Nucleation Scheme Research Articles

New particle formation induced by anthropogenic–biogenic interactions on the southeastern Tibetan Plateau

Abstract. New particle formation (NPF) plays a crucial role in the atmospheric aerosol population and has significant implications on climate dynamics, particularly in climate-sensitive zones such as the Tibetan Plateau (TP). However, our understanding of NPF on the TP is still limited due to a lack of comprehensive measurements and verified model simulations. To fill this knowledge gap, we conducted an integrated study combining comprehensive field measurements and chemical transport modeling to investigate NPF events on the southeastern TP during the pre-monsoon season. NPF was observed to occur frequently on clear-sky days on the southeastern TP, contributing significantly to the cloud condensation nuclei (CCN) budget in this region. The observational evidence suggests that highly oxygenated organic molecules (HOMs) from monoterpene oxidation participate in the nucleation on the southeastern TP. After updating the monoterpene oxidation chemistry and nucleation schemes in the meteorology–chemistry model, the model well reproduces observed NPF and reveals an extensive occurrence of NPF across the southeastern TP. The dominant nucleation mechanism is the synergistic nucleation of sulfuric acid, ammonia, and HOMs, driven by the transport of anthropogenic precursors from South Asia and the presence of abundant biogenic gases. By investigating the vertical distribution of NPF, we find a significant influence of vertical transport on the southeastern TP. More specifically, strong nucleation near the surface leads to an intense formation of small particles, which are subsequently transported upward. These particles experience enhanced growth to larger sizes in the upper planetary boundary layer (PBL) due to favorable conditions such as lower temperatures and a reduced condensation sink. As the PBL evolves, the particles in larger sizes are brought back to the ground, resulting in a pronounced increase in near-surface particle concentrations. This study highlights the important roles of anthropogenic–biogenic interactions and meteorological dynamics in NPF on the southeastern TP.

Radiative and Microphysical Impacts of the Saharan Dust on Two Concurrent Tropical Cyclones: Danielle and Earl (2010)

AbstractSaharan dust exerts profound impacts on the genesis and intensification of tropical cyclones (TCs). Such impacts on various stages of the TCs have yet to be explored. In this study, we utilize the Cloud‐Resolving weather research and forecasting model (WRF) to investigate the relative importance of the microphysical and radiative effects of dust on two hurricanes (Earl and Danielle) at different life stages under similar dynamical conditions in 2010. Both TCs were embedded in a dusty environment throughout their lifetime. A new dust ice nucleation scheme was implemented into the aerosol‐aware Texas A&M University two‐moment microphysical scheme in WRF. Moreover, the dust radiative effect was included in the Goddard Shortwave Scheme of WRF. Our sensitivity experiments show that the radiative effect of dust (DRAD) amplified the mid‐level ridge in the Central Atlantic Ocean through temperature perturbation, changing the tracks of Danielle and Earl. Further analyses reveal an early shift of Danielle's maximum intensity for 12 hours but a significantly suppressed Earl in DRAD. In addition, the microphysical effect of dust had little impact on the large‐scale dynamical fields and storm tracks. The inclusion of dust as ice nucleation particles results in more variations in the intensity of Danielle and Earl than in other scenarios. This is owing to the higher maximum diabatic heating rate in the rainband region that perturbs the size of the TC. This study shows the dominant dust radiative effects on both intensity and track of the storm. In addition, there is evidence that dust suppresses the early stage TC but provides favorable conditions for matured TC. Both findings have profound implications for hurricane forecast and address the importance of accounting for detailed cloud microphysics and aerosol‐TC interactions in the operational forecasting models.

Cloud Characteristics and Their Effects on Solar Irradiance According to the ICON Model, CLOUDNET and BSRN Observations

We investigated the liquid water path and global solar irradiance (Q) at ground level according to the ICON model; CLOUDNET measurements in Lindenberg, Munich, and Jülich; and BSRN observations in Lindenberg. This research is focused on stratiform non-precipitating clouds. The liquid water path (LWP) is underestimated, while Q is overestimated. The lower LWP is due to liquid water content underestimation practically in all atmosphere layers and a lower frequency of liquid cloud occurrence compared to observations. This is partly associated with the structure of the cloud nucleation scheme of the ICON model and with the default cloud condensation nuclei (CCN) number concentration. An increase in CCNs from 250 cm−3 (typical background value for the region of interest) to 1700 cm−3 (characteristic of polluted continental clouds) leads to an increase in the grid-scale liquid water path by 40% and a decrease in Q by 12% in overcast conditions. However, we also showed that the liquid water path is not a key factor of Q overestimation. The main factor is an inaccurate description of the cloud spatial structure, where the correct prediction of the ratio of direct to global irradiance as a spatial characteristic of clouds plays a more important role than the standard cloud fraction.

Nonclassical Nucleation and Crystallization of LiNbO3 Nanoparticles from the Aqueous Solvothermal Alkoxide Route.

The exact molecular reaction pathway and crystallization mechanisms of LiNbO3 nanoparticles under solvothermal conditions are derived through extensive time- and temperature-resolved experiments allowing to track all the transient molecular and solid species. Starting with a simple mixing of Li/Nb ethoxides, water addition is used to promote condensation after ligand exchange with different co-solvents including alcohols and glycols of variable carbon-chain length. A nonclassical nucleation scheme is first demonstrated after the identification of new octanuclear complexes with a {Li4Nb4O10} core whose solvophobic interactions mediate their aggregation, thus, resulting in a colloidal gel at room-temperature. Upon heating, a more or less frustrated aggregation-mediated crystallization process is then evidenced leading to LiNbO3 nanocrystals of adjustable mean size between 20 and 100nm. Such a fine control can be attributed to the variable Nb-OR (R = alkoxy/glycoxy ligand) binding interactions at the surface of crystalline intermediates. Demonstration of such a nonclassical nucleation process and crystallization mechanism for LiNbO3 not only sheds light on the entire growth process of multifunctional nanomaterials with non-perovskite crystalline structures, but also opens new avenues for the identification of novel bimetallic oxoclusters involved in the formation of several mixed oxides from the aqueous alkoxide route.

Description and performance of a sectional aerosol microphysical model in the Community Earth System Model (CESM2)

Abstract. We implemented the Community Aerosol and Radiation Model for Atmospheres (CARMA) in both the high- and low-top model versions of the Community Earth System Model Version 2 (CESM2). CARMA is a sectional microphysical model, which we use for aerosol in both the troposphere and stratosphere. CARMA is fully coupled to chemistry, clouds, radiation, and transport routines in CESM2. This development enables the comparison of simulations with a sectional (CARMA) and a modal (MAM4) aerosol microphysical model in the same modeling framework. The new implementation of CARMA has been adopted from previous work, with some additions that align with the current CESM2 Modal Aerosol Model (MAM4) implementation. The main updates include an interactive secondary organic aerosol description in CARMA, using the volatility basis set (VBS) approach, updated wet removal, and the use of transient emissions of aerosols and trace gases. In addition, we implemented an alternative aerosol nucleation scheme in CARMA, which is also used in MAM4. Detailed comparisons of stratospheric aerosol properties after the Mount Pinatubo eruption reveal the importance of prescribing sulfur injections in a larger region rather than in a single column to better represent the observed evolution of aerosols. Both CARMA and MAM4 in CESM2 are able to represent stratospheric and tropospheric aerosol properties reasonably well when compared to observations. Several differences in the performance of the two aerosol models show, in general, an improved representation of aerosols when using the sectional aerosol model in CESM2. These include a better representation of the aerosol size distribution after the Mount Pinatubo volcanic eruption in CARMA compared to MAM4. MAM4 produces on average smaller aerosols and less removal than CARMA, which results in a larger total mass. Both CARMA and MAM4 reproduce the stratospheric aerosol optical depth (AOD) within the error bar of the observations between 2001 and 2020, except for recent larger volcanic eruptions that are overestimated by both model configurations. The CARMA background surface area density and aerosol size distribution in the stratosphere and troposphere compare well to observations, with some underestimation of the Aitken-mode size range. MAM4 shows shortcomings in reproducing coarse-mode aerosol distributions in the stratosphere and troposphere. This work outlines additional development needs for CESM2 CARMA to improve the model compared to observations in both the troposphere and stratosphere.

Growth of Dichalcogenide Layers on TiO2(110)—MoSe2 or TiSe2

Transition‐metal dichalcogenide (TMDC) islands and thin films are grown on TiO2(110) via physical vapor deposition of Mo and Se and are analyzed with electron diffraction, Auger spectroscopy, and scanning tunneling microscopy (STM). Surprisingly, large, crystalline TiSe2 patches develop on the TiO2 surface instead of the expected MoSe2 islands. They are identified by a hexagonal lattice with 3.4 Å periodicity, a unique (2 × 2) superstructure related to charge‐density waves, and an empty conductance doublet in STM spectroscopy. Density‐function‐theory calculations assign the imaging contrast and the conductance doublet to tunneling into the 3p orbitals of the topmost Se layer and Ti 3d‐related electronic states, respectively. Control experiments without Mo deposition confirm that the observed TMDC growth indeed results from a surface reaction between gas‐phase Se and Ti3+ atoms, segregating out of the reduced TiO2 crystal. From the unique shape and orientation of the TiSe2 islands in the low‐coverage regime, a distinct nucleation scheme is proposed, in which the Se(3 × 1) superstructure on TiO2 provides pinning centers for the TMDC. This article aims at increasing the awareness that Mo and Se co‐deposition does not automatically result in MoSe2 formation, but parasitic processes may trigger the growth of other TMDCs.

Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements

Abstract. New particle formation (NPF) and subsequent particle growth are important sources of condensation nuclei (CN) and cloud condensation nuclei (CCN). While many observations have shown positive contributions of NPF to CCN at low supersaturation, negative NPF contributions were often simulated in polluted environments. Using the observations in a coastal city of Qingdao, Beijing, and Gucheng in north China, we thoroughly evaluate the simulated number concentrations of CN and CCN using an NPF-explicit parameterization embedded in the WRF-Chem model. For CN, the initial simulation shows large biases of particle number concentrations at 10–40 and 40–100 nm. By adjusting the process of gas–particle partitioning, including the mass accommodation coefficient (MAC) of sulfuric acid, the phase changes in primary organic aerosol emissions, and the condensational amount of nitric acid, the improvement of the particle growth process yields substantially reduced overestimation of CN. Regarding CCN, secondary organic aerosol (SOA) formed from the oxidation of semi-volatile and intermediate-volatility organic compounds (S/IVOCs) is called SI-SOA, the yield of which is an important contributor. At default settings, the SI-SOA yield is too high without considering the differences in precursor oxidation rates. Lowering the SI-SOA yield under linear H2SO4 nucleation scheme results in much-improved CCN simulations compared to observations. On the basis of the bias-corrected model, we find substantially positive contributions of NPF to CCN at low supersaturation (∼ 0.2 %) over broad areas of China, primarily due to competing effects of increasing particle hygroscopicity, a result of reductions in SI-SOA amount, surpassing that of particle size decreases. The bias-corrected model is robustly applicable to other schemes, such as the quadratic H2SO4 nucleation scheme, in terms of CN and CCN, though the dependence of CCN on SI-SOA yield is diminished likely due to changes in particle composition. This study highlights potentially much larger NPF contributions to CCN on a regional and even global basis.

Analysis of new particle formation events and comparisons to simulations of particle number concentrations based on GEOS-Chem–advanced particle microphysics in Beijing, China

Abstract. Aerosol particles play important roles in air quality and global climate change. In this study, we analyze the measurements of particle size distribution from 12 March to 6 April 2016 in Beijing to characterize new particle formation (NPF) using the observational data of sulfuric acid, meteorological parameters, solar radiation, and the mass concentration of fine particles (PM2.5, particulate matter with diameters less than 2.5 µm). During this 26 d campaign, 11 new particle formation events are identified with obvious bursts of sub-3 nm particle number concentrations and subsequent growth of these nucleated particles. It is found that sulfuric acid concentration in Beijing does not have a significant difference between NPF event and non-event days. Low relative humidity (RH) and high daily total solar radiation appear to be favorable for the occurrence of NPF events, which is quite obvious in this campaign. The simulations using four nucleation schemes, i.e., H2SO4–H2O binary homogeneous nucleation (BHN), H2SO4–H2O–NH3 ternary homogeneous nucleation (THN), H2SO4–H2O–ion binary ion-mediated nucleation (BIMN), and H2SO4–H2O–NH3–ion ternary ion-mediated nucleation (TIMN), based on a global chemistry transport model (GEOS-Chem) coupled with an advanced particle microphysics (APM) model, are conducted to study the particle number concentrations and new particle formation process. Our comparisons between measurements and simulations indicate that the BHN scheme and BIMN scheme significantly underestimate the observed particle number concentrations, and the THN scheme captures the total particle number concentration on most NPF event days well but fails to capture the noticeable increase in particle number concentrations on 18 March and 1 April. The TIMN scheme has obvious improvement in terms of total and sub-3 nm particle number concentrations and nucleation rates. This study provides a basis for further understanding of the nucleation mechanism in Beijing.

Impact of formulations of the homogeneous nucleation rate on ice nucleation events in cirrus

Abstract. Homogeneous freezing of solution droplets is an important pathway of ice formation in the tropopause region. The nucleation rate can be parameterized as a function of water activity, based on empirical fits and some assumptions on the underlying properties of super-cooled water, although a general theory is missing. It is not clear how nucleation events are influenced by the exact formulation of the nucleation rate or even their inherent uncertainty. In this study we investigate the formulation of the nucleation rate of homogeneous freezing of solution droplets (1) to link the formulation to the nucleation rate of pure water droplets, (2) to derive a robust and simple formulation of the nucleation rate, and (3) to determine the impact of variations in the formulation on nucleation events. The nucleation rate can be adjusted, and the formulation can be simplified to a threshold description. We use a state-of-the-art bulk ice microphysics model to investigate nucleation events as driven by constant cooling rates; the key variables are the final ice crystal number concentration and the maximum supersaturation during the event. The nucleation events are sensitive to the slope of the nucleation rate but only weakly affected by changes in its absolute value. This leads to the conclusion that details of the nucleation rate are less important for simulating ice nucleation in bulk models as long as the main feature of the nucleation rate (i.e. its slope) is represented sufficiently well. The weak sensitivity of the absolute values to the nucleation rate suggests that the amount of available solution droplets also does not crucially affect nucleation events. The use of only one distinct nucleation threshold function for analysis and model parameterization should be reinvestigated, since it corresponds to a very high nucleation rate value, which is not reached in many nucleation events with low vertical updrafts. In contrast, the maximum supersaturation and thus the nucleation thresholds reached during an ice nucleation event depend on the vertical updraft velocity or cooling rate. This feature might explain some high supersaturation values during nucleation events in cloud chambers and suggests a reformulation of ice nucleation schemes used in coarse models based on a purely temperature-dependent nucleation threshold.

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.

Performance of Two‐Moment Stratiform Microphysics With Prognostic Precipitation in GFDL's CM4.0

AbstractWe describe the model performance of a new global coupled climate model configuration, CM4‐MG2. Beginning with the Geophysical Fluid Dynamics Laboratory's fourth‐generation physical climate model (CM4.0), we incorporate a two‐moment Morrison‐Gettelman bulk stratiform microphysics scheme with prognostic precipitation (MG2), and a mineral dust and temperature‐dependent cloud ice nucleation scheme. We then conduct and analyze a set of fully coupled atmosphere‐ocean‐land‐sea ice simulations, following Coupled Model Intercomparison Project Phase 6 protocols. CM4‐MG2 generally captures CM4.0's baseline simulation characteristics, but with several improvements, including better marine stratocumulus clouds off the west coasts of Africa and North and South America, a reduced bias toward “double” Intertropical Convergence Zones south of the equator, and a stronger Madden‐Julian Oscillation (MJO). Some degraded features are also identified, including excessive Arctic sea ice extent and a stronger‐than‐observed El Nio‐Southern Oscillation. Compared to CM4.0, the climate sensitivity is reduced by about 10% in CM4‐MG2.

A “parallel universe” scheme for crack nucleation in the phase field approach to fracture

Crack nucleation is crucial in many industrial applications. The phase field method for fracture transforms the crack nucleation problem into a minimization problem of the sum of the elastic potential energy and the crack surface energy. Due to the polyconvexity of the formulation, starting from a crackless solid, a standard Newton iteration may lead to a solution with no crack, even though a cracked solution has a lower total energy. As such, the critical load for cracking is highly overestimated. Here, we propose an algorithm termed “parallel universe” algorithm to capture the global minimum. This algorithm has two key ingredients: (a) a necessary condition for cracking solely based on the current crackless solution, and (b) beginning from when this condition is met, Newton iteration with two initial guesses, a crackles one and a cracked one, will both be performed and the converged candidate solution with lower energy is accepted as the solution at that load step. Once the cracked candidate solution is accepted, the crackless one is discarded, i.e., only one universe is retained. This cracked initial guess is obtained only once for all load steps by solving a series of similar minimization problems with a progressively reduced critical crack energy release rate. Numerical examples with isotropic and anisotropic critical crack energy release rates indicate that the proposed algorithm is more reliable (as there is no need to retrace) and more efficient than the standard Newton iteration and a well-known backtracking algorithm.

Vigorous New Particle Formation Above Polluted Boundary Layer in the North China Plain

AbstractAtmospheric new particle formation (NPF) is vital in climate and air pollution for its contribution to aerosols and cloud condensation nuclei; however, a vertical understanding of NPF is still limited. Here, simultaneous observations at two altitudes were conducted over the North China Plain. Despite a high aerosol loading during cold season, NPF is still frequently observed. The upper‐air NPF is increasingly intensive and starts earlier as haze pollution deteriorated, and the onset time gap could exceed 3 hr. To understand the factors modulating NPF vertically, we updated the meteorology‐chemistry model by incorporating state‐of‐the‐art nucleation schemes and performed highly vertical‐resolved simulations. It is revealed that vertical disparities in NPF are attributed to the pronounced stratification of sulfur dioxide, ozone, and particulate matter. As the evolution of the boundary layer, strong NPF in the upper air elevates the near‐surface nucleation‐mode particles. This work sheds more light on the vertical structure of NPF.

Hot-Wall MOCVD for High-Quality Homoepitaxy of GaN: Understanding Nucleation and Design of Growth Strategies

Thick GaN layers with a low concentration of defects are the key to enable next-generation vertical power electronic devices. Here, we explore hot-wall metalorganic chemical vapor deposition (MOCVD) for the development of GaN homoepitaxy. We propose a new approach to grow high-quality homoepitaxial GaN in N2-rich carrier gas and at a higher supersaturation as compared to heteroepitaxy. We develop a low-temperature GaN as an optimum nucleation scheme based on the evolution and thermal stability of the GaN surface under different gas compositions and temperatures. Analysis in the framework of nucleation theory of homoepitaxial layers simultaneously grown on GaN templates on SiC and on hydride vapor phase epitaxy GaN substrates is presented. We show that residual strain and screw dislocation densities affect GaN nucleation and subsequent growth leading to distinctively different morphologies of GaN homoepitaxial layers grown on GaN templates and native substrates, respectively. The established comprehensive picture provides a guidance for designing strategies for growth conditions optimization in GaN homoepitaxy. GaN with atomically flat and smooth epilayer surfaces with a root-mean-square roughness value as low as 0.049 nm and low background carbon concentration of 5.3 × 1015 cm–3 has been achieved. It is also shown that there is no generation of additional dislocations during homoepitaxial growth. Thus, our results demonstrate the potential of the hot-wall MOCVD technique to deliver high-quality GaN material for vertical power devices.

Cloud Droplet Nucleation Simulation and Parameterization

Abstract Cloud droplet nucleation is classically defined as a droplet growing to a size such that its ambient supersaturation exceeds its surface equilibrium water vapor pressure. Unactivated particles are always in equilibrium with the ambient vapor pressure. Further studies showed that such an equilibrium assumption leads to many more cloud droplets being nucleated due to neglecting kinetic growth limitations, including the inertial mechanism, evaporation mechanism, and deactivation mechanism. Moreover, the inertial mechanism results in great discrepancy between the actual size and the critical size of nucleation for large aerosol particles. These issues complicate cloud droplet nucleation parameterization for applications in cloud modeling. To establish a physically based nucleation scheme, we established a highly size-resolved Lagrangian parcel model. Vapor diffusion and heat conduction were calculated according to Maxwell theory, and the surface vapor density and temperature were explicitly simulated. The surface temperature variation of a droplet with its size was considered. The surface supersaturation of a droplet, taking into account the surface temperature variation, is different from its equilibrium supersaturation at its large sizes. The nucleation simulation showed that the inertial and deactivation mechanisms can impact droplet nucleation. Moreover, very large nuclei can trigger rain embryo formation in a short time period. Even though there are kinetic limitations, the classical equilibrium assumption can be applied to determine the primary nucleation number of cloud droplets. Meanwhile, a regression formula for the size of a nucleated droplet and its dry aerosol size was established.

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.

Assessment of meta-atom scheme for nucleation of dislocation loops in TWIP steel

We use atomistic calculations to explore the process of homogeneous nucleation of dislocation loops in TWIP steel with the nudged-elastic-band method and meta-atom interatomic potential. Energy barriers to the nucleation process have been estimated at different applied shear stresses, and an atomistically informed nucleation model is fitted to the results for both Shockley and twinning dislocation loops. Besides exhibiting excellent agreement with the direct atomistic results, the nucleation model also provides the critical size of the dislocation loop. Comparison of the critical loop diameters with the intrinsic spatial scale of the meta-atom potential reveals that the loop nucleation is sensitive to the local compositional heterogeneity. As a result, the simulation results obtained with a meta-atom potential are shown to require careful interpretation in terms of their statistical ramifications.

Primary and secondary ice production: interactions and their relative importance

Abstract. A discrepancy of up to 5 orders of magnitude between ice crystal and ice nucleating particle (INP) number concentrations was found in the measurements, indicating the potentially important role of secondary ice production (SIP) in the clouds. However, the interactions between primary and SIP processes and their relative importance remain unexplored. In this study, we implemented five different ice nucleation schemes as well as physical representations of SIP processes (i.e., droplet shattering during rain freezing, ice-ice collisional break-up, and rime splintering) in the Community Earth System Model version 2 (CESM2). We ran CESM2 in the single column mode for model comparisons with the DOE Atmospheric Radiation Measurement (ARM) Mixed-Phase Arctic Cloud Experiment (M-PACE) observations. We found that the model experiments with aerosol-aware ice nucleation schemes and SIP processes yield the best simulation results for the M-PACE single-layer mixed-phase clouds. We further investigated the relative importance of ice nucleation and SIP to ice number and cloud phase as well as interactions between ice nucleation and SIP in the M-PACE single-layer mixed-phase clouds. Our results show that SIP contributes 80 % to the total ice formation and transforms ∼30 % of pure liquid-phase clouds simulated in the model experiments without considering SIP into mixed-phase clouds. The SIP is not only a result of ice crystals produced from ice nucleation, but also competes with the ice nucleation by reducing the number concentrations of cloud droplets and cloud-borne dust INPs. Conversely, strong ice nucleation also suppresses SIP by glaciating mixed-phase clouds and thereby reducing the amount of precipitation particles (rain and graupel).

Nanostructure of PMMA/MAM Blends Prepared by Out-of-Equilibrium (Extrusion) and Near-Equilibrium (Casting) Self-Assembly and Their Nanocellular or Microcellular Structure Obtained from CO2 Foaming.

Blends of poly(methyl methacrylate) (PMMA) and a triblock copolymer poly(methyl methacrylate)-b-poly(butyl acrylate)-b-poly(methyl methacrylate) (MAM) have been obtained following both out-of-equilibrium (extrusion) and near-equilibrium (solvent casting) production routes. The self-assembly capability and the achievable nanostructures of these blends are analyzed by transmission electron microscopy (TEM) regarding their production route and potential for the achievement of nanocellular foams by CO2 gas dissolution foaming. The influence of the initial nanostructure of the solids on the obtained cellular structure of bulk and film samples is determined by high-resolution scanning electron microscopy (HRSEM) for diverse foaming conditions (saturation pressure, saturation temperature, and post-foaming stage), taking into account the required use of a foaming mold to achieve foams from films. Moreover, the influence of the nanostructuration on the presence of solid outer layers, typical of the selected foaming process, is addressed. Finally, consideration of a qualitative model and the obtained results in terms of nanostructuration, cellular structure, and foaming behavior, allow proposing a detailed cell nucleation, growth, and stabilization scheme for these materials, providing the first direct evidence of the cell nucleation happening inside the poly(butyl acrylate) phase in the PMMA/MAM blends.

Ice microphysical processes exert a strong control on the simulated radiative energy budget in the tropics

Simulations of the global climate system at storm-resolving resolutions of 2 km are now becoming feasible and show promising realism in clouds and precipitation. However, shortcomings in their representation of microscale processes, like the interaction of cloud droplets and ice crystals with radiation, can still restrict their utility. Here, we illustrate how changes to the ice microphysics scheme dramatically alter both the vertical profile of cloud-radiative heating and top-of-atmosphere outgoing longwave radiation (terrestrial infrared cooling) in storm-resolving simulations over the Asian monsoon region. Poorly-constrained parameters in the ice nucleation scheme, overactive conversion of ice to snow, and inconsistent treatment of ice crystal effective radius between microphysics and radiation alter cloud-radiative heating by a factor of four and domain-mean infrared cooling by 30 W m−2. Vertical resolution, on the other hand, has a very limited impact. Even in state-of-the-art models then, uncertainties in microscale cloud properties exert a strong control on the radiative budget that propagates to both atmospheric circulation and regional climate. These uncertainties need to be reduced to realize the full potential of storm-resolving models.