Number Concentration Measurements Research Articles

One-Point Calibration of Low-Cost Sensors for Particulate Air Matter (PM) Concentration Measurement

The use of low-cost sensors has dramatically increased in recent years in all engineering sectors. In the buildings and automotive field, low-cost sensors open very interesting perspectives, because they allow one to monitor temperature and humidity distributions together with air quality in a widespread and punctual way and allow for the control of all energy parameters. The main issue remains the validation of the measurements. In this work, we propose an innovative approach to verify the measurements given by some low-cost systems built ad hoc for automotive applications. Two independent low-cost measurement systems were set to measure Particulate Air Matter (PM) concentration, TVOC concentration, CO2 concentration, formaldehyde concentration, air temperature, relative humidity, pressure, air flow velocity, and GPS position. These systems were calibrated for PM concentration measurement by comparison with standard and certified sensors used by the regional authority of the Emilia-Romagna region (ARPAE, Italy) for characterizing air quality. The duration of the analysis, three days, is not representative of the diverse environmental conditions that occur across different seasons. However, the innovation of this approach lies in both the in-field comparison of low-cost and high-quality sensors and the use of proper conversion approaches for mass concentration measurements. A quantitative analysis of the sensors’ performance is given, with a focus on the effects of time granularity, relative humidity, mass conversion from particle counts, and size detection response. The results show that the low-cost sensors’ measurements of air temperature, relative humidity, and particle number concentration are in good agreement with high-quality sensors’ measurements, with a strong impact of relative humidity on performance indicators. Overall, good quality and consistency of the data among the sensors were achieved.

Balloon Baseline Stratospheric Aerosol Profiles (B2SAP)—Perturbations in the Southern Hemisphere, 2019–2022

AbstractVolcanic and pyrocumulonimbus (pyroCB) injections into the stratosphere perturb the aerosol layer and can have important radiative and chemical impacts on timescales spanning from months to several years. Repeated in situ balloon‐borne measurements of aerosol size and number concentration (>140 nm in diameter), ozone, water vapor, and atmospheric state variables made at midlatitudes in the southern hemisphere (SH) since 2019 enable us to better characterize such events. We use this record and coincident lidar extinction profiles to study several moderate to large stratospheric perturbations in the SH between 2019 and 2022 in detail, including the Australian New Year Super Outbreak (ANYSO) pyroCB in 2020. Median vertical profiles of aerosol number concentration, effective radius, and surface area in SH midlatitudes are also compared with those recorded in Northern Hemisphere midlatitudes under baseline conditions using an identical payload. These data depict the variability in stratospheric aerosol properties in the SH midlatitudes during this period and provide a benchmark for global sectional aerosol models. They reveal that sulfate particle size distributions under baseline conditions and in volcanic plumes are relatively well represented in the Community Earth System Model—Community Aerosol Radiation Model for Atmospheres (CESM‐CARMA), but more observations of biomass burning plumes are needed to improve model skill in simulating pyroCB. Comparisons between in situ and lidar observations also highlight a need for more observations of aerosol composition and refractive index in both fresh and aging biomass burning plumes.

Adding More Shape to Nanoscale Reference Materials─LiYF4:Yb,Tm Bipyramids as Standards for Sizing Methods and Particle Number Concentration.

The increasing industrial use of nanomaterials calls for the reliable characterization of their physicochemical key properties like size, size distribution, shape, and surface chemistry, and test and reference materials (RMs) with sizes and shapes, closely matching real-world nonspheric nano-objects. An efficient strategy to minimize efforts in producing nanoscale RMs (nanoRMs) for establishing, validating, and standardizing methods for characterizing nanomaterials are multimethod nanoRMs. Ideal candidates are lanthanide-based, multicolor luminescent, and chemically inert nanoparticles (NPs) like upconversion nanoparticles (UCNPs), which can be prepared in different sizes, shapes, and chemical composition with various surface coatings. This makes UCNPs interesting candidates as standards not only for sizing methods, but also for element-analytical methods like laser ablation-inductively coupled plasma mass spectrometry (LA-ICP-MS), quantitative bioimaging methods like X-ray fluorescence computed tomography (XFCT), and luminescence methods and correlative measurements. Here, we explore the potential of two monodisperse LiYF4:Yb,Tm bipyramids with peak-to-peak distances of (43 ± 2) nm and (29 ± 2) nm as size standards for small-angle X-ray scattering (SAXS) and tools for establishing and validating the sophisticated simulations required for the analysis of SAXS data derived from dispersions of nonspheric nano-objects. These SAXS studies are supplemented by two-dimensional (2D)-transmission electron microscopy measurements of the UCNP bipyramids. Additionally, the particle number concentration of cyclohexane dispersions of these UCNP bipyramids is determined by absolute SAXS measurements, complemented by gravimetry, thermogravimetric analysis (TGA), and inductively coupled plasma optical emission spectrometry (ICP-OES). This approach enables traceable particle number concentration measurements of ligand-capped nonspheric particles with unknown chemical composition.

Process of SCR Catalyst Deactivation by Dimethylsiloxanes Present in Marine Fuels

In recent years, there have been reports of the deactivation of selective catalytic reduction (SCR) exhaust gas catalysts after a short period of operation in marine applications. The trigger and the processes of this catalyst damage have now been investigated experimentally using a fuel burner test bench and various analysis techniques. It was found that organic silicon compounds (OSCs), which are present in marine fuels after use in mineral oil extraction and processing, cause the catalyst deactivation. In practice, these are predominantly dimethylsiloxanes. By the burner experiments, it was found that the OSCs were completely converted into combustion products, in particular SiO2. Measurements of particle size distributions and particle number concentrations up- and downstream of the catalyst showed that SiO2 particles < 20 nm in particular were retained in the catalyst. This filtration effect decreased until no further reduction was observed for particles > 50 nm. Other inorganic, particulate, SiO2-containing fuel impurities (catalyst fines) had no poisoning effect here, as these particles are mostly > 50 nm. The small particles formed a closed SiO2 layer with a thickness of approx. 5 µm on the catalyst surface which grew from the catalyst inlet to the outlet and blocked the catalyst as a diffusion barrier. As the SiO2 layer increased, the NO conversion rate decreased. The poisoning effects were observed experimentally at OSC concentrations of 5 to 60 mg Si kg−1 fuel. A field-aged catalyst that had been operated on board of a merchant ship revealed the same findings.

Long term measurements of aerosol mass concentration with optical particle counters: Discrepancies with plausible reasons

Gravimetry-based direct measurements of mass concentration require offline analysis which is not suited for field campaigns. Hence such campaigns rely on the estimation of mass concentration by indirect methods mostly calibrated in controlled laboratory conditions. Optical particle counter (OPC) employs algorithms converting the measured number concentration to mass concentration using appropriate conversion factors. The accuracy of such conversion has not been validated for widely varying atmospheric conditions. This study compares the mass concentration estimated by OPC with those directly obtained from gravimetry-based instruments for outdoor samples collected in Bathinda City, Punjab, India from January 2022 to November 2023. The difference in the gravimetrically measured and OPC predicted values quantified in terms of ratios (gravimetric to optically estimated mass concentration), came out to be 1.42 ± 0.77, 0.99 ± 0.51, and 1.17 ± 0.58 for PM10, PM2.5 and PM1, respectively. This difference when estimated with the back-up filter of OPC itself (C Factor), was 1.37 ± 0.66. More than half of the samples showed ratios outside the 0.8–1.2 range thus indicating under or over-estimation in the OPC predicted values. The probable role of variation in density, shape, and refractive index of atmospheric aerosol particles towards the observed inaccuracy of estimated mass concentration has been highlighted. In the absence of clear guidelines and protocols, the study suggests ways to improve the accuracy via periodic measurement of the C Factor and/or incorporating calibration factors in such measurements.

Comparing novel small-angle x-ray scattering approaches for absolute size and number concentration measurements of spherical SiO2 particles to established methods

Biomedical analytical applications, as well as the industrial production of high-quality nano- and sub-micrometre particles, require accurate methods to quantify the absolute number concentration of particles. In this context, small-angle x-ray scattering (SAXS) is a powerful tool to determine the particle size and concentration traceable to the Système international d’unités (SI). Therefore, absolute measurements of the scattering cross-section must be performed, which require precise knowledge of all experimental parameters, such as the electron density of solvent and particles, whereas the latter is often unknown. Within the present study, novel SAXS-based approaches to determine the size distribution, density and number concentrations of sub-micron spherical silica particles with narrow size distributions and mean diameters between 160 nm and 430 nm are presented. For the first-time traceable density and number concentration measurements of silica particles are presented and current challenges in SAXS measurements such as beam-smearing, poorly known electron densities and moderately polydisperse samples are addressed. In addition, and for comparison purpose, atomic force microscopy has been used for traceable measurements of the size distribution and single particle inductively coupled plasma mass spectrometry with the dynamic mass flow approach for the accurate quantification of the number concentrations of silica particles. The possibilities and limitations of the current approaches are critically discussed in this study.

Use of a sample injection loop for an accurate measurement of particle number concentration by flow cytometry

Flow cytometry plays a pivotal role in biotechnology by providing quantitative measurements for a wide range of applications. Nonetheless, achieving precise particle quantification, particularly without relying on counting beads, remains a challenge. In this study, we introduce a novel exhaustive counting method featuring a sample loop–based injection system that delivers a defined sample volume to a detection system to enhance quantification in flow cytometry. We systematically assess the performance characteristics of this system with micron-sized polystyrene beads, addressing issues related to sample introduction, adsorption, and volume measurement. Results underscore the excellent analytical performance of the proposed method, characterized by high linearity and repeatability. We compare our approach to counting bead–based measurements, and while an approximate bias value was observed, the measured values were found to be similar between the methods, demonstrating its comparability and reliability. This method holds great promise for improving the accuracy and precision of particle quantification in flow cytometry, with implications for various fields including healthcare and environmental monitoring.

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.

Tethered balloon measurements reveal enhanced aerosol occurrence aloft interacting with Arctic low-level clouds

Low-level clouds in the Arctic affect the surface energy budget and vertical transport of heat and moisture. The limited availability of cloud-droplet-forming aerosol particles strongly impacts cloud properties and lifetime. Vertical particle distributions are required to study aerosol–cloud interaction over sea ice comprehensively. This article presents vertically resolved measurements of aerosol particle number concentrations and sizes using tethered balloons. The data were collected during the Multidisciplinary drifting Observatory for the Study of Arctic Climate expedition in the summer of 2020. Thirty-four profiles of aerosol particle number concentration were observed in 2 particle size ranges: 12–150 nm (N12−150) and above 150 nm (N&amp;gt;150). Concurrent balloon-borne meteorological measurements provided context for the continuous profiles through the cloudy atmospheric boundary layer. Radiosoundings, cloud remote sensing data, and 5-day back trajectories supplemented the analysis. The majority of aerosol profiles showed more particles above the lowest temperature inversion, on average, double the number concentration compared to below. Increased N12−150 up to 3,000 cm−3 were observed in the free troposphere above low-level clouds related to secondary particle formation. Long-range transport of pollution increased N&amp;gt;150 to 310 cm−3 in a warm, moist air mass. Droplet activation inside clouds caused reductions of N&amp;gt;150 by up to 100%, while the decrease in N12−150 was less than 50%. When low-level clouds were thermodynamically coupled with the surface, profiles showed 5 times higher values of N12−150 in the free troposphere than below the cloud-capping temperature inversion. Enhanced N12−150 and N&amp;gt;150 interacting with clouds were advected above the lowest inversion from beyond the sea ice edge when clouds were decoupled from the surface. Vertically discontinuous aerosol profiles below decoupled clouds suggest that particles emitted at the surface are not transported to clouds in these conditions. It is concluded that the cloud-surface coupling state and free tropospheric particle abundance are crucial when assessing the aerosol budget for Arctic low-level clouds over sea ice.

Efficient droplet activation of ambient black carbon particles in a suburban environment

Abstract. The cloud condensation nuclei (CCN) activity of black carbon (BC) particles importantly determines their impacts on cloud microphysics and atmospheric lifetime. This process is crucially influenced by the number of hygroscopic coating materials that BC acquire during the ageing process. It remains a challenge for ambient measurements to capture this process and link this with CCN activity of BC. Here, we directly measured the droplet activation diameter (D50) and activation fraction of BC-containing (BCc) particles (Fact,BC) in suburban Beijing using coupled measurements of size-resolved number concentrations of CCN at configured water supersaturation (SS) and BCc particles. The number concentration of BCc particles was found to peak at diameter 180–210 nm after acquiring coatings, larger than that for all particles (50–150 nm). Consequently, the initially smaller BC particles become enlarged and more hygroscopic, thereby exhibiting CCN activities than other particles. The Fact,BC increased from 42 % to 69 % in number and from 67 % to 85 % in mass as SS increased from 0.1 % to 0.2 % but tended to reach a plateau when SS &gt; 0.2 %. Notably, Fact,BC and D50 linearly correlated with equivalent photochemical age, at a rate of +2 % h−1 and −3 nm h−1, respectively. The results suggest BCc particles from anthropogenic sources can readily serve as CCN at a relatively low SS, and more than half of the BC population can be activated within a few hours, indicating that the surface-sourced BC can efficiently incorporate into clouds and potentially exert important indirect radiative impacts.

Reply to “Comment on Comparison of direct and indirect measures of transport efficiency in single particle inductively coupled plasma mass spectrometry” by H. Goenaga-Infante

This paper provides a rebuttal to the comments on our original research article entitled “Comparison of Direct and Indirect Measures of Transport Efficiency in Single Particle ICP-MS” recently published by Goenaga-Infante in Spectrochimica Acta Part B: Atomic Spectroscopy.The intent of our study is not to condemn the dynamic mass flow (DMF) method but rather to explore the use parameters under which it can and cannot be applied. As explained in the original paper, the goal of this study is to evaluate the ranges of use conditions under which measures of transport efficiency (TE) yield accurate and reproducible results for spICP-MS measurements of particle number concentration (PNC) and particle size (diameter, PS) of various gold nanoparticle (AuNP) suspensions. The evaluation was performed through a systematic comparison of three methods for the measurement of TE: the particle frequency (TEF), particle size (TES), and DMF methods using three types of spray chambers operated at cooled and ambient temperature conditions and employing different ICP-MS platforms. While we appreciate thorough critical and constructive comments on our paper, we strongly disagree that the conclusions and highlights are not supported by the content and findings about the features and benefits of the DMF method.The discussion of three additional independent studies in this field by other spICP-MS expert groups that have been published after the submission of our manuscript is included in this paper. While the DMF approach has been used in two interlaboratory comparisons for TE determination in spICP-MS measurements of PNC, only one laboratory, namely the laboratory led by Goenaga-Infante, provided results using the DMF method in both projects. A method cannot be considered validated if successful results have only been demonstrated within one laboratory.The paper by Goenaga-Infante claims that the main use of DMF, the assignment of a SI traceable PNC value to new commercial nanomaterials (NMs), has not been highlighted explicitly in our original paper. The advantages and disadvantages of the DMF, TES, and TEF methods to measure TE were presented throughout the manuscript and are clearly summarized in the conclusion. The assignment of PNC that is metrologically traceable to the SI implies that all known or suspected uncertainty components including bias are taken into account. Our research shows that under some use conditions, the biases inherent to the DMF method are not yet fully understood and cannot be accounted for. While Cuello-Nuñez et al. Journal of Analytical Atomic Spectrometry, 2020, DOI: https://doi.org/10.1039/c9ja00415g state that cooled conditions (2 °C) were used in their work, they do not define the level of bias that can be expected if different spray chamber temperatures are used, and they do not provide recommendations on the optimal use conditions that define the field of applicability of the DMF method. Furthermore, besides the use of a Scott-type spray chamber cooled to 2 °C, neither the composition material of the spray chamber nor the volume of the Scott-type spray chamber were specified. It is important to note that in our original research, fifteen of the nineteen experiments were conducted using a cooled spray chamber. Also, the four different ICP-MS platforms were used in the standard configuration and with additional spray chamber options encountered in common ICP-MS usage. The value of our work is that it extends the study of Cuello-Nuñez et al. to a wide variety of use conditions routinely encountered in spICP-MS analysis.

Traceable characterization of hollow organosilica beads as potential reference materials for extracellular vesicle measurements with optical techniques

The concentration of cell-type specific extracellular vesicles (EVs) is a promising biomarker for various diseases. However, concentrations of EVs measured by optical techniques such as flow cytometry (FCM) or particle tracking analysis (PTA) in clinical practice are incomparable. To allow reliable and comparable concentration measurements suitable reference materials (RMs) and SI-traceable (SI—International system of units) methods are required. Hollow organosilica beads (HOBs) are promising RM candidates for concentration measurements of EVs based on light scattering, as the shape, low refractive index, and number concentration of HOBs are comparable to EVs of the respective size range that can be detected with current optical instrumentation. Here, we present traceable methods for measuring the particle size distribution of four HOB types in the size range between 200 and 500 nm by small-angle X-ray scattering (SAXS) and atomic force microscopy (AFM), as well as the number concentration by single-particle inductively coupled plasma mass spectrometry (spICP-MS). Based on the size and shape results, traceable reference values were obtained to additionally determine the refractive index of the shell of the HOB samples by FCM. Furthermore, the estimated refractive indexes of the HOBs plausibly agree with the refractive indexes of EVs of corresponding size. Due to their narrow size distribution and their similar shape, and low refractive index, all HOB samples studied are suitable RM candidates for calibration of the measured sample volume by optical methods within the photon wavelength range used, and thus for calibration of number concentration measurements of EVs in the size range indicated. This was confirmed as the number concentration values obtained by PTA and two independent flow cytometric measurements agreed with the concentration reference values obtained by two independent spICP-MS measurements within the calculated uncertainty limits.

Evaluation of a Partector Pro for atmospheric particle number size distribution and number concentration measurements at an urban background site

Abstract. Particle number size distributions, total number concentrations and mean particle sizes have been measured for 70 d at an urban background site in Mülheim-Styrum, Germany, with a handheld Partector Pro of the first generation and a TSI mobility particle size spectrometer (MPSS). The aim of the study was to evaluate the performance of the Partector Pro against the MPSS. The results show that the size distributions, measured with the Partector Pro, agree with the MPSS mostly within ± 25 % for particle sizes between 10 and 113.5 nm, whereas higher, systematic differences were observed for larger particles. The measurement accuracy was shown to be dependent on the geometric mean diameter and the geometric standard deviation of the aerosol. Best results were found for the most abundant size distributions with geometric mean particle diameters ≥ 30 nm and geometric standard deviations larger than 1.8. The total number concentration, measured by the Partector Pro, was found to be in excellent agreement with the MPSS with a slope of the linear fit of 0.9977 and a regression coefficient of R2=0.9956. The agreement of the geometric mean particle diameter, determined with the Partector Pro and the MPSS was good but moderately dependent on the particle size distribution. For mean particle sizes between 20 and 50 nm, the bias was within ±15 %. Higher deviations of up to 30 % were observed when the geometric mean particle sizes exceeded 70 nm and when the geometric standard deviations exceeded approximately 2.7.

Nanofluidic resistive pulse sensing for characterization of extracellular vesicles.

This paper describes the development, design and characterization of a resistive pulse sensing (RPS) system for the analysis of size distributions of extracellular vesicles (EVs). The system is based on microfluidic chips fabricated using soft-lithography and operated in pressure-driven mode. This fabrication approach provided reproducible pore dimensions and the best performing chip design enabled, without calibration, sizing of both 252 nm and 460 nm test particles within 8% of theoretically calculated values, based on the size specifications provided by suppliers. The number concentration measurement had higher variations and without calibration provided estimates within an order of magnitude, for sample concentrations across 4 orders of magnitude. The RPS chips could also measure successfully EVs and other biological nanoparticles in purified samples from cell culture media and human serum. A compact, fast and inexpensive RPS system based on this design could be an attractive alternative to current gold-standard techniques for routine characterization of EV samples.

Characteristics of airborne particles in stone quarrying areas: Human exposure assessment and mitigation

This investigation aims to assess the levels of human exposure to airborne particulate matter (PM) in various locations of a natural stone quarry for the first time based on simultaneous measurements of both PM mass and number concentrations (PMC and PNC). A quarry located in Danang city, Vietnam, considered to be a “hotspot” of air pollution in the city, was selected for detailed investigations. Both PMC and PNC were found to be significantly higher (1.2–6.0 times) within the quarry compared to surrounding areas. Mechanical activities during mining, notably crushing, screening, hauling, and loading stones, contributed to increased emissions of PM in the coarser mode (1–10 μm) compared to the accumulation mode (0.1–1 μm) and thus increased deposition of PM1-10 in the human upper respiratory tract. In contrast, combustion activities, especially the diesel engine exhaust from various machines and vehicles used in the quarry, resulted in increased emissions of small particles in the accumulation mode that dominated the PNC and in their deposition in the lower respiratory tract. Simultaneous measurements of PNC and PMC revealed that the PM counts were strongly associated with PM deposition in the alveolar region (accounting for ≈ 76% of total PNC of particles less than 10 μm, N10), while the PM mass concentration was a better indicator of the deposition of PM in the head airway region (≈92% of total PMC of PM10). Overall, this study demonstrates the significance of measuring both PNC and PMC to assess PM exposure levels, regional respiratory doses, and potential health effects associated with human exposure to PM generated from stone quarrying activities. The novelty of this work is the integration of real-time mass and number concentrations of PM over the size range from 20 nm to 10 μm to provide insights into respiratory deposited doses of size-fractionated PM among quarry workers.

Development of a physics-based method for calibration of low-cost particulate matter sensors and comparison with machine learning models

Low cost particulate matter sensors are receiving significant attention as they can be used in large number for spatial and temporal measurement of PM mass and number concentration. However, the data reliability is questionable as these sensors are affected by numerous parameters such as temperature, relative humidity, and hygroscopicity of particles. To ensure accurate and reliable measurement of particulate matter concentrations, performance evaluation and calibration of LCS co-located with reference instrument at site is essential. In this study, the performance of the low-cost sensor (APT Maxima) was evaluated with the reference instrument SASS (Speciation Air Sampling System) sampler for developing suitable calibration factor that include impact of the meteorological parameter such as relative humidity and temperature, and hygroscopicity. In this study, we have demonstrated a systematic physics-based method for calibration of LCS based on κ-Köhler theory and Mie theory. For comparison with statistical models, linear regression and machine learning algorithm were also applied. In physics-based model, calculated total light scattered intensity shows good linearity with reference PM2.5 measurements. Physics based model performed better for both the sites as compared to MLR, kNN, RF, and GB ML algorithms with R2, RMSE, and MAE values of 0.72,18.21, and 13.36 for Bhopal site, and 0.91, 7.84, and 5.76 for Kashmir site, respectively. Study indicates that physics-based approach for LCS calibration is suitable and can be transferable to different sites.

Numerical simulation and evaluation of global ultrafine particle concentrations at the Earth's surface

Abstract. A new global dataset of annually averaged ultrafine particle (UFP) concentrations at the Earth's surface for the years 2015–2017 has been developed through numerical simulations using the ECHAM/MESSy Atmospheric Chemistry model (EMAC). We present total and size-resolved concentrations along with their interannual variability. Size distributions of emitted particles from the contributing source sectors have been derived based on literature reports. The model results of UFP concentrations are evaluated using particle size distribution and particle number concentration measurements from available datasets and the literature. While we obtain reasonable agreement between the model results and observations (logarithmic-scale correlation of r=0.76 for non-remote, polluted regions), the highest values of observed, street-level UFP concentrations are systematically underestimated, whereas in rural environments close to urban areas the model generally overestimates observed UFP concentrations. As the relatively coarse global model does not resolve concentration gradients in urban centres and industrial UFP hotspots, high-resolution data of anthropogenic emissions are used to account for such differences in each model grid box, obtaining UFP concentrations with unprecedented 0.1∘×0.1∘ horizontal resolution at the Earth's surface. This observation-guided downscaling further improves the agreement with observations, leading to an increase in the logarithmic-scale correlation between observed and simulated UFP concentrations to r=0.84 in polluted environments (and 0.95 in all regions), a decrease in the root mean squared logarithmic error (from 0.57 to 0.43), and removal of discrepancies associated with air quality and population density gradients within the model grid boxes. The model results are made publicly available for studies on public health and other impacts of atmospheric UFPs, as well as for intercomparison with other regional and global models and datasets.

Exhaust particle number and composition for diesel and gasoline passenger cars under transient driving conditions: Real-world emissions down to 1.5 nm

Recent recommendations given by WHO include systematic measurements of ambient particle number concentration and black carbon (BC) concentrations. In India and several other highly polluted areas, the air quality problems are severe and the need for air quality related information is urgent. This study focuses on particle number emissions and BC emissions of passenger cars that are technologically relevant from an Indian perspective. Particle number and BC were investigated under real-world conditions for driving cycles typical for Indian urban environments. Two mobile laboratories and advanced aerosol and trace gas instrumentation were utilized. Our study shows that passenger cars without exhaust particle filtration can emit in real-world conditions large number of particles, and especially at deceleration a significant fraction of particle number can be even in 1.5–10 nm particle sizes. The mass concentration of exhaust plume particles was dominated by BC that was emitted especially at acceleration conditions. However, exhaust particles contained also organic compounds, indicating the roles of engine oil and fuel in exhaust particle formation. In general, our study was motivated by serious Indian air quality problems, by the recognized lack of emission information related to Indian traffic, and by the recent WHO air quality guidance; our results emphasize the importance of monitoring particle number concentrations and BC also in Indian urban areas and especially in traffic environments where people can be significantly exposed to fresh exhaust emissions.

Exploring the potential for continuous measurement of ultrafine particle mass concentration (PM 0.1 ) based on measurements of particle number concentration above 50 nm ( N 50 )

Exploring the potential for continuous measurement of ultrafine particle mass concentration (PM _0.1 ) based on measurements of particle number concentration above 50 nm ( <i>N</i> ₅₀ )

Effect of radiation interaction and aerosol processes on ventilation and aerosol concentrations in a real urban neighbourhood in Helsinki

Abstract. Large-eddy simulation (LES) is an optimal tool to examine aerosol particle concentrations in detail within urban neighbourhoods. The concentrations are a complex result of local emissions, meteorology, aerosol processes and local mixing conditions due to thermal and mechanical effects. Despite this, most studies have focused on simplification of the affecting processes such as examining the impact of local mixing in idealised street canyons or treating aerosols as passive scalars. The aim of this study is to include all these processes into LES using the PALM model system and to examine the importance of radiative heating and aerosol processes in simulating local aerosol particle concentrations and different aerosol metrics within a realistic urban neighbourhood in Helsinki under morning rush hour with calm wind conditions. The model outputs are evaluated against mobile laboratory measurements of air temperature and total particle number concentration (Ntot) as well as drone measurements of lung-deposited surface area (LDSA). The inclusion of radiation interaction in LES has a significant impact on simulated near-surface temperatures in our study domain, increasing them on average from 8.6 to 12.4 ∘C. The resulting enhanced ventilation reduces the pedestrian-level (4 m) Ntot by 53 %. The reduction in Ntot due to aerosol processes is smaller, only 18 %. Aerosol processes particularly impact the smallest particle range, whereas radiation interaction is more important in the larger particle range. The inclusion of radiation interaction reduces the bias between the modelled and mobile-laboratory-measured air temperatures from −3.9 to +0.2 ∘C and Ntot from +98 % to −13 %. With both aerosol and radiation interaction on, the underestimation is 16 %, which might be due to overestimation of the ventilation. The results show how inclusion of radiative interaction is particularly important in simulating PM2.5, whereas aerosol processes are more important in simulating LDSA in this calm wind situation.