Condensation Nuclei Research Articles

Condensation of organic-inorganic vapours governs the production of ultrafine secondary marine cloud nuclei

Ultrafine secondary marine aerosol (<100 nm), formed via gas-to-particle conversion, can make an important contribution to the number of cloud condensation nuclei in the marine boundary layer. It has long been known that the growth of ultrafine secondary marine aerosol cannot be sustained solely by condensation of the inorganic species that drive the initial nucleation, and condensation of organic vapours has been suggested as the most likely mechanism. However, the evidence from field observations had been lacking. Here we report observational evidence on the importance of the condensation of organic and inorganic vapours onto Aitken mode particles in forming cloud condensation nuclei. Further long-term analysis (over 10 years) with additional hygroscopicity growth measurements reveals that the ultrafine secondary marine aerosol growth events are driven by condensation of biogenic vapours, which leads to up to substantial increases in cloud condensation nuclei number at realistic marine cloud supersaturation.

Applying the multi-level perspective to climate geoengineering: Sociotechnical bottlenecks for negative emissions and cloud seeding technologies

Carbon dioxide removal and negative emissions technologies, such as bioenergy with carbon capture (BECCS) and direct air capture with carbon storage (DACCS), may have an important role to play in reducing greenhouse gas emissions (GHGs). Cloud seeding (CS), a controversial form of weather modification, might also help to reduce the severity and intensity of storms and address widespread drought from climate change. Nevertheless, costs, technical complexity, social acceptance, and other unknown risks have so far kept these climate geoengineering interventions at uncertin levels of research and deployment in the response to climate change. Although a large corpus of literature sufficiently deals with the technical aspects underlying such interventions, the nontechnical and social aspects of geoengineering mark fertile research territory. This study applies the sociotechnical concept of the Multi-Level Perspective (MLP)—commonly used for analysis of sustainability transitions—to explore the risks, costs, uncertainties, and complexities of rolling out BECCS in the United Kingdom, DACCS in the United States, and cloud seeding in Australia. We examine the interaction of the MLP across three levels (niche, regime, and landscape), then explore windows of opportunity and technological transition bottlenecks. Specifically, we show that BECCS align with the “stretch-and-transform” transition, DACCS can be construed as “fit-and-conform”, and CS can be seen as within the “stretch-and-conform.”

Are turbulence effects on droplet collision–coalescence a key to understanding observed rain formation in clouds?

Rain formation is a critical factor governing the lifecycle and radiative forcing of clouds and therefore it is a key element of weather and climate. Cloud microphysics-turbulence interactions occur across a wide range of scales and are challenging to represent in atmospheric models with limited resolution. Based on past experiments and idealized numerical simulations, it has been postulated that cloud turbulence accelerates rain formation by enhancing drop collision-coalescence. We provide substantial evidence for significant impacts of turbulence on the evolution of cloud droplet size distributions and rain formation by comparing high-resolution observations of cumulus congestus clouds with state-of-the-art large-eddy simulations coupled with a Lagrangian particle-based microphysics scheme. Turbulent coalescence must be included in the model to accurately represent the observed drop size distributions, especially for drizzle drop sizes at lower heights in the cloud. Turbulence causes earlier rain formation and greater rain accumulation compared to simulations with gravitational coalescence only. The observed rain size distribution tail just above cloud base follows a power law scaling that deviates from theoretical scalings considering either a purely gravitation collision kernel or a turbulent kernel neglecting droplet inertial effects, providing additional evidence for turbulent coalescence in clouds. In contrast, large aerosols acting as cloud condensation nuclei ("giant CCN") do not significantly impact rain formation owing to their long timescale to reach equilibrium wet size relative to the lifetime of rising cumulus thermals. Overall, turbulent drop coalescence exerts a dominant influence on rain initiation in warm cumulus clouds, with limited impacts of giant CCN.

Simulations of primary and secondary ice production during an Arctic mixed-phase cloud case from the Ny-Ålesund Aerosol Cloud Experiment (NASCENT) campaign

Abstract. The representation of Arctic clouds and their phase distributions, i.e., the amount of ice and supercooled water, influences predictions of future Arctic warming. Therefore, it is essential that cloud phase is correctly captured by models in order to accurately predict the future Arctic climate. Ice crystal formation in clouds happens through ice nucleation (primary ice production) and ice multiplication (secondary ice production). In common weather and climate models, rime splintering is the only secondary ice production process included. In addition, prescribed number concentrations of cloud condensation nuclei or cloud droplets and ice-nucleating particles are often overestimated in Arctic environments by standard model configurations. This can lead to a misrepresentation of the phase distribution and precipitation formation in Arctic mixed-phase clouds, with important implications for the Arctic surface energy budget. During the Ny-Ålesund Aerosol Cloud Experiment (NASCENT), a holographic probe mounted on a tethered balloon took in situ measurements of number and mass concentrations of ice crystals and cloud droplets in Svalbard, Norway, during fall 2019 and spring 2020. In this study, we choose one case study from this campaign that shows evidence of strong secondary ice production and use the Weather Research and Forecasting (WRF) model to simulate it at a high vertical and spatial resolution. We test the performance of different microphysical parametrizations and apply a new state-of-the-art secondary ice parametrization. We find that agreement with observations highly depends on the prescribed cloud condensation nuclei/cloud droplet and ice-nucleating particle concentrations and requires an enhancement of secondary ice production processes. Lowering mass mixing ratio thresholds for rime splintering inside the Morrison microphysics scheme is crucial to enable secondary ice production and thereby match observations for the right reasons. In our case, rime splintering is required to initiate collisional breakup. The simulated contribution from collisional breakup is larger than that from droplet shattering. Simulating ice production correctly for the right reasons is a prerequisite for reliable simulations of Arctic mixed-phase cloud responses to future temperature or aerosol perturbations.

Is a more physical representation of aerosol chemistry needed for fog forecasting?

AbstractWith the changing climate, the study of fog formation is essential due to the impact of the complexity of natural and anthropogenic aerosols. The evolution of the droplet size distribution in the presence of different aerosol species remains poorly understood. To make progress towards reducing the uncertainty of fog forecasts, the Eulerian–Lagrangian particle‐based small‐scale model for the diffusional growth of droplets is used to better understand the droplet activation and growth. The small‐scale model simulations are performed using observed data from the Winter Fog Experiment study over Indira Gandhi International Airport, New Delhi. The microphysical properties, such as droplet number concentrations (Nd) and liquid water content (LWC), important for fog simulation, are evaluated to gain more insights. The small‐scale simulations have shown the droplet microphysical properties at different evolutionary stages. The Nd and effective radius change with variations in LWC for different aerosol chemistries (i.e., organics, mix, and inorganic). The calculated visibility at small scale is also shown with the variation of Nd and LWC. This study compared visibility from an existing parametrization with parcel–direct numerical simulation calculation. The hygroscopicity , which is highly related to the activation of aerosols to condensation nuclei, is taken into account to demonstrate the contribution of aerosol chemistry to fog droplet formation. The results highlight that hygroscopicity is essential in the numerical model for fog and visibility prediction as the microphysical properties of fog are regulated by aerosol species.

Aitken Mode Aerosols Buffer Decoupled Mid‐Latitude Boundary Layer Clouds Against Precipitation Depletion

AbstractAerosol‐cloud‐precipitation interactions are a leading source of uncertainty in estimating climate sensitivity. Remote marine boundary layers where accumulation mode (∼100–400 nm diameter) aerosol concentrations are relatively low are very susceptible to aerosol changes. These regions also experience heightened Aitken mode aerosol (∼10–100 nm) concentrations associated with ocean biology. Aitken aerosols may significantly influence cloud properties and evolution by replenishing cloud condensation nuclei and droplet number lost through precipitation (i.e., Aitken buffering). We use a large‐eddy simulation with an Aitken‐mode enabled microphysics scheme to examine the role of Aitken buffering in a mid‐latitude decoupled boundary layer cloud regime observed on 15 July 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic flight campaign: cumulus rising into stratocumulus under elevated Aitken concentrations (∼100–200 mg−1). In situ measurements are used to constrain and evaluate this case study. Our simulation accurately captures observed aerosol‐cloud‐precipitation interactions and reveals time‐evolving processes driving regime development and evolution. Aitken activation into the accumulation mode in the cumulus layer provides a reservoir for turbulence and convection to carry accumulation aerosols into the drizzling stratocumulus layer above. Further Aitken activation occurs aloft in the stratocumulus layer. Together, these activation events buffer this cloud regime against precipitation removal, reducing cloud break‐up and associated increases in heterogeneity. We examine cloud evolution sensitivity to initial aerosol conditions. With halved accumulation number, Aitken aerosols restore accumulation concentrations, maintain droplet number similar to original values, and prevent cloud break‐up. Without Aitken aerosols, precipitation‐driven cloud break‐up occurs rapidly. In this regime, Aitken buffering sustains brighter, more homogeneous clouds for longer.

High-accuracy method for modeling nucleation and growth of particles

High-accuracy method for modeling nucleation and growth of particles

On the theory of nucleation of coherent inclusions in irradiated crystals

Based on a critical analysis of the existing model for the effect of excess vacancies and interstitials on the nucleation of coherent particles under irradiation, a new nucleation model is developed that uses the Brailsford-Bullough model for the steady state occupation probabilities of vacancies and interstitials at the particle interface, recently refined by the author. It is shown that, depending on the surface tension γ of a coherent particle, the nucleation mechanism can be qualitatively different. In the case of a relatively small γ, an instability can arise in the irradiated solid solution leading to the barrier-free nucleation of coherent precipitates. In the opposite case of a relatively large γ, the classical one-dimensional theory of homogeneous nucleation is applicable. In order to eliminate the uncertainty in the magnitude of surface tension (from the literature) and to better understand the underlying mechanisms of coherent particle nucleation in irradiation tests, additional atomistic studies are recommended.

Evidence of Surface-Tension Lowering of Atmospheric Aerosols by Organics from Field Observations in an Urban Atmosphere: Relation to Particle Size and Chemical Composition.

Surface-active organics lower the aerosol surface tension (σs/a), leading to enhanced cloud condensation nuclei (CCN) activity and potentially exerting impacts on the climate. Quantification of σs/a is mainly limited to laboratory or modeling work for particles with selected sizes and known chemical compositions. Inferred values from ambient aerosol populations are deficient. In this study, we propose a new method to derive σs/a by combining field measurements made at an urban site in northern China with the κ-Köhler theory. The results present new evidence that organics remarkably lower the surface tension of aerosols in a polluted atmosphere. Particles sized around 40 nm have an averaged σs/a of 53.8 mN m-1, while particles sized up to 100 nm show σs/a values approaching that of pure water. The dependence curve of σs/a with the organic mass resembles the behavior of dicarboxylic acids, suggesting their critical role in reducing the surface tension. The study further reveals that neglecting the σs/a lowering effect would result in lowered ultrafine CCN (diameter <100 nm) concentrations by 6.8-42.1% at a typical range of supersaturations in clouds, demonstrating the significant impact of surface tension on the CCN concentrations of urban aerosols.

Aerosol‐Cloud Interactions Near Cloud Base Deteriorating the Haze Pollution in East China

AbstractAtmospheric aerosols not only cause severe haze pollution, but also affect climate through changes in cloud properties. However, during the haze pollution, aerosol‐cloud interactions are not well understood due to a lack of in situ observations. In this study, we conducted simultaneous observations of cloud droplet and particle number size distribution, together with supporting atmospheric parameters, from ground to cloud base in East China using a high‐payload tethered airship. We found that high concentrations of aerosols and cloud condensation nuclei were constrained below cloud, leading to the pronounced “Twomey effect” near the cloud base. The cloud inhibited the pollutants dispersion by reducing surface heat flux and thus deteriorated the near‐surface haze pollution. Satellite retrievals matched well with the in situ observations for low stratus clouds, while were insufficient to quantify aerosol‐cloud interactions for other cases. Our results highlight the importance to combine in situ vertical and satellite observations to quantify the aerosol‐cloud interactions.

Natural Marine Precursors Boost Continental New Particle Formation and Production of Cloud Condensation Nuclei.

Marine dimethyl sulfide (DMS) emissions are the dominant source of natural sulfur in the atmosphere. DMS oxidizes to produce low-volatility acids that potentially nucleate to form particles that may grow into climatically important cloud condensation nuclei (CCN). In this work, we utilize the chemistry transport model ADCHEM to demonstrate that DMS emissions are likely to contribute to the majority of CCN during the biological active period (May-August) at three different forest stations in the Nordic countries. DMS increases CCN concentrations by forming nucleation and Aitken mode particles over the ocean and land, which eventually grow into the accumulation mode by condensation of low-volatility organic compounds from continental vegetation. Our findings provide a new understanding of the exchange of marine precursors between the ocean and land, highlighting their influence as one of the dominant sources of CCN particles over the boreal forest.

The Preliminary Application of Spectral Microphysics in Numerical Study of the Effects of Aerosol Particles on Thunderstorm Development

Progress in numerical models and improved computational capabilities have significantly advanced our comprehension of how aerosol particles impact thunderstorm clouds. Yet, much of this research has focused on employing bulk microphysics models to explain the impacts of aerosol particles acting as cloud condensation nuclei (CCN) on electrical activities in thunderstorm clouds. The bulk thunderstorm models use mean sizes of particles and terminal-fall velocities. This causes calculation deviation in the electrification simulation, which in turn leads to deviations in the simulation of lightning processes. Developing this further, we established a three-dimensional high-resolution cloud–aerosol bin thunderstorm model with electrification and lightning to provide more accurate microphysics and dynamic fields for studying electrical activities. For evaluating the impacts of aerosol particles, specifically CCN, on the properties of continental thunderclouds, aerosols from both clean and polluted continental environments were selected. Cloud simulations indicate that droplets develop a narrower spectrum in polluted continental conditions, and weakened ice crystal growth increases the number of small ice crystals compared to clean conditions. Smaller droplets and ice crystals result in less effective riming and decreased graupel concentration and mass. Consequently, a significant decrease in large ice particles leads to a weakened process of charge separation under conditions of pollution. As a direct result, there is about a 43% reduction in lightning frequency and a delay of approximately 5 min in the lightning process under polluted conditions.

The Association Between Cloud Droplet Number over the Summer Southern Ocean and Air Mass History

AbstractThe cloud properties and governing processes in Southern Ocean marine boundary layer clouds have emerged as a central issue in understanding the Earth's climate sensitivity. While our understanding of Southern Ocean cloud feedbacks have evolved in the most recent climate model intercomparison, the background properties of simulated summertime clouds in the Southern Ocean are not consistent with measurements due to known biases in simulating cloud condensation nuclei concentrations. This paper presents several case studies collected during the Capricorn 2 and Marcus campaigns held aboard Australian research vessels in the Austral Summer of 2018. Combining the surface‐observed cases with MODIS data along forward and backward air mass trajectories, we demonstrate the evolution of cloud properties with time. These cases are consistent with multi‐year statistics showing that long trajectories of air masses over the Antarctic ice sheet are critical to creating high droplet number clouds in the high latitude summer Southern Ocean. We speculate that secondary aerosol production via the oxidation of biogenically derived aerosol precursor gasses over the high actinic flux region of the high latitude ice sheets is fundamental to maintaining relatively high droplet numbers in Southern Ocean clouds during Summer.

Road Traffic Emissions Lead to Much Enhanced New Particle Formation through Increased Growth Rates.

New particle formation (NPF) is a major source of atmospheric aerosol particles, including cloud condensation nuclei (CCN), by number globally. Previous research has highlighted that NPF is less frequent but more intense at roadsides compared to urban background. Here, we closely examine NPF at both background and roadside sites in urban Central Europe. We show that the concentration of oxygenated organic molecules (OOMs) is greater at the roadside, and the condensation of OOMs along with sulfuric acid onto new particles is sufficient to explain the growth at both sites. We identify a hitherto unreported traffic-related OOM source contributing 29% and 16% to total OOMs at the roadside and background, respectively. Critically, this hitherto undiscovered OOM source is an essential component of urban NPF. Without their contribution to growth rates and the subsequent enhancements to particle survival, the number of >50 nm particles produced by NPF would be reduced by a factor of 21 at the roadside site. Reductions to hydrocarbon emissions from road traffic may thereby reduce particle numbers and CCN counts.

Direct measurements of sea spray particle fluxes using a high temporal resolution optical particle counter over the coastal ocean

ABSTRACT Sea spray particles play a key role in transferring momentum, heat, and gas across the atmosphere–ocean interface at high wind speeds and represent an important source of cloud condensation nuclei which affect the genesis, chemistry, and radiative properties of marine clouds. Here, we present direct measurements of sea spray particle fluxes obtained using an eddy covariance technique through the use of a newly developed high temporal resolution optical particle counter. With this instrumentation measurements were made over the coastal ocean during a 5-week field campaign conducted at an observation pier from November to December 2021. Our optical particle counter was capable of measuring size spectra at a rate of 10 Hz in 8 channels covering a range of mean radii between 0.3 and 15. The power spectra of particle number density followed the Kolmogorov −2/3 power law. The shape of the cospectrum of the particle number density flux was basically similar to that of the cospectra of the heat and gas fluxes. The measured sea spray particle fluxes at mean wind speeds of up to 21 m s−1 were dominated by an upward flux, which likely represents aerosol production caused by the bursting of bubbles at the ocean surface.

Long-term observations of cloud condensation nuclei (CCN) characteristics of atmospheric aerosols: Results from a rural location in India

Long-term measurement of cloud condensation nuclei (CCN) is essential to assess the role of seasonally varying aerosol sources and underlying synoptical meteorological conditions in aerosol-cloud interactions. However, long-term measurement of CCN is limited over the Indian region and globally. This study provides first-ever long-term observations of CCN concentrations at different supersaturation (SS) values ranging from 0.2 to 1.0% using a CCN counter from a rural location of Gadanki, India (13.5°N, 79.2°E, and 375 m AMSL) during October 2019–August 2023. The total CCN concentration (NCCN) was the highest during pre-monsoon season (2847 ± 1148 #/cc), followed by winter (2463 ± 1066 #/cc), post-monsoon (2124 ± 1145 #/cc), and monsoon (1099 ± 740 #/cc) at 0.4% SS. Diurnal variations in NCCN showed bi-modal distribution with a relatively weak peak at around 8:00 h (Local time, LT) and a substantial rise at about 20 h LT. However, a systematic increase in NCCN was observed during the daytime in all the seasons except for the monsoon. The two peaks in diurnal variation of NCCN were associated with CCN of sizes less than 2 μm. The peak diameter of the mono-modal size distribution of CCN shifted towards the higher SS, implying the growth of small aerosols and available CCN. The broad peak indicates that most aerosol particles over Gadanki grow at the SS of 0.4%. Estimates of the k-parameter (Twomey's empirical fit) show the aerosols over Gadanki are relatively more hygroscopic during the monsoon than in winter, with their respective k-values of 0.7 and 0.4. Further, the diurnal variation in the k-parameter suggests significant variability in hygroscopicity within a day during monsoon and winter. Comparison with other locations suggests the CCN concentrations over Gadanki lies between those of polluted urban, coastal, and high-altitude stations.

Fast formation of large ice pebbles after FU Orionis outbursts

During their formation, nascent planetary systems are subject to FU Orionis outbursts that heat a substantial part of the disc. This causes water ice in the affected part of the disc to sublimate as the ice line moves outwards to several to tens of astronomical units. In this paper, we investigate how the subsequent cooling of the disc impacts the particle sizes. We calculate the resulting particle sizes in a disc model with cooling times between 100 and 1000 yr, corresponding to typical FU Orionis outbursts. As the disc cools and the ice line retreats inwards, water vapour forms icy mantles on existing silicate particles. This process is called heterogeneous nucleation. The nucleation rate per surface area of silicate substrate strongly depends on the degree of super-saturation of the water vapour in the gas. Fast cooling results in high super-saturation levels, high nucleation rates, and limited condensation growth because the main ice budget is spent in the nucleation. Slow cooling, on the other hand, leads to rare ice nucleation and efficient growth of ice-nucleated particles by subsequent condensation. We demonstrate that close to the quiescent ice line, pebbles with a size of about centimetres to decimetres form by this process. The largest of these are expected to undergo cracking collisions. However, their Stokes numbers still reach values that are high enough to potentially trigger planetesimal formation by the streaming instability if the background turbulence is weak. Stellar outbursts may thus promote planetesimal formation around the water ice line in protoplanetary discs.

Characteristics of new particle formation events occurred over the Yellow Sea in Springtime from 2019 to 2022

Characteristics of atmospheric new particle formation (NPF) events were investigated using the data obtained from the ship measurement campaign named Yellow Sea Air Quality (YES-AQ) over the Yellow Sea during the springtime from 2019 to 2022. NPF events occurred 15 times for the valid 128 observation days for the four-year period, and the average and standard deviation formation rate (FR) and growth rate (GR) of the NPF events were 2.38 ± 1.53 cm−3 s−1 and 4.11 ± 2.81 nm h−1, respectively. The FR and GR were close to those in urban regions, implying the unique characteristics of the Yellow Sea. Owing to the NPF events, the number concentrations of total aerosols and nucleation mode particles increased by approximately 7850 and 6002 cm−3, respectively, and those of cloud condensation nuclei at 0.2% and 0.6% supersaturation increased by about 1269 and 3269 cm−3, respectively. The NPF events mostly occurred under the meteorological conditions of low temperature and relative humidity as well as high solar radiation and wind speed. These meteorological conditions appeared predominantly when the air mass originated from the continent north of the Korean Peninsula. The current analyses based on the data measured repeatedly during a specific period each year, which were not well conducted in other maritime NPF studies, highlight the reliability of the presented characteristics of NPF events over the Yellow Sea.

Long term variation of microphysical properties of black carbon in Beijing derived from observation and machine learning

The microphysical attributes of black carbon (BC) can determine its absorption and hygroscopic properties. However, long-term information is difficult to obtain from the field. In this study, the BC properties including mass concentration, the coating volume ratio (VR) relative to the refractory BC (rBC), the rBC diameter and the fraction of cloud condensation nuclei (CCN), are derived from a number of field experiments using a random forest model. This model effectively derives the long-term BC microphysical properties in the Beijing region from 2013 to 2020 using continuous measurements of particulate matter, gas, BC mass concentration and meteorological parameters. The results reveal notably higher BC coatings (mean VR = 7.2) and a greater fraction of CCN-like BC (51%) in the winter compared to other seasons. Following the implementation of national air pollution control measures in 2017, BC mass exhibited a substantial reduction of 60% (29%) in the winter (summer), and VR decreased by 45% (24%). Apart from the influence of meteorological variations, these can be attributed to the declined primary emissions and the gas precursors which are associated with secondary formation of BC coatings. The reduction of both BC mass loading and coatings leads to its solar absorption decreasing by 50%, and the fraction of CCN-like BC (likely in clouds) decreasing by 23%. Environmental regulation will therefore continue to reduce both direct and indirect radiative impacts of BC in this region.

Enhanced 3D printing and crack control in melt-grown eutectic ceramic composites with high-entropy alloy doping

As a 3D printing method, laser powder bed fusion (LPBF) technology has been extensively proven to offer significant advantages in fabricating complex structured specimens, achieving ultra-fine microstructures, and enhancing performances. In the domain of manufacturing melt-grown oxide ceramics, it encounters substantial challenges in suppressing crack defects during the rapid solidification process. The strategic integration of high entropy alloys (HEA), leveraging the significant ductility and toughness into ceramic powders represents a major innovation in overcoming the obstacles. The ingenious doping of HEA particles preserves the eutectic microstructures of the Al2O3/GdAlO3(GAP)/ZrO2 ceramic composite. The high damage tolerance of the HEA alloy under high strain rates enables the absorption of crack energy and alleviation of internal stresses during LPBF, effectively reducing crack initiation and growth. Due to increased curvature forces and intense Marangoni convection at the top of the molt pool, particle collision intensifies, leading to the tendency of HEA particles to agglomerate at the upper part of the molt pool. However, this phenomenon can be effectively alleviated in the remelting process of subsequent layer deposition. Furthermore, a portion of the HEA particles partially dissolves and sinks into the molten pool, acting as heterogeneous nucleation particles, inducing the formation of equiaxed eutectic and leading primary phase nucleation. Some HEA particles diffuse into the lamellar ternary eutectic structures, further promoting the refinement of eutectic microstructures due to increased undercooling. The innovative doping of HEA particles has effectively facilitated the fabrication of turbine-structured, conical, and cylindrical ternary eutectic ceramic composite specimens with diameters of about 70 mm, demonstrating significant developmental potential in the field of ceramic composite manufacturing.