Browsing by Author "Khlystov, AY"

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Open Access
A method for the in situ measurement of fine aerosol water content of ambient aerosols: The dry-ambient aerosol size spectrometer (DAASS)
(AEROSOL SCIENCE AND TECHNOLOGY, 2004) Stanier, CO; Khlystov, AY; Chan, WR; Mandiro, M; Pandis, SN
Hygroscopic growth of atmospheric particles affects a number of environmentally important aerosol properties. Due to the hysteresis exhibited by the aerosol hygroscopic growth, the physical state of particles and the amount of aerosol water are uncertain within a wide range of relative humidities (RHs) found in the troposphere, leading to uncertainties in optical and chemical properties of the aerosol. Here we report the design and tests of an automated system that was built to assess the amount of aerosol water at atmospheric conditions. The system consists of two scanning mobility particle sizers (SMPS) and an aerodynamic particle sizer (APS) that measure the aerosol size distribution between 3 nm and 10 mum in diameter. The inlets of the instruments and their sheath air lines are equipped with computer-controlled valves that direct air through Nation dryers or bypass them. The Nation dryers dehydrate the air streams to below 30\% RH at which point ambient particles are expected to lose most or all water. The switch between the dried and the ambient conditions occurs every 7 min and is synchronized with the scan times of the aerosol spectrometers. In this way the system measures alternatively dried (below 30\% RH) and ambient aerosol size distributions. A comparison of the ambient RH and the dried RH size distributions and the corresponding integrated volume concentrations provides a measure of the physical state of particles and the amount of aerosol water. The aerosol water content can be treated as a growth factor or as an absolute quantity and can be calculated as a time series or as a function of RH (humidigram). When combined with aerosol composition measurements, the DAASS can be used to compare hygroscopic growth models and measurements.
Open Access
Ambient aerosol size distributions and number concentrations measured during the Pittsburgh Air Quality Study (PAQS)
(Atmospheric Environment, 2004-06-01) Stanier, CO; Khlystov, AY; Pandis, SN
Twelve months of aerosol size distributions from 3 to 560nm, measured using scanning mobility particle sizers are presented with an emphasis on average number, surface, and volume distributions, and seasonal and diurnal variation. The measurements were made at the main sampling site of the Pittsburgh Air Quality Study from July 2001 to June 2002. These are supplemented with 5 months of size distribution data from 0.5 to 2.5μm measured with a TSI aerosol particle sizer and 2 months of size distributions measured at an upwind rural sampling site. Measurements at the main site were made continuously under both low and ambient relative humidity. The average Pittsburgh number concentration (3-500nm) is 22,000cm-3 with an average mode size of 40nm. Strong diurnal patterns in number concentrations are evident as a direct effect of the sources of particles (atmospheric nucleation, traffic, and other combustion sources). New particle formation from homogeneous nucleation is significant on 30-50% of study days and over a wide area (at least a hundred kilometers). Rural number concentrations are a factor of 2-3 lower (on average) than the urban values. Average measured distributions are different from model literature urban and rural size distributions. © 2004 Elsevier Ltd. All rights reserved.
Open Access
Nucleation events during the Pittsburgh air quality study: Description and relation to key meteorological, gas phase, and aerosol parameters
(AEROSOL SCIENCE AND TECHNOLOGY, 2004) Stanier, CO; Khlystov, AY; Pandis, SN
During the Pittsburgh Air Quality Study (PAQS) aerosol size distributions between 3 nm and 680 nm were measured between July 2001 and June 2002. These distributions have been analyzed to assess the importance of nucleation as a source of ultrafine particles in Pittsburgh and the surrounding areas. The analysis shows nucleation on 50\% of the study days and regional-scale formation of ultrafine particles on 30\% of the days. Nucleation occurred during all seasons, but it was most frequent in fall and spring and least frequent in winter. Regional nucleation was most common on sunny days with below average PM2.5 concentrations. Local nucleation events were usually associated with elevated SO2 concentrations. The observed nucleation events ranged from weak events with only a slight increase in the particle number to relatively intense events with increases of total particle counts between 50,000 cm(-3) up to 150,000 cm(-3). Averaging all days of the study, days with nucleation events had number concentrations peaking at around noon at about 45,000 cm(-3). This is compared to work days without nucleation, when the daily maximum was 8 am at 23,000 cm-3, and to weekends without nucleation, when the daily maximum was at noon at 16,000 cm(-3). Twenty-four-hour average number concentrations were approximately 40\% higher on days with nucleation compared to those without. Nucleation was typically observed starting around 9 am EST, although the start of nucleation events was later in winter and earlier in summer. The nucleation events are fairly well correlated with the product of {[}UV intensity {*} SO2 concentration] and also depend on the effective area available for condensation. This indicates that H2SO4 is a component of the new particles. Published correlations for nucleation by binary H2SO4-H2O cannot explain the observed nucleation frequency and intensity, suggesting that an additional component (perhaps ammonia) is participating in the particle formation.
Open Access
Pittsburgh air quality study overview
(Atmospheric Environment, 2004-06-01) Wittig, AE; Anderson, N; Khlystov, AY; Pandis, SN; Davidson, C; Robinson, AL
Ambient sampling for the Pittsburgh Air Quality Study (PAQS) was conducted from July 2001 to September 2002. The study was designed (1) to characterize particulate matter (PM) by examination of size, surface area, and volume distribution, chemical composition as a function of size and on a single particle basis, morphology, and temporal and spatial variability in the Pittsburgh region; (2) to quantify the impact of the various sources (transportation, power plants, biogenic sources, etc.) on the aerosol concentrations in the area; and (3) to develop and evaluate the next generation of atmospheric aerosol monitoring and modeling techniques. The PAQS objectives, study design, site descriptions and routine and intensive measurements are presented. Special study days are highlighted, including those associated with elevated concentrations of daily average PM2.5 mass. Monthly average and diurnal patterns in aerosol number concentration, and aerosol nitrate, sulfate, elemental carbon, and organic carbon concentrations, light scattering as well as gas-phase ozone, nitrogen oxides, and carbon monoxide are discussed with emphasis on the processes affecting them. Preliminary findings reveal day-to-day variability in aerosol mass and composition, but consistencies in seasonal average diurnal profiles and concentrations. For example, the seasonal average variations in the diurnal PM2.5 mass were predominately driven by the sulfate component. © 2004 Elsevier Ltd. All rights reserved.
Open Access
Positive and negative artifacts in particulate organic carbon measurements with denuded and undenuded sampler configurations
(Aerosol Science and Technology, 2004-05-01) Subramanian, R; Khlystov, AY; Cabada, JC; Robinson, AL
Measurement of ambient particulate organic carbon (POC) with quartz filters is prone to positive and negative sampling artifacts. One approach for estimating these artifacts is to sample with a backup quartz filter placed behind either the main quartz filter or a Teflon filter in a parallel line. Another approach is to use a denuder to reduce the positive artifact in combination with a highly adsorbent backup filter to capture any negative artifact. Results obtained using both of these approaches in parallel for over one year in Pittsburgh, PA are presented in this article. A sampler using an activated carbon monolith denuder has been developed and tested extensively. Transmission losses were found to be negligible, and the denuder is on average 94% efficient at removing gas-phase organics. Denuder breakthrough is corrected for each run using a dynamic blank in parallel with the sample line. Comparisons with the dynamic blank indicate that the denuder almost eliminates the positive artifact on the quartz filter. Negative artifact from the denuded quartz filter is quantified using a carbon-impregnated glass fiber (CIG) backup filter and was found to be small, typically less than 10% of the ambient POC. Compared to the denuded sampler POC, 24 h bare quartz samples showed an almost constant positive artifact of 0.5 μg-C/m3 for samples taken throughout the year-long study period. Sampling for shorter durations (4-6 h) resulted in a larger positive artifact. A quartz filter behind a Teflon filter (QBT) provides a consistent estimate of the positive artifact on the bare quartz filter irrespective of sample duration, though it overcorrects for the positive artifact by 16-20% (attributed to particulate matter volatilizing off the upstream Teflon filter). The quartz behind quartz (QBQ) approach provides a reasonable estimate of the positive artifact on the bare quartz filter for the 24 h samples but not for the shorter samples. A slight seasonal variation is observed in the absolute value of the positive artifact, with higher values observed during the summer months.
Open Access
Semi-continuous PM2.5 inorganic composition measurements during the Pittsburgh Air Quality Study
(Atmospheric Environment, 2004-06-01) Wittig, AE; Takahama, S; Khlystov, AY; Pandis, SN; Hering, S; Kirby, B; Davidson, C
A method for semi-continuous (10min time resolution) PM2.5 nitrate and sulfate measurements, based on the humidified impaction with flash volatilization design of Stolzenburg and Hering (Environ. Sci. Technol. 34 (2000) 907), was evaluated during the Pittsburgh Air Quality Study (PAQS) from July 2001 to August 2002. The semi-continuous measurements were corrected for several operating parameters. The overall corrections were less than 10% on average, but could be quite large for individual 10min measurements. These corrections resulted in an improvement in the agreement of the measurements with the filter-based measurements, with a major axis regression relationship of y=0.83x+0.20μgm-3 and R2 of 0.84 for nitrate and y=0.71x+0.42μgm-3 and R2 of 0.83 for sulfate. The corrected semi-continuous measurements were calibrated over the entire year using collocated denuder/filter-pack-based measurements. These calibrated semi-continuous measurements are used in conjunction with temporally resolved gas-phase measurements of total (gas- and aerosol-phase) nitrate and meteorological measurements to investigate short-term phenomena at the Pittsburgh Supersite. The gas-to-particle partitioning of nitrate varied daily and seasonally, with a majority of the nitrate in the particle phase at night and during the winter months. © 2004 Elsevier Ltd. All rights reserved.
Open Access
Variability of particulate matter concentrations along roads and motorways determined by a moving measurement unit
(Atmospheric Environment, 2004-06-01) Weijers, EP; Khlystov, AY; Kos, GPA; Erisman, JW
The spatial variability of aerosol number and mass along roads was determined in different regions (urban, rural and coastal-marine) of the Netherlands. A condensation particle counter (CPC) and an optical aerosol spectrometer (LAS-X) were installed in a van along with a global positioning system (GPS). Concentrations were measured with high-time resolutions while driving allowing investigations not possible with stationary equipment. In particular, this approach proves to be useful to identify those locations where numbers and mass attain high levels ('hot spots'). In general, concentrations of number and mass of particulate matter increase along with the degree of urbanisation, with number concentration being the more sensitive indicator. The lowest particle numbers and PM1-concentrations are encountered in a coastal and rural area: <5000cm-3 and 6μgm-3, respectively. The presence of sea-salt material along the North-Sea coast enhances PM>1-concentrations compared to inland levels. High-particle numbers are encountered on motorways correlating with traffic intensity; the largest average number concentration is measured on the ring motorway around Amsterdam: about 160000cm-3 (traffic intensity 100000vehday-1). Peak values occur in tunnels where numbers exceed 106cm-3. Enhanced PM1 levels (i.e. larger than 9μgm-3) exist on motorways, major traffic roads and in tunnels. The concentrations of PM>1 appear rather uniformly distributed (below 6μgm-3 for most observations). On the urban scale, (large) spatial variations in concentration can be explained by varying intensities of traffic and driving patterns. The highest particle numbers are measured while being in traffic congestions or when behind a heavy diesel-driven vehicle (up to 600×103cm-3). Relatively high numbers are observed during the passages of crossings and, at a decreasing rate, on main roads with much traffic, quiet streets and residential areas with limited traffic. The number concentration exhibits a larger variability than mass: the mass concentration on city roads with much traffic is 12% higher than in a residential area at the edge of the same city while the number of particles changes by a factor of two (due to the presence of the ultrafine particles (aerodynamic diameter <100nm). It is further indicated that people residing at some 100m downwind a major traffic source are exposed to (still) 40% more particles than those living in the urban background areas. © 2004 Elsevier Ltd. All rights reserved.