprediction (for all but one mixing state and chemical composition scenario considered) from over 190–240% to less than 20%. CCN activity is parameterized using a single hygroscopicity parameter, κ, which averages to 0.16 ± 0.07 for 80 nm particles and exhibits considerable variability (from 0.03 to 0.48) throughout the study period. Particles in the 60–100 nm range exhibited similar hygroscopicity, with a κ range for 60 nm between 0.06–0.076 (mean of 0.18 ± 0.09). Smaller particles (40 nm) had on average greater κ, with a range of 0.20–0.92 (mean of 0.3 ± 0.12). Analysis of the droplet activation kinetics of the aerosol sampled suggests that most of the CCN activate as rapidly as calibration aerosol, suggesting that aerosol composition exhibits a minor (if any) impact on CCN activation kinetics.


The model considered in part I is generalized to include growth mechanisms in which the chemical reaction which proceeds at the particle-atm osphere interface is reversible, so that molecules may evaporate from a particle as well as condense upon it. The Becker-Döring-Zeldovich-Frenkel theory of homogeneous nucleation kinetics is then reviewed in the light of the known statistical problem of the birth -and -death process, and an improved approximation is introduced which significantly alters the calculated results. Both steady-state nucleation kinetics and the time lag problem are discussed.


1956 ◽  
Vol 34 (5) ◽  
pp. 473-490 ◽  
Author(s):  
K. A. Jackson ◽  
Bruce Chalmers

The kinetic theory of melting and freezing is developed from consideration of atom movements at an interface between solid and liquid. The equations developed are shown to have the same form as the corresponding thermodynamic equations. The homogeneous nucleation of a solid phase in a liquid is then considered from the point of view of this theory. Agreement with experimental observation is obtained on the following points. (1) The supercooling at which homogeneous nucleation occurs is proportional to the absolute equilibrium temperature. (2) The surface free energy per atom used in the quasi-thermodynamic treatment of nucleation should be equal to one-half the latent heat per atom. (3) The amount of liquid supercooled has a very small effect on the temperature at which homogeneous nucleation occurs.


2008 ◽  
Vol 35 (7) ◽  
pp. n/a-n/a ◽  
Author(s):  
R. H. Moore ◽  
E. D. Ingall ◽  
A. Sorooshian ◽  
A. Nenes

2016 ◽  
Vol 18 (5) ◽  
pp. 4102-4111 ◽  
Author(s):  
Melisa M. Gianetti ◽  
Amir Haji-Akbari ◽  
M. Paula Longinotti ◽  
Pablo G. Debenedetti

Critical nuclei for bulk homogeneous nucleation at ζ = 0.845 for different values of λ.


2012 ◽  
Vol 45 (9) ◽  
pp. 3816-3828 ◽  
Author(s):  
Andreas Wurm ◽  
Evgeny Zhuravlev ◽  
Kathrin Eckstein ◽  
Dieter Jehnichen ◽  
Doris Pospiech ◽  
...  

2020 ◽  
Author(s):  
Marta Tena-Solsona ◽  
Jacqueline Janssen ◽  
Caren Wanzke ◽  
Fabian Schnitter ◽  
Hansol Park ◽  
...  

Active droplets are made of phase-separated molecules that are activated and deactivated by a metabolic reaction cycle. Such droplets play a crucial role in biology as a class of membrane-less organelles. Moreover, theoretical studies show that active droplets can evolve to the same size or spontaneously self-divide when energy is abundant. All of these exciting properties, i.e., emergence, decay, collective behavior, and self-division, are pivotal to the functioning of life. However, these theoretical predictions lack experimental systems to test them quantitively. Here, we describe the synthesis of synthetic active droplets driven by a metabolic chemical cycle and we find a surprising new behavior, i.e., the dynamics of droplet-growth is regulated by the kinetics of the fuel-driven reaction cycle. Consequently, these droplets ripen orders of magnitude faster compared to Ostwald ripening. Combining experiments and theory, we elucidate the underlying mechanism, which could help better understand how cells regulate the growth of membrane-less organelles.<br>


1977 ◽  
Vol 62 (1) ◽  
pp. 303-307 ◽  
Author(s):  
G.J. Shiflet ◽  
K.C. Russell ◽  
H.I. Aaronson

2009 ◽  
Vol 9 (3) ◽  
pp. 795-812 ◽  
Author(s):  
A. Asa-Awuku ◽  
G. J. Engelhart ◽  
B. H. Lee ◽  
S. N. Pandis ◽  
A. Nenes

Abstract. This study investigates the droplet formation characteristics of secondary organic aerosol (SOA) formed during the ozonolysis of sesquiterpene β-caryophyllene (with and without hydroxyl radicals present). Emphasis is placed on understanding the role of semi-volatile material on Cloud Condensation Nucleus (CCN) activity and droplet growth kinetics. Aging of β-caryophyllene SOA significantly affects all CCN-relevant properties measured throughout the experiments. Using a thermodenuder and two CCN instruments, we find that CCN activity is a strong function of temperature (activation diameter at ~0.6% supersaturation: 100±10 nm at 20°C and 130±10 nm at 35°C), suggesting that the hygroscopic fraction of the SOA is volatile. The water-soluble organic carbon (WSOC) is extracted from the SOA and characterized with Köhler Theory Analysis (KTA); the results suggest that the WSOC is composed of low molecular weight (<200 g mol−1) slightly surface-active material that constitute 5–15% of the SOA mass. These properties are similar to the water-soluble fraction of monoterpene SOA, suggesting that predictive understanding of SOA CCN activity requires knowledge of the WSOC fraction but not its exact speciation. Droplet growth kinetics of the CCN are found to be strongly anticorrelated with WSOC fraction, suggesting that the insoluble material in the SOA forms a kinetic barrier that delays droplet growth. Overall, volatilization effects can increase activation diameters by 30%, and depress droplet growth rate by a factor of two; these results may have important implications for the droplet formation characteristics of SOA, and the atmospheric relevance of CCN measurements carried out at temperatures different from ambient.


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