Cloud condensation nuclei activity of internally mixed particle populations at a remote marine free troposphere site in the North Atlantic Ocean.

This study reports results from research conducted at the Observatory of Mount Pico (OMP), 2225 m above mean sea level on Pico Island in the Azores archipelago in June and July 2017. We investigated the chemical composition, mixing state, and cloud condensation nuclei (CCN) activities of long-range transported free tropospheric (FT) particles. FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) simulations reveal that most air masses that arrived at the OMP during the sampling period originated in North America and were highly aged (average plume age > 10 days). We probed size-resolved chemical composition, mixing state, and hygroscopicity parameter (κ) of individual particles using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX). Based on the estimated individual particle mass from elemental composition, we calculated the mixing state index, χ. During our study, FT particle populations were internally mixed (χ of samples are between 53 % and 87 %), owing to the long atmospheric aging time. We used data from a miniature Cloud Condensation Nucleus Counter (miniCCNC) to derive the hygroscopicity parameter, κCCNC. Combining κCCNC and FLEXPART, we found that air masses recirculated above the North Atlantic Ocean with lower mean altitude had higher κCCNC due to the higher contribution of sea salt particles. We used CCSEM-EDX and phase state measurements to predict single-particle κ (κCCSEM-EDX) values, which overlap with the lower range of κCCNC measured below 0.15 % SS. Therefore, CCSEM-EDX measurements can be useful in predicting the lower bound of κ, which can be used in climate models to predict CCN activities, especially in remote locations where online CCN measurements are unavailable.

Profile observations of the Arctic atmospheric boundary layer with the BELUGA tethered balloon during MOSAiC.

During the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition, the Balloon-bornE moduLar Utility for profilinG the lower Atmosphere (BELUGA) was deployed from an ice floe drifting in the Fram Strait from 29 June to 27 July 2020. The BELUGA observations aimed to characterize the cloudy Arctic atmospheric boundary layer above the sea ice using a modular setup of five instrument packages. The in situ measurements included atmospheric thermodynamic and dynamic state parameters (air temperature, humidity, pressure, and three-dimensional wind), broadband solar and terrestrial irradiance, aerosol particle microphysical properties, and cloud particle images. In total, 66 profile observations were collected during 33 balloon flights from the surface to maximum altitudes of 0.3 to 1.5 km. The profiles feature a high vertical resolution of 0.01 m to 1 m, including measurements below, inside, and above frequently occurring low-level clouds. This publication describes the balloon operations, instruments, and the obtained data set. We invite the scientific community for joint analysis and model application of the freely available data on PANGAEA.

Particle number emission rates of aerosol sources in 40 German households and their contributions to ultrafine and fine particle exposure.

More representative data on source-specific particle number emission rates and associated exposure in European households are needed. In this study, indoor and outdoor particle number size distributions (10-800 nm) were measured in 40 German households under real-use conditions in over 500 days. Particle number emission rates were derived for around 800 reported indoor source events. The highest emission rate was caused by burning candles (5.3 × 1013  h-1 ). Data were analyzed by the single-parameter approach (SPA) and the indoor aerosol dynamics model approach (IAM). Due to the consideration of particle deposition, coagulation, and time-dependent ventilation rates, the emission rates of the IAM approach were about twice as high as those of the SPA. Correction factors are proposed to convert the emission rates obtained from the SPA approach into more realistic values. Overall, indoor sources contributed ~ 56% of the daily-integrated particle number exposure in households under study. Burning candles and opening the window leads to seasonal differences in the contributions of indoor sources to residential exposure (70% and 40% in the cold and warm season, respectively). Application of the IAM approach allowed to attribute the contributions of outdoor particles to the penetration through building shell and entry through open windows (26% and 15%, respectively).

Size-fractioned particulate air pollution and cardiovascular emergency room visits in Beijing, China.

BACKGROUND: Although short-term exposure to ambient particulate matter has increasingly been linked with cardiovascular diseases, it is not quite clear how physical characteristics of particles, such as particle size may be responsible for the association. This study aimed at investigating whether daily changes in number or mass concentrations of accurately size-segregated particles in the range of 3nm-10µm are associated with daily cardiovascular emergency room visits in Beijing, China. METHODS: Cardiovascular emergency room visit counts, particle size distribution data, and meteorological data were collected from Mar. 2004 to Dec. 2006. Particle size distribution data was used to calculate particle number concentration in different size fractions, which were then converted to particle mass concentration assuming spherical particles. We applied a time-series analysis approach. We evaluated lagged associations between cardiovascular emergency room visits and particulate number and mass concentration using distributed lag non-linear models up to lag 10. We calculated percentage changes of cardiovascular emergency room visits, together with 95% confidence intervals (CI), in association with an interquartile range (IQR, difference between the third and first quartile) increase of 11-day or 2-day moving average number or mass concentration of particulate matter within each size fraction, assuming linear effects. We put interaction terms between season and 11-day or 2-day average particulate concentration in the models to estimate the modification of the particle effects by season. RESULTS: We observed delayed associations between number concentration of ultrafine particles and cardiovascular emergency room visits, mainly from lag 4 to lag 10, mostly contributed by 10-30nm and 30-50nm particles. An IQR (9040cm(-3)) increase in 11-day average number concentration of ultrafine particles was associated with a 7.2% (1.1-13.7%) increase in total, and a 7.9% (0.5-15.9%) increase in severe cardiovascular emergency room visits. The delayed effects of particulate mass concentration were small. Regarding immediate effects, 2-day average number concentration of Aitken mode (30-100nm) particles had strongest effects. An IQR (2269cm(-3)) increase in 2-day average number concentration of 30-50nm particles led to a 2.4% (-1.5-6.5%) increase in total, and a 1.7% (-2.9-6.5%) increase in severe cardiovascular emergency room visits. The immediate effects of mass concentration came mainly from 1000-2500nm particles. An IQR (11.7µgm(-3)) increase in 2-day average mass concentration of 1000-2500nm particles led to an around 2.4% (0.4-4.4%) increase in total, and a 1.7% (-0.8-4.2%) increase in severe cardiovascular emergency room visits. The lagged effect curves of number and mass concentrations of 100-300nm particles or 300-1000nm particles were quite similar, indicating that using particulate number or mass concentrations seemed not to affect the cardiovascular effect (of particles within one size fraction). The effects of number concentration of ultrafine particles, sub-micrometer particles (3-1000nm) and 10-30nm particles were substantially higher in winter comparing with in summer. CONCLUSIONS: Elevated concentration levels of sub-micrometer particles were associated with increased cardiovascular morbidity. Ultrafine particles showed delayed effects, while accumulation mode (100-1000nm) particles showed immediate effects. Using number or mass concentrations did not affect the particle effects.

Associations between size-segregated particle number concentrations and respiratory mortality in Beijing, China.

Numerous studies have described the adverse associations between particle mass and respiratory health. The aim of the study was to analyze the associations of particle properties, especially size-segregated particle number concentrations (PNC), and respiratory mortality in Beijing, P.R. China. We gathered daily values of respiratory mortality and air pollution data of the Beijing urban area. Generalized additive models were used to estimate the associations. Single pollutant models showed that delayed concentrations of SO(2), total PNCs, and PNC of 300-1000 nm were adversely associated with total respiratory mortality. There was an indication that adverse health effects of PNCs might be stronger for stagnant air masses. Two-pollutant models verified the independence of associations of total PNCs of other pollutants (SO(2), NO(2), and PM(10)). In conclusion, particle number concentrations, especially accumulation mode particles, might be factors influencing the adverse associations between particulate matter and respiratory health.

Sub-micrometer particulate air pollution and cardiovascular mortality in Beijing, China.

BACKGROUND: While the link between particulate matter and cardiovascular mortality is well established, it is not fully investigated and understood which properties of the aerosol might be responsible for the health effects, especially in polluted mega-city areas. OBJECTIVES: Our goal was to explore the association between daily cardiovascular mortality and different particle metrics in the sub-micrometer range in Beijing, China. METHODS: We obtained daily counts of cause-specific cardiovascular deaths in the Beijing urban area for the period March 2004 to August 2005. Concurrently, continuous measurements of particle number size distributions were performed. Particle number concentrations (NC) between 0.003 µm and 0.8 µm were converted to particle mass and surface area concentrations assuming spherical particles. Semi-parametric Poisson regression models adjusting for trend, seasonality, day of the week, and meteorology were used to estimate immediate, delayed and cumulative particle effects. Additionally, effect modification by air mass origin was investigated. RESULTS: We observed associations between daily cardiovascular mortality and particle NC for a 2-days delay. Moreover, nearly all particle metrics showed 2-days delayed associations with ischemic heart disease mortality. The strongest association was found for particle NC in the size range 0.03-0.1 µm (7.1% increase in daily mortality with a 95%-confidence interval of 2.9%-11.5%, per an increase of 6250 particles/cm3). Results for surface and mass concentrations with a lag of two days indicated effect modification by air mass origin, whereas effects of particle NC were not modified. CONCLUSIONS: Results show an elevated risk of cardiovascular mortality in Beijing from short-term exposure to particulate air pollution in the sub-micrometer range. Results also indicate that locally produced smaller particles and regionally transported particles may exhibit different effects in Beijing.

The effect of particle size on cardiovascular disorders--the smaller the worse.

BACKGROUND: Previous studies observed associations between airborne particles and cardio-vascular disease. Questions, however, remain as to which size of the inhalable particles (coarse, fine, or ultrafine) exerts the most significant impact on health. METHODS: For this retrospective study, data of the total number of 23,741 emergency service calls, registered between February 2002 and January 2003 in the City of Leipzig, were analysed, identifying 5326 as being related to cardiovascular incidences. Simultaneous particle exposure was determined for the particle sizes classes <100 nm (UFP), <2.5 µm (PM2.5) and <10 µm (PM10). We used a time resolution of 1 day for both parameters, emergency calls and exposure. RESULTS: Within the group of cardiovascular diseases, the diagnostic category of hypertensive crisis showed a significant association with particle exposure. The significant effect on hypertensive crisis was found for particles with a size of <100 nm in diameter and starting with a lag of 2 days after exposure. No consistent influence could be observed for PM2.5 and PM10. The Odds Ratios on hypertensive crisis were significant for the particle size <100 nm in diameter from day 2 post exposure OR=1.06 (95%CI: 1.02-1.10, p=0.002) up to day 7 OR=1.05 (95%CI 1.02-1.09, p=0.005). CONCLUSION: Ultrafine particles affect cardiovascular disease adversely, particularly hypertensive crises. Their effect is significant compared with PM2.5 and PM10. It appears necessary, from a public health point of view, to consider regulating this type of particles using appropriate measurands as particle number.

Volatile nanoparticle formation and growth within a diluting diesel car exhaust.

A major source of particle number emissions is road traffic. However, scientific knowledge concerning secondary particle formation and growth of ultrafine particles within vehicle exhaust plumes is still very limited. Volatile nanoparticle formation and subsequent growth conditions were analyzed here to gain a better understanding of "real-world" dilution conditions. Coupled computational fluid dynamics and aerosol microphysics models together with measured size distributions within the exhaust plume of a diesel car were used. The impact of soot particles on nucleation, acting as a condensational sink, and the possible role of low-volatile organic components in growth were assessed. A prescribed reduction of soot particle emissions by 2 orders of magnitude (to capture the effect of a diesel particle filter) resulted in concentrations of nucleation-mode particles within the exhaust plume that were approximately 1 order of magnitude larger. Simulations for simplified sulfuric acid-water vapor gas-oil containing nucleation-mode particles show that the largest particle growth is located in a recirculation zone in the wake of the car. Growth of particles within the vehicle exhaust plume up to detectable size depends crucially on the relationship between the mass rate of gaseous precursor emissions and rapid dilution. Chassis dynamometer measurements indicate that emissions of possible hydrocarbon precursors are significantly enhanced under high engine load conditions and high engine speed. On the basis of results obtained for a diesel passenger car, the contributions from light diesel vehicles to the observed abundance of measured nucleation-mode particles near busy roads might be attributable to the impact of two different time scales: (1) a short one within the plume, marked by sufficient precursor emissions and rapid dilution; and (2) a second and comparatively long time scale resulting from the mix of different precursor sources and the impact of atmospheric chemistry.

Size-segregated particle number concentrations and respiratory emergency room visits in Beijing, China.

BACKGROUND: The link between concentrations of particulate matter (PM) and respiratory morbidity has been investigated in numerous studies. OBJECTIVES: The aim of this study was to analyze the role of different particle size fractions with respect to respiratory health in Beijing, China. METHODS: Data on particle size distributions from 3 nm to 1 µm; PM10 (PM ≤ 10 µm), nitrogen dioxide (NO(2)), and sulfur dioxide concentrations; and meteorologic variables were collected daily from March 2004 to December 2006. Concurrently, daily counts of emergency room visits (ERV) for respiratory diseases were obtained from the Peking University Third Hospital. We estimated pollutant effects in single- and two-pollutant generalized additive models, controlling for meteorologic and other time-varying covariates. Time-delayed associations were estimated using polynomial distributed lag, cumulative effects, and single lag models. RESULTS: Associations of respiratory ERV with NO(2) concentrations and 100-1,000 nm particle number or surface area concentrations were of similar magnitude-that is, approximately 5% increase in respiratory ERV with an interquartile range increase in air pollution concentration. In general, particles < 50 nm were not positively associated with ERV, whereas particles 50-100 nm were adversely associated with respiratory ERV, both being fractions of ultrafine particles. Effect estimates from two-pollutant models were most consistent for NO(2). CONCLUSIONS: Present levels of air pollution in Beijing were adversely associated with respiratory ERV. NO(2) concentrations seemed to be a better surrogate for evaluating overall respiratory health effects of ambient air pollution than PM(10) or particle number concentrations in Beijing.

Weak correlation of ultrafine aerosol particle concentrations <800 nm between two sites within one city.

Ambient aerosol has been identified as a major pollutant affecting human health. Standards to reduce particles mass concentrations have therefore been established in many countries. Recent studies suggest that the number concentration of aerosol particles, which is dominated by the ultrafine size range smaller than 100 nm in diameter, may be independently associated with health effects. Currently, epidemiological evidence for such effects is conflicting. We have measured aerosol size distributions at two stations (urban background, street canyon) located at a distance of 1.5 km for a time period of 1 year. Number concentrations and particle size distributions at both sites were significantly different. Short-term correlation between the two sites was weak for individual measurements of number concentrations and size bins of ultrafine particles (0.19-0.46). Correlation coefficients for hourly and daily averages in selected size ranges ranged from 0.35 to 0.46. On the other hand, the correlation coefficient for daily average particle volume concentrations was found to be 0.67. About 10% to 20% of the population of European cities lives close to roads with traffic densities comparable to our site. The underestimation of the exposure of a considerable part of a study population may therefore severely influence the outcome of epidemiological studies focused on health effects associated with ultrafine particles. A single background measurement site may not be sufficient for exposure assessment in these studies without taking spatial and temporal variability into account.

[Effects of high temperature, high relative humidity and rain process on particle size distributions in the summer of Beijing].

On-line measurements of particle number size distribution were conducted during 2004-07-13 - 2004-08-23 by using TDMPS-APS system in Beijing; in between the size distributions of particle mass and chemical compositions were measured by using MOUDI cascade impactor under three kinds of weather conditions: (1) high temperature and high relative humidity night, (2) high temperature and high relative humidity day, and (3) clear days. The results indicate that particulate matter, especially fine particle pollution becomes severe under high temperature and high relative humidity conditions, which results in low visibility (2.5km); the average concentrations of PM1.8 and PM10 are 170.68 microg/m3 and 249.35 microg/m3, respectively, PM1.8 accounts for 68% of PM10; number concentration mainly concentrates in the range of 50 - 100nm, about 2 x 10(4) - 3 x 10(4)cm(-3); rain process has a great effect on scavenging particles, especially fine particles. After the rain process PM10 is 3 times lower and PM1.8 is 6 times lower than the values before the rain; in the following clear day, new particle formation is observed, the newly formed particles (3 - 20nm) grow to 50 - 100nm rapidly. After that, the pollutants start to accumulate and it becomes heavy polluted in few days.