Binary Nucleation Research Articles

How CO2 gas accelerates water nucleation at low temperature.

We conducted homogeneous nucleation experiments for dilute binary H2O-CO2 mixtures in Ar-N2 carrier gas with different CO2/H2O ratios at temperatures of 57 and 75K and total pressures of ∼40 and 70Pa, respectively. Direct experimental information on the number and type of molecules in the clusters and on the cluster number concentration is obtained by mass spectrometric detection of nucleating clusters that form in the uniform region of Laval expansions. Only homo-molecular water clusters are observed in the mass spectra. However, as the CO2/H2O ratio increases, a significant increase in the nucleation rate is observed. A simple kinetic model suggests that this acceleration of nucleation is due to the formation of short-lived, transient hetero-molecular H2O-CO2 dimers. Comparison with homogeneous binary nucleation of toluene-CO2 and unary nucleation of H2O shows that nucleation becomes more efficient in systems with stronger intermolecular interactions and a larger number of degrees of freedom. Such studies at the molecular level will improve our understanding of homogeneous nucleation mechanisms in atmospheric and industrial processes.

Application of binary homogeneous nucleation theory to the generation of liquid aerosols from water vapor with a highly dilute reactant

Application of binary homogeneous nucleation theory to the generation of liquid aerosols from water vapor with a highly dilute reactant

Development of the Reiss theory for binary homogeneous nucleation of aerosols

Development of the Reiss theory for binary homogeneous nucleation of aerosols

On the Influence of Atmospheric Ions on Aerosol Formation: Numerical Modeling

A new mathematical model of the global transport of multicomponent gas impurities and aerosols has been constructed, including the formation of sulfate aerosols in the atmosphere in both hemispheres. Calculations of the nucleation rates and particle number concentrations were performed for the winter period in the troposphere using a unified model that takes into account chemical and kinetic transformation processes (photochemistry, nucleation, condensation/evaporation, and coagulation). Binary nucleation of sulfuric acid and water vapor was coupled with new-particle formation due to atmospheric ions. The numerical results indicate a significant role of ion nucleation in aerosol formation in the Northern and Southern hemispheres in winter. The factors controlling the dynamics of ionic processes in the atmosphere and their influence on the spatiotemporal distribution of aerosol particles involve not only the level of air ionization but also temperature, relative humidity, and the content of sulfur and water vapor in the air. At a height of 4.2 km, the formation of particle nuclei with the participation of ions occurs only over the Lake Baikal and Kamchatka regions as well as the regions of the northeast and northwest of the American continent. Within the regions of localization of this process in the atmosphere, the rate of new particle generation varies by more than an order of magnitude.

Significant contributions of trimethylamine to sulfuric acid nucleation in polluted environments

As one of the least understood aerosol processes, nucleation can be a dominant source of atmospheric aerosols. Sulfuric acid (SA)-amine binary nucleation with dimethylamine (DMA) has been recognized as a governing mechanism in the polluted continental boundary layer. Here we demonstrate the importance of trimethylamine (TMA) for nucleation in the complex atmosphere and propose a molecular-level SA-DMA-TMA ternary nucleation mechanism as an improvement upon the conventional binary mechanism. Using the proposed mechanism, we could connect the gaseous amines to the SA-amine cluster signals measured in the atmosphere of urban Beijing. Results show that TMA can accelerate the SA-DMA-based new particle formation in Beijing by 50–100%. Considering the global abundance of TMA and DMA, our findings imply comparable importance of TMA and DMA to nucleation in the polluted continental boundary layer, with probably higher contributions from TMA in polluted rural environments and future urban environments with controlled DMA emissions.

Mutual independence of water and n-nonane nucleation at low temperatures.

The interaction of water with different substances in the earth's atmosphere lies at the heart of many processes that influence our climate. However, it is still unclear how different species interact with water on the molecular level and in which ways this interaction contributes to the water vapor phase transition. Here, we report the first measurements of water-nonane binary nucleation in the 50-110K temperature range, along with unary nucleation data of both. The time-dependent cluster size distribution in a uniform post-nozzle flow was measured by time-of-flight mass spectrometry coupled with single-photon ionization. From these data, we extract experimental rates and rate constants for both nucleation and cluster growth. The observed mass spectra of water/nonane clusters are not or only slightly affected by the introduction of the other vapor, and the formation of mixed clusters was not observed during nucleation of the mixed vapor. Additionally, the nucleation rate of either substance is not much affected by the presence (or absence) of the other species, i.e., the nucleation of water and nonane proceeds independently, indicating that hetero-molecular clusters do not play a role during nucleation. Only at the lowest temperature of our experiment (i.e., 51K) do the measurements suggest that interspecies interaction slows water cluster growth. The findings here are in contrast to our earlier work in which we showed that vapor components in other mixtures, e.g., CO2 and toluene/H2O, can interact to promote nucleation and cluster growth in a similar temperature range.

Particle number concentrations and size distributions in the stratosphere: implications of nucleation mechanisms and particle microphysics

Abstract. While formation and growth of particles in the troposphere have been extensively studied in the past two decades, very limited efforts have been devoted to understanding these in the stratosphere. Here we use both Cosmics Leaving OUtdoor Droplets (CLOUD) laboratory measurements taken under very low temperatures (205–223 K) and Atmospheric Tomography Mission (ATom) in situ observations of particle number size distributions (PNSDs) down to 3 nm to constrain nucleation mechanisms and to evaluate model-simulated particle size distributions in the lowermost stratosphere (LMS). We show that the binary homogenous nucleation (BHN) scheme used in most of the existing stratospheric aerosol injection (a proposed method of solar radiation modification) modeling studies overpredicts the nucleation rates by 3–4 orders of magnitude (when compared to CLOUD data) and particle number concentrations in the background LMS by a factor ∼ 2–4 (when compared to ATom data). Based on a recently developed kinetic nucleation model, which gives rates of both ion-mediated nucleation (IMN) and BHN at low temperatures in good agreement with CLOUD measurements, both BHN and IMN occur in the stratosphere. However, IMN rates are generally more than 1 order of magnitude higher than BHN rates and thus dominate nucleation in the background stratosphere. In the Southern Hemisphere (SH) LMS with minimum influence of anthropogenic emissions, our analysis shows that ATom-measured PNSDs generally have four apparent modes. The model captures reasonably well the two modes (Aitken mode and the first accumulation mode) with the highest number concentrations and size-dependent standard deviations. However, the model misses an apparent second accumulation mode peaking around 300–400 nm, which is in the size range important for aerosol direct radiative forcing. The bimodal structure of accumulation mode particles has also been observed in the stratosphere well above tropopause and in the volcano-perturbed stratosphere. We suggest that this bimodal structure may be caused by the effect of charges on coagulation and growth, which is not yet considered in any existing models and may be important in the stratosphere due to high ionization rates and the long lifetime of aerosols. Considering the importance of accurate PNSDs for projecting a realistic radiation forcing response to stratospheric aerosol injection (SAI), it is essential to understand and incorporate such potentially important processes in SAI model simulations and to carry out further research to find out what other processes the present models might have missed.

Methanesulfonic acid and iodous acid nucleation: a novel mechanism for marine aerosols.

By seeding clouds, new particle formation (NPF) has a substantial impact on radiation balance, bio-geochemical cycles and global climate. Over oceans, both methanesulfonic acid (CH3S(O)2OH, MSA) and iodous acid (HIO2) have been reported to be closely associated with NPF events; however, much less is known about whether they can jointly nucleate to form nanoclusters. Hence, quantum chemical calculations and Atmospheric Cluster Dynamics Code (ACDC) simulations were performed to investigate the novel mechanism of MSA-HIO2 binary nucleation. The results indicate that MSA and HIO2 can form stable clusters via multiple interactions including hydrogen bonds, halogen bonds, and electrostatic forces between ion pairs after proton transfer, which are more diverse than those in MSA-iodic acid (HIO3) and MSA-dimethylamine (DMA) clusters. Interestingly, HIO2 can be protonated by MSA exhibiting base-like behavior, but it differs from base nucleation precursors by self-nucleation rather than solely binding to MSA. Due to the greater stability of MSA-HIO2 clusters, the formation rate of MSA-HIO2 clusters can be even higher than that of MSA-DMA clusters, suggesting that MSA-HIO2 nucleation is a non-negligible source of marine NPF. This work proposes a novel mechanism of MSA-HIO2 binary nucleation for marine aerosols and provides deeper insights into the distinctive nucleation characteristics of HIO2, which can help in constructing a more comprehensive sulfur- and iodine-bearing nucleation model for marine NPF.

The effects of methanol clustering on methanol-water nucleation.

The formation of subcritical methanol clusters in the vapor phase is known to complicate the analysis of nucleation measurements. Here, we investigate how this process affects the onset of binary nucleation as dilute water-methanol mixtures in nitrogen carrier gas expand in a supersonic nozzle. These are the first reported data for water-methanol nucleation in an expansion device. We start by extending an older monomer-dimer-tetramer equilibrium model to include larger clusters, relying on Helmholtz free energy differences derived from Monte Carlo simulations. The model is validated against the pressure/temperature measurements of Laksmono et al. [Phys. Chem. Chem. Phys. 13, 5855 (2011)] for dilute methanol-nitrogen mixtures expanding in a supersonic flow prior to the appearance of liquid droplets. These data are well fit when the maximum cluster size imax is 6-12. The extended equilibrium model is then used to analyze the current data. On the addition of small amounts of water, heat release prior to particle formation is essentially unchanged from that for pure methanol, but liquid formation proceeds at much higher temperatures. Once water comprises more than ∼24 mol% of the condensable vapor, droplet formation begins at temperatures too high for heat release from subcritical cluster formation to perturb the flow. Comparing the experimental results to binary nucleation theory is challenged by the need to extrapolate data to the subcooled region and by the inapplicability of explicit cluster models that require a minimum of 12 molecules in the critical cluster.

Performance Evaluation of a Novel Pilot-Scale Wet Electrostatic Precipitator in a Bio-Drying-Assisted Solid Recovered Fuel (SRF) Generation Plant: Particulate Matter (PM) Collection Efficiency

The production of solid recovered fuel (SRF) from sewage sludge has been credited with facilitating Korea’s waste management shift toward a resource circular economy. In this study, a novel pilot-scale wet electrostatic precipitator (WESP) was developed and installed in a bio-drying-assisted solid recovered fuel (SRF) generation plant for the first time. To investigate the performance of the novel WESP, various sizes of particulate matter, i.e., total particle matter (PM), particle matter smaller than 10 μm (PM10), and particle matter smaller than 0.1 μm (PM0.1), collection efficiencies were evaluated and demonstrated promising performances. Under optimal operating conditions (flow rate of 5 m3/min and an applied voltage of 30 kV), 99.76% PM and 91% PM10 collection efficiencies were achieved, and the PM concentration was 0.16 mg/m3, which met the exhaust emission standard. However, a dramatic increase in PM0.1 was observed and could be explained by the break-up theory, binary homogenous nucleation, and ion-induced nucleation. The experimental findings could serve as useful information to understand the WESP system.

Influence of emission size distribution and nucleation on number concentrations over Greater Paris

Abstract. With the growing evidence that high particle number concentrations may impact health, modelling their emissions and understanding formation processes is necessary, especially in cities where many people are exposed. As emission inventories of particle numbers and size distribution over cities are usually not available, a methodology is defined to estimate them from PM2.5 emissions and ratios of PM1 / PM2.5 and PM0.1 / PM2.5 by activity sector. In this methodology, a fitting parameter αem is used to redistribute the number concentrations in the lowest emission diameter range. This parameter is chosen by comparing measured and simulated number concentrations during non-nucleation days. The emission size distribution is then finely discretised by conserving both mass and number in each of the size ranges where emissions are specified. The methodology is applied over Greater Paris during the MEGAPOLI campaign (July 2009). Three-dimensional simulations are performed using the chemistry transport model Polair3D/Polyphemus coupled to the aerosol module SSH-aerosol to represent the evolution of particles by condensation, evaporation, coagulation, and nucleation, with a sectional approach for the size distribution. The model is first compared to measurements during non-nucleation days, and the influence over the month of July 2009 of three different nucleation parameterisations is assessed, i.e. binary (sulfuric acid, water), ternary (sulfuric acid, ammonia, water), and heteromolecular (extremely low-volatility organic compounds (ELVOCs) from monoterpenes and sulfuric acid). The modelled number concentrations compare very well to measurements, with an average normalised mean error of 42 % for the daily number concentrations of particles larger than 10 nm and 37 % for the number concentrations of particles larger than 100 nm. The influence of the binary nucleation is low, and the ternary nucleation scheme leads to better simulated number concentrations (in terms of bias and error) at only one site out of three, but it systematically reduces the model to measurement correlation, suggesting that ternary nucleation may not be the dominant process in new particle formation. However, the relative bias and error, as well as the correlation at suburban sites, are systematically improved using the heteromolecular nucleation scheme involving sulfuric acid and ELVOCs from monoterpenes. This suggests that heteromolecular nucleation may be important in cities, especially at suburban sites in summer, and that a better characterisation of the emissions of ELVOC precursors from traffic is needed.

Compilation of reaction kinetics parameters determined in the Key Development Project for Air Pollution Formation Mechanism and Control Technologies in China

A compilation of new advances made in the research field of laboratory reaction kinetics in China's Key Development Project for Air Pollution Formation Mechanism and Control Technologies was presented. These advances are grouped into six broad, interrelated categories, including volatile organic compound (VOC) oxidation, secondary organic aerosol (SOA) formation, new particle formation (NPF) and gas-particle partitioning, ozone chemistry, model parameters, and secondary inorganic aerosol (SIA) formation, highlighting the laboratory work done by Chinese researchers. For smog chamber applications, the current knowledge gained from laboratory studies is reviewed, with emphasis on summarizing the oxidation mechanisms of long-chain alkanes, aromatics, alkenes, aldehydes/ketones in the atmosphere, SOA formation from anthropogenic emission sources, and oxidation of aromatics, isoprene, and limonene, as well as SIA formation. For flow tube applications, atmospheric oxidation mechanisms of toluene and methacrolein, SOA formation from limonene oxidation by ozone, gas-particle partitioning of peroxides, and sulfuric acid-water (H2SO4-H2O) binary nucleation, methanesulfonic acid-water (MSA-H2O) binary nucleation, and sulfuric acid-ammonia-water (H2SO4-NH3-H2O) ternary nucleation are discussed.

On the Fokker–Planck approximation in the kinetic equation of multicomponent classical nucleation theory

We examine the validity of the Fokker–Planck equation with linear force coefficients as an approximation to the kinetic equation of nucleation in homogeneous isothermal multicomponent condensation. Starting with a discrete equation of balance governing the temporal evolution of the distribution function of an ensemble of multicomponent droplets and reducing it (by means of Taylor series expansions) to the differential form in the vicinity of the saddle point of the free energy surface, we have identified the parameters whereof the smallness is necessary for the resulting kinetic equation to have the form of the Fokker–Planck equation with linear (in droplet variables) force coefficients. The “non-smallness” of these parameters results either in the appearance of the third or higher order partial derivatives of the distribution function in the kinetic equation or in its force coefficients becoming non-linear functions of droplet variables, or both; this would render the conventional kinetic equation of multicomponent nucleation and its predictions inaccurate. As a numerical illustration, we carried out calculations for isothermal condensation in five binary systems of various non-ideality at T=293.15 K: 1-butanol–1-hexanol, water–methanol, water–ethanol, water–1-propanol, water–1-butanol. Our results suggest that under typical experimental conditions the kinetic equation of binary nucleation of classical nucleation theory may require a two-fold modification and, hence, the conventional expression for the steady-state binary nucleation rate may not be adequate for the consistent comparison of theoretical predictions with experimental data.

Critical cluster composition from homogeneous nucleation data: application to water in carbon dioxide\u2013nitrogen carrier gases

Knowledge on critical cluster composition is important for improving the nucleation theory. Thus, homogeneous water nucleation experiments previously carried out in nitrogen and 0%, 5%, 15% and 25% of carbon dioxide ( Campagna et al. 2020a, 2021) are analyzed. The tests were conducted at 240 K and 0.1 MPa, 1 MPa and 2 MPa. The observed nucleation rates are strongly dependent on supersaturation, pressure, temperature and mixture composition. These experimentally found dependencies can be used to derive the composition of critical clusters by means of the nucleation theorem. In this way, a macroscopic quantity, nucleation rate, reveals properties of critical clusters consisting of a few tens of molecules. Two novel methods are presented for the detailed application of the nucleation theorem. The first method extends to mixtures of ,,,,,,,N>2,,,,,, components the approach used in literature for two components. The second method not only applies to N>2 mixtures in a more straightforward manner, but it can also be used for unary as well as for binary and multi-component nucleation cases. To the best of our knowledge, for the first time the critical cluster composition is computed for high pressure nucleation data of a vapor (here water) in mixtures of two carrier gases (here carbon dioxide–nitrogen). After a proper parameterization of the nucleation rate data, both methods consistently lead to the same critical nuclei compositions within the experimental uncertainty. Increasing pressure and carbon dioxide molar fraction at fixed supersaturation leads to a decrease in the water content of the critical cluster, while the adsorbed number of nitrogen and carbon dioxide molecules increases. As a consequence, the surface tension decreases. This outcome explains the observed increase in the nucleation rate with increasing pressure and carbon dioxide molar fraction at constant supersaturation.Graphic abstract

Simulation of Aerosol Evolution within Background Pollution for Nucleated Vehicle Exhaust via TEMOM

This work is intended to study the effect of background particles on vehicle emissions in representative realistic atmospheric environments. The coupling of Reynolds-Averaged Navier–Stokes equation (RANS) and Taylor-series Expansion Method Of Moments (TEMOM) is performed to track the emissions of the vehicle and simulating the evolution of the matters. The transport equation of mass, momentum, heat, and the first three orders of moments are taken into account with the effect of binary homogeneous nucleation, Brownian coagulation, condensation, and thermophoresis. The parameterization model is utilized for nucleation. The measured data for Beijing’s particle size distribution under both polluted and nonpolluted conditions are utilized as background particles. The relationship between the macroscopic measurement results and the microscopic dynamic process is analyzed by comparing the variation trend of several physical quantities in the process of aerosol evolution. It is found with an increase of background particle concentration, the nucleation is inhibited, which is consistent with the existing studies.

An Artificial Neural Network Reveals the Nucleation Mechanism of a Binary Colloidal AB13 Crystal.

Colloidal suspensions of two species have the ability to form binary crystals under certain conditions. The hunt for these functional materials and the countless investigations on their formation process are justified by the plethora of synergetic and collective properties these binary superlattices show. Among the many crystal structures observed over the past decades, the highly exotic colloidal icosahedral AB13 crystal was predicted to be stable in binary hard-sphere mixtures nearly 30 years ago, yet the kinetic pathway of how homogeneous nucleation occurs in this system is still unknown. Here we investigate binary nucleation of the AB13 crystal from a binary fluid phase of nearly hard spheres. We calculate the nucleation barrier and nucleation rate as a function of supersaturation and draw a comparison with nucleation of single-component and other binary crystals. To follow the nucleation process, we employ a neural network to identify the AB13 phase from the binary fluid phase and the competing fcc crystal with single-particle resolution and significant accuracy in the case of bulk phases. We show that AB13 crystal nucleation proceeds via a coassembly process where large spheres and icosahedral small-sphere clusters simultaneously attach to the nucleus. Our results lend strong support for a classical pathway that is well-described by classical nucleation theory, even though the binary fluid phase is highly structured and exhibits local regions of high bond orientational order.

The Role of Binary and Ion Nucleation of Sulfuric Acid and Water Vapor in the Dynamics of Sulfate Aerosol Formation in the Atmosphere

The results of one-dimensional calculations of the height profiles of nucleated sulfate aerosol particles for the northern mid-latitudes and tropics in winter are presented. Numerical calculations were performed using a three-dimensional model of the transport and transformation of multicomponent gas and aerosol substances in the atmosphere, incorporating photochemistry, nucleation involving neutral molecules and ions, as well as condensation/evaporation and coagulation. It is found that the resulting dynamics of the formation of aerosol particle nuclei is not a simple sum of ion and binary (water vapor/sulfuric acid) nucleation rates. This dynamics is determined by the ratio of critical radii of nucleated particles due to binary and ion nucleation of these substances (rcr_bin and rcr_ion) depending on temperature, relative humidity, and ionization rate. This should be taken into account in modeling the gas and aerosol composition of the atmosphere and comparing calculated and observed data.

The Role of Binary and Ion Nucleation of Sulfuric Acid and Water Vapor in the Dynamics of Sulfate Aerosol Formation in the Atmosphere

The results of one-dimensional calculations of the height profiles of nucleated sulfate aerosol particles for the northern mid-latitudes and tropics in winter are presented. Numerical calculations were performed using a three-dimensional model of the transport and transformation of multicompo- nent gas and aerosol substances in the atmosphere, incorporating photochemistry, nucleation involving neutral molecules and ions, as well as condensation/evaporation and coagulation. It is found that the resulting dynamics of the formation of aerosol particle nuclei is not a simple sum of ion and binary (water vapor/sulfuric acid) nucleation rates. This dynamics is determined by the ratio of critical radii of nucleated particles due to binary and ion nucleation of these substances (rcr_bin and rcr_ion) depending on temperature, relative humidity, and ionization rate. This should be taken into account in modeling the gas and aerosol composition of the atmosphere and comparing calculated and observed data.

The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere

Abstract. Global observations and model studies indicate that new particle formation (NPF) in the upper troposphere (UT) and subsequent particles supply 40 %–60 % of cloud condensation nuclei (CCN) in the lower troposphere, thus affecting the Earth's radiative budget. There are several plausible nucleation mechanisms and precursor species in this atmospheric region, which, in the absence of observational constraints, lead to uncertainties in modeled aerosols. In particular, the type of nucleation mechanism and concentrations of nucleation precursors, in part, determine the spatial distribution of new particles and resulting spatial distribution of CCN from this source. Although substantial advances in understanding NPF have been made in recent years, NPF processes in the UT in pristine marine regions are still poorly understood and are inadequately represented in global models. Here, we evaluate commonly used and state-of-the-art NPF schemes in a Lagrangian box model to assess which schemes and precursor concentrations best reproduce detailed in situ observations. Using measurements of aerosol size distributions (0.003 < Dp < 4.8 µm) in the remote marine troposphere between ∼0.18 and 13 km altitude obtained during the NASA Atmospheric Tomography (ATom) mission, we show that high concentrations of newly formed particles in the tropical UT over both the Atlantic and Pacific oceans are associated with outflow regions of deep convective clouds. We focus analysis on observations over the remote Pacific Ocean, which is a region less perturbed by continental emissions than the Atlantic. Comparing aerosol size distribution measurements over the remote Pacific with box model simulations for 32 cases shows that none of the NPF schemes most commonly used in global models, including binary nucleation of sulfuric acid and water (neutral and ion-assisted) and ternary involving sulfuric acid, water, and ammonia, are consistent with observations, regardless of precursor concentrations. Through sensitivity studies, we find that the nucleation scheme among those tested that is able to explain most consistently (21 of 32 cases) the observed size distributions is that of Riccobono et al. (2014), which involves both organic species and sulfuric acid. The method of Dunne et al. (2016), involving charged sulfuric acid–water–ammonia nucleation, when coupled with organic growth of the nucleated particles, was most consistent with the observations for 5 of 32 cases. Similarly, the neutral sulfuric acid–water–ammonia method of Napari (2002), when scaled with a tuning factor and with organic growth added, was most consistent for 6 of 32 cases. We find that to best reproduce both nucleation and growth rates, the mixing ratios of gas-phase organic precursors generally need to be at least twice that of SO2, a proxy for dimethyl sulfide (DMS). Unfortunately, we have no information on the nature of oxidized organic species that participated in NPF in this region. Global models rarely include organic-driven nucleation and growth pathways in UT conditions where globally significant NPF takes place, which may result in poor estimates of NPF and CCN abundance and contribute to uncertainties in aerosol–cloud–radiation effects. Furthermore, our results indicate that the organic aerosol precursor vapors may be important in the tropical UT above marine regions, a finding that should guide future observational efforts.

Liquid vaporization under thermodynamic phase non-equilibrium condition at the gas-liquid interface

Liquid vaporization under thermodynamic phase non-equilibrium condition at the gas-liquid interface is investigated over a wide range of fluid state typical of many liquid-fueled energy conversion systems. The validity of the phase-equilibrium assumption commonly used in the existing study of liquid vaporization is examined using molecular dynamics theories. The interfacial mass flow rates on both sides of the liquid surface are compared to the net vaporization rate through an order-of-magnitude analysis Results indicated that the phase-equilibrium assumption holds valid at relatively high pressures and low temperatures, and for droplets with relatively large initial diameters (for example, larger than 10 µm for vaporizing oxygen droplets in gaseous hydrogen in the pressure range from 10 atm to the oxygen critical state). Droplet vaporization under superheated conditions is also explored using classical binary homogeneous nucleation theory, in conjunction with a real-fluid equation of state. It is found that the bubble nucleation rate is very sensitive to changes in saturation ratio and pressure; it increases by several orders of magnitude when either the saturation ratio or the pressure is slightly increased. The kinetic limit of saturation ratio decreases with increasing pressure, leading to reduced difference between saturation and superheat conditions. As a result, the influence of non-equilibrium conditions on droplet vaporization is lower at a higher pressure.