Low Number Concentrations Research Articles

Airborne Observations of Highly Variable and Complex Freezing Drizzle and Mixed-Phase Environments

Abstract Airframe icing caused by interactions with supercooled cloud droplets and precipitation can pose a risk to aviation operations and life safety. The In-Cloud Icing and Large-drop Experiment (ICICLE) was conducted in January–March 2019 to capture measurements in freezing conditions in support of the Federal Aviation Administration (FAA) Terminal Area Icing Weather Information for NextGen (TAIWIN) program. The National Research Council of Canada’s Convair-580 research aircraft fulfilled the airborne data collection requirements for the ICICLE campaign and sampled icing clouds and atmospheric conditions over the midwestern United States. ICICLE flight 18, conducted on 17 February 2019, collected cloud and precipitation measurements during a widespread storm that generated supercooled small drops and freezing drizzle (FZDZ) within both liquid and mixed-phase regions. Supercooled liquid water content (LWC) typically ranged 0.30–0.45 g m−3 and exceeded 0.70 g m−3 in one instance. Maximum FZDZ diameters of 300–400 μm were commonly sampled near the base of clouds. Missed approaches performed at four Illinois airfields provided measurements of conditions from near ground level to above cloud top and supplied information regarding FZDZ formation and evolution. FZDZ was found to form at altitudes featuring relatively high LWC and sufficiently low droplet number concentrations. FZDZ formation zones were sometimes collocated with regions of atmospheric instability and/or wind shear. Flight through highly variable supercooled cloud droplet and FZDZ conditions resulted in significant Convair-580 airframe icing, highlighting the risk that icing conditions can pose to aircraft safety.

The Transition from Aerosol- to Updraft-Limited Susceptibility Regime in Large-Eddy Simulations with Bulk Microphysics

Large-eddy simulation (LES) is often used as a benchmark simulation in climate science and is suggested as a fundamental tool to examine, e.g., marine cloud brightening. Therefore, it is necessary to critically evaluate if these high-resolution models can skillfully simulate expected physical phenomena. This study focuses on the first indirect aerosol effect in warm stratocumulus clouds. We investigate if an LES code with explicit aerosol-cloud interactions and a widely used two-moment bulk microphysical scheme can reproduce well-known cloud droplet number susceptibility regimes previously identified by observations and supported by detailed parcel model simulations—the updraft-limited regime (typically occurring at high aerosol number concentrations and low updraft speeds) and the aerosol-limited regime (typically occurring at low aerosol number concentrations and high updraft speeds). Our simulations show that the LES in its default configuration cannot reproduce the two regimes if the initial droplet radius of newly activated droplets (rid) is estimated by integrating the wet aerosol size distribution. The main reason is related to the relatively coarse (but commonly used) time step in the model (Δt ≈ 1s), which is too long to resolve relevant microphysical processes adequately at high aerosol concentrations. A regime transition does occur if the timestep is decreased to Δt ≈ 0.1s and if a renormalization procedure is applied, which limits the number of activated droplets so that the water mass of the newly activated droplets cannot exceed the available amount of supersaturated water vapor. Another way to obtain a regime transition is to increase rid to values >1 µm. However, a clear recommendation for the choice of rid cannot be made upon physical arguments. An alternative solution could be to introduce a sub-time-stepping or adaptive time-stepping algorithm to calculate droplet formation and growth, particularly for updraft-limited conditions. Our study highlights the importance of critically evaluating LES results to guarantee that relevant physical processes are properly represented.

Evolution of refractory black carbon mixing state in an urban environment

The size distribution and hygroscopicity of the refractory black carbon (rBC) aerosol are critical properties for understanding its impact on human health, the extent to which the particles disperse through the atmosphere, and the effect that the particles have on clouds and the climate system. The hygroscopicity of black carbon is primarily controlled by the degree to which the black carbon cores are coated with other compounds. Here we show new measurements of rBC obtained from a single particle soot photometer at an urban location in Houston, TX, USA during the Department of Energy TRacking Aerosol Convection Interactions ExpeRiment (TRACER) campaign. We classified rBC particles into uncoated, thinly coated and thickly coated, where the latter is defined as the optical coating thickness exceeding 10 nm. To understand how aerosol aging and the prevailing winds interact to affect rBC coatings, a slice of the size distribution with rBC core diameter 143–166 nm is considered. For this slice, the average coating thickness of thickly coated particles was 29 ± 8 nm. The rBC number concentration, the fraction of thinly and thickly coated particles, and the average coating thickness strongly vary with the wind direction. We found that onshore flows are associated with lower number concentrations, more thinly coated particles, and thinner coatings when compared to offshore flows. Diurnal profiles show that the fraction of coated particles increases during daytime, likely due to photochemical aging. The estimated fraction of rBC particles that may activate into cloud droplets at 0.1% and 1% water supersaturation was generally ∼0.6% and ∼9%, respectively. This suggests that substantial further aging is needed to precondition the majority of rBC particles for incorporation into cloud droplets.

A New Method for Size‐Resolved Aerosol CCN Activity Measurement at Low Supersaturation in Pristine Atmosphere

AbstractUnderstanding aerosol‐cloud interactions under pristine atmospheric conditions is crucial for meaningful global climate change predictions. However, ability of aerosol particles to act as cloud condensation nuclei (CCN) activity of aerosols in pristine atmosphere remains limited, mainly because of the difficulty of measuring it in pristine environments. Given the extremely low CCN number concentration under low supersaturations (SSs) and the complex impact of the kinetic limitation in CCN measurements, size‐resolved CCN activity measurements at low SSs cannot be achieved with traditional methods using differential mobility analyzers and a CCN counter (CCNC) because of the low sample efficiency and the impact of particles with multiple charges. To overcome this difficulty, we propose a new method for measuring size‐resolved CCN activity at low aerosol number concentrations. The new method is based on a combined system comprising an aerodynamic aerosol classifier (AAC) and a CCNC (AAC‐CCNC system). A control program was developed to achieve high‐resolution scans of the SS and particle size within a reasonable time frame. A data inversion scheme, including corrections for the transfer function and kinetic limitation, was developed to obtain accurate size‐resolved CCN activity. In July‐August 2022, the new method was used to measure the size‐resolved CCN activity on the Tibetan Plateau. This new method can advance the size‐resolved CCN measurements, thereby enhancing our understanding of aerosol‐cloud interactions in pristine atmosphere.

Towards zero pollution vehicles by advanced fuels and exhaust aftertreatment technologies

Vehicular emissions deteriorate air quality in urban areas notably. The aim of this study was to conduct an in-depth characterization of gaseous and particle emissions, and their potential to form secondary aerosol emissions, of the cars meeting the most recent emission Euro 6d standards, and to investigate the impact of fuel as well as engine and aftertreatment technologies on pollutants at warm and cold ambient temperatures. Studied vehicles were a diesel car with a diesel particulate filter (DPF), two gasoline cars (with and without a gasoline particulate filter (GPF)), and a car using compressed natural gas (CNG). The impact of fuel aromatic content was examined for the diesel car and the gasoline car without the GPF. The results showed that the utilization of exhaust particulate filter was important both in diesel and gasoline cars. The gasoline car without the GPF emitted relatively high concentrations of particles compared to the other technologies but the implementation of the GPF decreased particle emissions, and the potential to form secondary aerosols in atmospheric processes. The diesel car equipped with the DPF emitted low particle number concentrations except during the DPF regeneration events. Aromatic-free gasoline and diesel fuel efficiently reduced exhaust particles. Since the renewal of vehicle fleet is a relatively slow process, changing the fuel composition can be seen as a faster way to affect traffic emissions.

Contrail formation on ambient aerosol particles for aircraft with hydrogen combustion: a box model trajectory study

Abstract. Future air traffic using (green) hydrogen (H2) promises zero carbon emissions, but the effects of contrails from this new technology have hardly been investigated. We study contrail formation behind aircraft with H2 combustion by means of the particle-based Lagrangian Cloud Module (LCM) box model. Assuming the absence of soot and ultrafine volatile particle formation, contrail ice crystals form solely on atmospheric background particles mixed into the plume. While a recent study extended the original LCM with regard to the contrail formation on soot particles, we further advance the LCM to cover the contrail formation on ambient particles. For each simulation, we perform an ensemble of box model runs using the dilution along 1000 different plume trajectories. The formation threshold temperature of H2 contrails is around 10 K higher than for conventional contrails (which form behind aircraft with kerosene combustion). Then, contrail formation becomes primarily limited by the homogeneous freezing temperature of the water droplets such that contrails can form at temperatures down to around 234 K. The number of ice crystals formed varies strongly with ambient temperature even far away from the contrail formation threshold. The contrail ice crystal number clearly increases with ambient aerosol number concentration and decreases significantly for ambient particles with mean dry radii ⪅ 10 nm due to the Kelvin effect. Besides simulations with one aerosol particle ensemble, we analyze contrail formation scenarios with two co-existing aerosol particle ensembles with different mean dry sizes or hygroscopicity parameters. We compare them to scenarios with a single ensemble that is the average of the two aerosol ensembles. We find that the total ice crystal number can differ significantly between the two cases, in particular if nucleation-mode particles are involved. Due to the absence of soot particle emissions, the ice crystal number in H2 contrails is typically reduced by more than 80 %–90 % compared to conventional contrails. The contrail optical thickness is significantly reduced, and H2 contrails either become visible later than kerosene contrails or are not visible at all for low ambient particle number concentrations. On the other hand, H2 contrails can form at lower flight altitudes where conventional contrails would not form.

Modification of Microphysical Parameterization Schemes and Their Application in the Simulation of an Extremely Heavy Rainfall Event in Zhengzhou

AbstractIn the present study, the Morrison and Thompson microphysics schemes in the Weather Research and Forecasting model were improved and used to simulate a record‐breaking heavy rainfall event occurred in Henan Province over central China during 19–21 July 2021. In the modified schemes, the terminal velocity of graupel and initial cloud droplet concentration were adjusted based on sensitivity tests. Results showed that the modified Morrison scheme (MORR_MOD) better captured the spatial distribution and temporal evolution of precipitation than the original scheme (MORR). Specifically, it produced a 40‐hr cumulative rainfall amount of 963 mm and an extreme hourly rainfall rate of 157.7 mm, which were closer to observations than MORR. Analysis of the dynamic and microphysical structures of the extreme‐rain‐producing convective clusters revealed that MORR_MOD predicted stronger updrafts, higher rain mass content and larger mean mass diameter of raindrops than MORR. By analyzing the tendencies of rain mass and number concentration, it was found that MORR_MOD predicted stronger accretion rates of cloud droplets by rain and weaker auto‐conversion rates of cloud droplets than MORR, which contributed to the high rain mixing ratio and low number concentration, respectively. In addition, MORR_MOD predicted stronger diabatic heating rates than MORR, which were primarily attributed to stronger condensation of water vapor, and may have been the reason why MORR_MOD simulated stronger updrafts.

Comparison of Simulated Warm‐Rain Microphysical Processes in a Record‐Breaking Rainfall Event Using Polarimetric Radar Observations

AbstractDuring 6–7 May 2017, a record‐breaking nocturnal rainfall event occurred in Guangzhou, China, and it was a typical warm‐sector heavy rainfall event under weak synoptic forcing. A prior observational study by the authors revealed that warm‐rain microphysical processes were dominant and responsible for the record‐breaking precipitation. In this study, the double‐moment Morrison, Thompson and NSSL microphysics schemes in WRF are evaluated against polarimetric radar observations in their ability of reproducing observed microphysical characteristics. The Thompson scheme shows the greatest fidelity to the observed raindrop size distribution (RSD) median value, corresponding to the most amount of precipitation forecast. While the Morrison and NSSL simulations overestimate (underestimate) the raindrop size (number concentration), exhibiting continental‐type convective precipitation. The three experiments slightly overestimate differential reflectivity (ZDR), but significantly underestimate specific differential phase (KDP) and liquid water content by about 30%–50%, implying the undervaluation of number of medium‐sized raindrops. Examinations of the occurrence frequencies of ZDR, KDP, mass‐weighted diameter, and logarithmic normalized intercept parameter for rain suggest that all three schemes fail to reproduce the full variability of observed RSD for the extreme rainfall. The vertical variations of RSD parameters and the Kumjian‐Ryzhkov parameter space suggest that the collision–coalescence is the dominant warm‐rain microphysical process but the simulated process is too weak. This may be attributed to the misrepresented RSD near the melting layer, where the raindrops with lower number concentration and larger sizes cannot grow through the collision–coalescence process as actively.

Differences in microphysical properties of cirrus at high and mid-latitudes

Abstract. Despite their proven importance for the atmospheric radiative energy budget, the effect of cirrus on climate and the magnitude of their modification by human activity is not well quantified. Besides anthropogenic pollution sources on the ground, aviation has a large local effect on cirrus microphysical and radiative properties via the formation of contrails and their transition to contrail cirrus. To investigate the anthropogenic influence on natural cirrus, we compare the microphysical properties of cirrus measured at mid-latitude (ML) regions (<60∘ N) that are often affected by aviation and pollution with cirrus measured in the same season in comparatively pristine high latitudes (HLs; ≥60∘ N). The number concentration, effective diameter, and ice water content of the observed cirrus are derived from in situ measurements covering ice crystal sizes between 2 and 6400 µm collected during the CIRRUS-HL campaign (Cirrus in High Latitudes) in June and July 2021. We analyse the dependence of cirrus microphysical properties on altitude and latitude and demonstrate that the median ice number concentration is an order of magnitude larger in the measured mid-latitude cirrus, with 0.0086 cm−3, compared to the high-latitude cirrus, with 0.001 cm−3. Ice crystals in mid-latitude cirrus are on average smaller than in high-latitude cirrus, with a median effective diameter of 165 µm compared to 210 µm, and the median ice water content in mid-latitude cirrus is higher (0.0033 g m−3) than in high-latitude cirrus (0.0019 g m−3). In order to investigate the cirrus properties in relation to the region of formation, we combine the airborne observations with 10 d backward trajectories to identify the location of cirrus formation and the cirrus type, i.e. in situ or liquid origin cirrus, depending on whether there is only ice or also liquid water present in the cirrus history, respectively. The cirrus formed and measured at mid-latitudes (M–M) have a particularly high ice number concentration and low effective diameter. This is very likely a signature of contrails and contrail cirrus, which is often observed in the in situ origin cirrus type. In contrast, the largest effective diameter and lowest number concentration were found in the cirrus formed and measured at high latitudes (H–H) along with the highest relative humidity over ice (RHi). On average, in-cloud RHi was above saturation in all cirrus. While most of the H–H cirrus were of an in situ origin, the cirrus formed at mid-latitudes and measured at high latitudes (M–H) were mainly of liquid origin. A pristine Arctic background atmosphere with relatively low ice nuclei availability and the extended growth of few nucleated ice crystals may explain the observed RHi and size distributions. The M–H cirrus are a mixture of the properties of M–M and H–H cirrus (preserving some of the initial properties acquired at mid-latitudes and transforming under Arctic atmospheric conditions). Our analyses indicate that part of the cirrus found at high latitudes is actually formed at mid-latitudes and therefore affected by mid-latitude air masses, which have a greater anthropogenic influence.

Physicochemical characteristics of airborne microplastics of a typical coastal city in the Yangtze River Delta Region, China

Airborne microplastics (MPs) are important pollutants that have been present in the environment for many years and are characterized by their universality, persistence, and potential toxicity. This study investigated the effects of terrestrial and marine transport of MPs in the atmosphere of a coastal city and compared the difference between daytime and nighttime. Laser direct infrared imaging (LDIR) and polarized light microscopy were used to characterize the physical and chemical properties of MPs, including number concentration, chemical types, shape, and size. Backward trajectories were used to distinguish the air masses from marine and terrestrial transport. Twenty chemical types were detected by LDIR, with rubber (16.7%) and phenol-formaldehyde resin (PFR; 14.8%) being major components. Three main morphological types of MPs were identified, and fragments (78.1%) are the dominant type. MPs in the atmosphere were concentrated in the small particle size segment (20–50 µm). The concentration of MPs in the air mass from marine transport was 14.7 items/m3 – lower than that from terrestrial transport (32.0 items/m3). The number concentration of airborne MPs was negatively correlated with relative humidity. MPs from terrestrial transport were mainly rubber (20.2%), while those from marine transport were mainly PFR (18%). MPs in the marine transport air mass were more aged and had a lower number concentration than those in the terrestrial transport air mass. The number concentration of airborne MPs is higher during the day than at night. These findings could contribute to the development of targeted control measures and methods to reduce MP pollution.

Observations of Fog‐Aerosol Interactions Over Central Greenland

AbstractSupercooled fogs can have an important radiative impact at the surface of the Greenland Ice Sheet, but they are difficult to detect and our understanding of the factors that control their lifetime and radiative properties is limited by a lack of observations. This study demonstrates that spectrally resolved measurements of downwelling longwave radiation can be used to generate retrievals of fog microphysical properties (phase and particle effective radius) when the fog visible optical depth is greater than ∼0.25. For 12 cases of fog under otherwise clear skies between June and September 2019 at Summit Station in central Greenland, nine cases were mixed‐phase. The mean ice particle (optically‐equivalent sphere) effective radius was 24.0 ± 7.8 µm, and the mean liquid droplet effective radius was 14.0 ± 2.7 µm. These results, combined with measurements of aerosol particle number concentrations, provide evidence supporting the hypotheses that (a) low surface aerosol particle number concentrations can limit fog liquid water path, (b) fog can act to increase near‐surface aerosol particle number concentrations through enhanced mixing, and (c) multiple fog events in quiescent periods gradually deplete near‐surface aerosol particle number concentrations.

Improved counting statistics of an ultrafine differential mobility particle size spectrometer system

Abstract. Differential mobility particle size spectrometers (DMPSs) are widely used to measure the aerosol number size distribution. Especially during new particle formation (NPF), the dynamics of the ultrafine size distribution determine the significance of the newly formed particles within the atmospheric system. A precision quantification of the size distribution and derived quantities such as new particle formation and growth rates is therefore essential. However, size-distribution measurements in the sub-10 nm range suffer from high particle losses and are often derived from only a few counts in the DMPS system, making them subject to very high counting uncertainties. Here we show that a CPC (modified Airmodus A20) with a significantly higher aerosol optics flow rate compared to conventional ultrafine CPCs can greatly enhance the counting statistics in that size range. Using Monte Carlo uncertainty estimates, we show that the uncertainties of the derived formation and growth rates can be reduced from 10 %–20 % down to 1 % by deployment of the high statistics CPC on a strong NPF event day. For weaker events and hence lower number concentrations, the counting statistics can result in a complete breakdown of the growth rate estimate with relative uncertainties as high as 40 %, while the improved DMPS still provides reasonable results at 10 % relative accuracy. In addition, we show that other sources of uncertainty are present in CPC measurements, which might become more important when the uncertainty from the counting statistics is less dominant. Altogether, our study shows that the analysis of NPF events could be greatly improved by the availability of higher counting statistics in the used aerosol detector of DMPS systems.

The Characteristics of Raindrop Size Distributions in Different Climatological Regions in South Korea

To understand the microphysical characteristics of rainfall in four different climatological regions (called BOS, BUS, CPO, and JIN) in South Korea, DSDs and their variables, including the mass-weighted mean diameter (Dm) and normalized number concentration (logNw), were examined. To examine the characteristics of DSDs at four sites with different climatology and topography, data measured from Parsivel disdrometer and wind direction from Automatic Weather System (AWS) during rainy seasons from June to August for three years (2018 to 2020) were analyzed. The DSDs variables were calculated using Gamma distribution model. In the coastal area, larger raindrops with a lower number concentration occurred, whereas smaller raindrops with a higher number concentration dominated in the middle land and mountain region. The mountain area of CPO and middle land area of JIN had a larger contribution to the rain rate than that of the coastal area of BOS and JIN in the range of the smallest diameter. The contribution of the drop size to the total number concentration at the CPO and JIN sites was larger (smaller) than that at BOS and BUS in the smallest (larger) diameter. The average shape and slope parameter of gamma model were higher values at the mountain area than at other sites for both rain types, Z-R relation and polarimetric variables were also shown different values at the four studied sites. The intercept coefficient of Z-R relation showed higher values in the mountain area and middle land area than the coastal area. The slope values of Z-R relation were the smallest in the mountain area. The polarimetric variables of ZH and ZDR were shown highest (lowest) value at the coastal region of BOS (mountain area of CPO) site for both rain types. The Dm-rose, which shows the Dm distributions with the wind direction, was used in this study. In the coastal area (mountain and middle land area), the dominant wind was east–southeast (east) direction. The ratio of the smaller diameter to the middle size at BOS was much smaller than that at CPO. In the analysis of the hourly distribution of the Dm and logNw, there were two and four peaks of Dm at BUS and BOS, respectively. There was one peak of the Dm at the CPO and JIN sites. The time variation of the Dm was much higher than that of the logNw.

Ultrafine particles exposure is associated with specific operative procedures in a multi-chair dental clinic

Air quality in dental clinics is critical, especially in light of the severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) pandemic, given that dental professionals and patients are at risk of regular exposure to aerosols and bioaerosols in dental clinics. High levels of ultrafine particles (UFP) may be produced by dental procedures. This study aimed to quantify ultrafine particles (UFP) concentrations in a real multi-chair dental clinic and compare the levels of UFP produced by different dental procedures. The efficiency of a high-volume evacuator (HVE) in reducing the UFP concentrations during dental procedures was also assessed. UFP concentrations were measured both inside and outside of a dental clinic in Shanghai, China during a 12-day period from July to September 2020. Dental activities were recorded during working hours. The mean (±standard deviation) concentrations of indoor and outdoor UFP during the sampling period were 8,209 (±4,407) counts/cm3 and 15,984 (±7,977) counts/cm3, respectively. The indoor UFP concentration was much higher during working hours (10,057 ± 5,725 counts/cm3) than during non-working hours (7,163 ± 2,972 counts/cm3). The UFP concentrations increased significantly during laser periodontal treatment, root canal filling, tooth drilling, and grinding, and were slightly elevated during ultrasonic scaling or tooth extraction by piezo-surgery. The highest UFP concentration (241,136 counts/cm3) was observed during laser periodontal treatment, followed by root canal filling (75,034 counts/cm3), which showed the second highest level. The use of an HVE resulted in lower number concentration of UFP when drilling and grinding teeth with high-speed handpieces, but did not significantly reduce UFP measured during laser periodontal therapy. we found that many dental procedures can generate high concentration of UFP in dental clinics, which may have a great health impact on the dental workers. The use of an HVE may help reduce the exposure to UFP during the use of high-speed handpieces.

Quiet New Particle Formation in the Atmosphere

Atmospheric new particle formation (NPF) has been observed to take place in practice all around the world. In continental locations, typically about 10–40% of the days are so-called NPF event days characterized by a clear particle formation and growth that continue for several hours, occurring mostly during daytime. The other days are either non-event days, or days for which it is difficult to decide whether NPF had occurred or not. Using measurement data from several locations (Hyytiälä, Järvselja, and near-city background and city center of Budapest), we were able to show that NPF tends to occur also on the days traditionally characterized as non-event days. One explanation is the instrument sensitivity towards low number concentrations in the sub-10 nm range, which usually limits our capability to detect such NPF events. We found that during such days, particle formation rates at 6 nm were about 2–20% of those observed during the traditional NPF event days. Growth rates of the newly formed particles were very similar between the traditional NPF event and non-event days. This previously overlooked phenomenon, termed as quiet NPF, contributes significantly to the production of secondary particles in the atmosphere.

Experimental investigation on combustion and emission characteristics of Fischer-Tropsch diesel/gasoline in a multi-cylinder heavy-duty diesel engine under different loads

To compare the combustion and emission characteristics of petroleum diesel (D100), Fischer-Tropsch diesel (FT100, indirect coal-to-liquid) and 80% F-T diesel blended with 20% petroleum gasoline by volume (FTG20), the three fuels were applied in a 6-cylinder heavy-duty diesel engine under different loads. The results show that the lowest premixed combustion is found for FT100, followed by FTG20 and D100, ranked in the descending order of ignitability. FT100 has higher BTE than D100 at high loads with single injection strategy. Adding gasoline to F-T diesel enhances fuel–air mixing quality and thus further increases BTE. However, too early pilot injection at low loads for FT100 and FTG20 is not beneficial to BTE improvement. Moreover, FTG20 has the highest BSHC and BSNOx at all loads. FT100 shows slightly higher BSHC and BSNOx at low loads with split injection, while lower BSNOx and similar BSHC at high loads with single injection than D100. In addition, FT100 has lower number concentration and geometric mean diameter (GMD) of ultrafine particulates (UFPs) than D100 at all loads. With the addition of gasoline, both of GMD at all loads and number concentration at low loads further decrease, but the aromatics, unsaturation and pool fire of gasoline lead to deteriorated ultrafine number concentration at high loads. With further addition of PODE to FTG20, the deteriorating UFPs at high load are improved. The results indicate that the addition of gasoline to FT100 can effectively improve BTE and reduce GMD of UFPs, but BSCO, BSNOx and number concentration at high loads are worsened, and PODE can be selected as a potential additive to reduce the UFPs at high loads.

Studies on the Competition Between Homogeneous and Heterogeneous Ice Nucleation in Cirrus Formation

AbstractCirrus ice crystals are produced heterogeneously on ice‐nucleating particles (INPs) and homogeneously in supercooled liquid solution droplets. They grow by uptake of water molecules from the ice‐supersaturated vapor. The precursor particles, characterized by disparate ice nucleation abilities and number concentrations, compete for available vapor during ice formation events. We investigate cirrus formation events systematically in different temperature and updraft regimes, and for different INP number concentrations and time‐independent nucleation efficiencies. We consider vertical air motion variability due to mesoscale gravity waves and effects of supersaturation‐dependent deposition coefficients for water molecules on ice surfaces. We analyze ice crystal properties to better understand the dynamics of competing nucleation processes. We study the reduction of ice crystal numbers produced by homogeneous freezing due to INPs in both, individual simulations assuming constant updraft speeds and in ensemble simulations based on a stochastic representation of vertical wind speed fluctuations. We simulate and interpret probability distributions of total nucleated ice crystal number concentrations, showing signatures of homogeneous and heterogeneous nucleation. At typically observed, mean updraft speeds (≈15 cm s−1) competing nucleation should occur frequently, even at rather low INP number concentrations (<10 L−1). INPs increase cirrus occurrence and may alter cirrus microphysical properties without entirely suppressing homogeneous freezing events. We suggest to improve ice growth models, especially for low cirrus temperatures (<220 K) and low ice supersaturation (<0.3).

Vertical profile of aerosol number size distribution during a haze pollution episode in Hefei, China

The vertical distribution of aerosols has important implications on haze formation as development, which is manifested to some extent by the planetary boundary layer (PBL)–aerosol interactions. Information on the number concentration and size of particles is essential to understand these processes, but studies on vertical profiles of particle number-size distribution are limited. Herein, an unmanned aerial vehicle (UAV) equipped with a custom-built optical particle counter (0.4–10 μm) was used to investigate the vertical profiles of particle number-size distribution in Hefei (China) during January 20–30, 2021. Combining ground-based scanning mobility particle sizer and meteorological data, the pollution accumulation and diffusion mechanisms were analyzed in depth. Results showed that as the pollution episode developed, the vertical distribution of the particle number concentration changed from a flat profile to a sharp vertical gradient. Under polluted conditions, a three-layer structure was clearly evident: uniform distribution in a mixed layer near the ground, a sharply reduced transition layer, and a low number concentration layer in the free atmosphere. Analysis revealed that fundamental to this conversion is that aerosols are highly affected by the PBL dynamics. Concurrent on-UAV and ground-based observations revealed that the ratio of particle numbers in the accumulation mode to that in the Aitken mode was 0.92 ± 0.05 in polluted days, which was almost three times that of clean days. This difference in the ratio of large to small particles suggests that hygroscopic growth of aerosol particles under high humidity conditions played an important role in haze development. Moreover, the sharp vertical gradient of the particle number concentration in the transition layer was identified as an important parameter for characterizing PBL height. The findings in this study highlight the importance of PBL dynamics on the under-studied vertical profiles of particle number-size distribution, especially during heavy pollution episodes.

Evaluating the Impacts of Cloud Processing on Resuspended Aerosol Particles After Cloud Evaporation Using a Particle‐Resolved Model

AbstractAerosol particles undergo physical and chemical changes during cloud processes. In this work, we quantified the changes in aerosol mixing state using a particle‐resolved model. To this end, we coupled the particle‐resolved aerosol model PartMC‐MOSAIC with the aqueous chemistry module CAPRAM 2.4 and designed cloud parcel simulations that mimicked several cloud cycles that a particle population may be exposed to in polluted urban environments. With ammonium nitrate and ammonium sulfate added to the activated particles, after the cloud evaporated, the activation potential of the resuspended aerosol particles increased for supersaturation thresholds lower than the maximum supersaturation attained in the cloud. Formation of sulfate and nitrate increased the internally mixed state of all particle populations, quantified by the mixing state index χ. The change of aerosol mixing state due to aqueous‐phase chemistry was related to the fraction of activated particles. For a case with low aerosol number concentration, where the activated fraction was up to 60%, χ increased by up to 50 percentage points after cloud processing, reaching an almost completely internal mixture. In contrast, for a case with high aerosol emissions and activated fraction of less than 20%, the increase in χ was less than 20 percentage points, and χ remained below 80% after cloud processing. The change in aerosol mixing state caused by coagulation within the cloud parcel was negligible. These findings highlight the complex influence of cloud processing on particle properties.

Impacts of long-range-transported mineral dust on summertime convective cloud and precipitation: a case study over the Taiwan region

Abstract. As one of the most abundant atmospheric aerosols and effective ice nuclei, mineral dust affects clouds and precipitation in the Earth system. Here numerical experiments are carried out to investigate the impacts of dust aerosols on summertime convective clouds and precipitation over the mountainous region of Taiwan by acting as ice-nucleating particles. We run the Weather Research and Forecasting model (WRF) with the Morrison two-moment and spectral-bin microphysics (SBM) schemes at 3 km resolution, using dust number concentrations from a global chemical transport model (GEOS-Chem-APM). The case study indicates that the long-range-transported mineral dust, with relatively low number concentrations, can notably affect the properties of convective clouds (ice and liquid water contents, cloud top height, and cloud coverage) and precipitation (spatial pattern and intensity). The effects of dust are evident during strong convective periods, with significantly increased ice water contents in the mixed-phase regime via the enhanced heterogeneous freezing. With both the Morrison and SBM schemes, we see the invigoration effects of dust aerosols on the convective intensity through enhanced condensation and deposition latent heating. The low-altitude dust particles are uplifted to the freezing level by updrafts, which, in turn, enhance the convective cloud development through immersion freezing and convective invigoration. Compared to the Morrison scheme, the SBM scheme predicts more realistic precipitation and different invigoration effects of dust. The differences are partially attributed to the saturation adjustment approach utilized in the bulk scheme, which leads to a stronger enhancement of condensation at midlatitudes to low altitudes and a weaker deposition increase at the upper level.