Hygroscopicity and cloud condensation nucleus (CCN) activity were measured for three mineral dust samples: one from the Canary Islands, representing North African dust transported across the ...Atlantic; one from outside Cairo, representing North African dust transported to the eastern Mediterranean; and Arizona Test Dust, representing dust in the southwestern United States. To reaerosolize bulk samples, dust samples were either suspended in high purity water and particles generated by atomization, or samples were resuspended in dry air using a fluidized bed. Only the Canary Island sample generated from aqueous suspension showed appreciable hygroscopic growth at subsaturated conditions; all other samples exhibited diameter growth factors of less than 1.1 for relative humidities ≤90%. Despite their low hygroscopicities at subsaturated conditions, all samples activated as cloud droplets at supersaturations lower than required for insoluble particles. We suggest that the CCN activity of these mineral dusts are well‐represented using the hygroscopicity parameter 0.01 ≤ κ ≤ 0.08.
During the Fire Laboratory at Missoula Experiments (FLAME), we studied the physical, chemical, and optical properties of biomass burning smoke from the laboratory combustion of various wildland ...fuels. A good understanding of these properties is important in determining the radiative effects of biomass burning aerosols, with impacts on both local and regional visibility and global climate. We measured aerosol size distributions with two instruments: a differential mobility particle sizer (DMPS) and an optical particle counter (OPC). Volume size distributions from different burns varied from monomodal to multimodal, with geometric mean diameters ranging from 0.20–0.57 μm and geometric standard deviations ranging from 1.68–2.97. By reconciling the differences between the two sizing instruments, we estimated aerosol effective refractive indices with values ranging from 1.41 to 1.61. We reconstructed aerosol chemical composition for each burn using data from filters collected and analyzed with the Interagency Monitoring of Protected Visual Environments (IMPROVE) samplers and protocols. Aerosols were generally comprised of carbon with organic species accounting for the largest mass fraction in most cases. We used composition data to calculate aerosol density, which ranged from 1.22–1.92 g cm−3, and real and imaginary refractive indices, which had ranges of 1.55–1.80 and 0.01–0.50 respectively. Aerosol physical, chemical, and optical characterizations were combined to calculate dry mass scattering (MSE) and absorption (MAE) efficiencies at 532 nm. These parameters had values between 1.6–5.7 m2 g−1 and 0.04–0.94 m2 g−1.
We analyzed the association between substance use (SU) and condomless sex (CS) among HIV-negative adults reporting heterosexual sex in the Seek, Test, Treat, and Retain (STTR) consortium. We describe ...the impact of SU as well as person/partner and context-related factors on CS, identifying combinations of factors that indicate the highest likelihood of CS.
We analyzed data from four US-based STTR studies to examine the effect of SU on CS using two SU exposures: 1) recent SU (within 3 months) and 2) SU before/during sex. Behavioral data were collected via 1:1 or self-administered computerized interviews. Adjusted individual-study, multivariable relative risk regression was used to examine the relationship between CS and SU. We also examined interactions with type of sex and partner HIV status. Pooled effect estimates were calculated using traditional fixed-effects meta-analysis. We analyzed data for recent SU (n = 6781; 82% men, median age = 33 years) and SU before/during sex (n = 2915; 69% men, median age = 40 years).
For both exposure classifications, any SU other than cannabis increased the likelihood of CS relative to non-SU (8-16%, p-values< 0.001). In the recent SU group, however, polysubstance use did not increase the likelihood of CS compared to single-substance use. Cannabis use did not increase the likelihood of CS, regardless of frequency of use. Type of sex was associated with CS; those reporting vaginal and anal sex had a higher likelihood of CS compared to vaginal sex only for both exposure classifications (18-21%, p < 0.001). Recent SU increased likelihood of CS among those reporting vaginal sex only (9-10%, p < 0.001); results were similar for those reporting vaginal and anal sex (5-8%, p < 0.01). SU before/during sex increased the likelihood of CS among those reporting vaginal sex only (20%; p < 0.001) and among those reporting vaginal and anal sex (7%; p = 0.002). Single- and poly-SU before/during sex increased the likelihood of CS for those with exclusively HIV-negative partners (7-8%, p ≤ 0.02), and for those reporting HIV-negative and HIV-status unknown partners (9-13%, p ≤ 0.03).
Except for cannabis, any SU increased the likelihood of CS. CS was associated with having perceived HIV-negative partners and with having had both anal/vaginal sex.
Celotno besedilo
Dostopno za:
DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Nitrogen deposition to the sensitive ecosystems in Rocky Mountain National Park (RMNP) has been increasing. Ammonia has been shown to be a large fraction of this nitrogen deposition, and sources in ...northeastern Colorado were found to be a significant contributor. In this work we report on the results from a small network of Radiello passive samplers to investigate the temporal and spatial variability of ammonia gas concentrations in northeastern Colorado. A URG denuder/filter-pack sampler was collocated with a Radiello passive sampler to provide a check on the accuracy of passive ammonia measurements and to provide information about complementary aerosol and trace gas species. These measurements showed seasonal variations in the concentrations of both particulate- and gas-phase aerosol components. The highest concentrations of ammonia occurred during summer months. These were almost twice the lowest concentrations, which occurred during spring and fall months. Ammonia also exhibited higher than expected concentrations during winter. There was considerable spatial variability in average ammonia concentrations, with May–August averages ranging from 3 μg m−3 in rural grasslands to 4–11 μg m−3 at suburban-urban sites to almost 30 μg m−3 in an area of intensive livestock feeding and farming operations. The large ammonia gradients near sources are expected for this primary pollutant with high deposition rates. The overall concentrations in this region are significantly larger than those measured in RMNP, which were around 0.5 μg m−3, and represent a large reservoir of ammonia that can be transported to RMNP with easterly winds.
► Ammonia from the plains of Colorado contributes to N deposition in RMNP. ► Ammonia and other inorganic aerosol species show seasonal variability. ► Ammonia concentrations exhibit large spatial variability.
Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the ...laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients revealed a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: (1) shielding of inner monomers after particle consolidation or collapse with water uptake; (2) the lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH) to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.
Secondary Organic Aerosols (SOA) studied in previous laboratory experiments generally showed only slight hygroscopic growth, but a much better activity as a CCN (Cloud Condensation Nucleus) than ...indicated by the hygroscopic growth. This discrepancy was examined at LACIS (Leipzig Aerosol Cloud Interaction Simulator), using a portable generator that produced SOA particles from the ozonolysis of α-pinene, and adding butanol or butanol and water vapor during some of the experiments. The light scattering signal of dry SOA-particles was measured by the LACIS optical particle spectrometer and was used to derive a refractive index for SOA of 1.45. LACIS also measured the hygroscopic growth of SOA particles up to 99.6% relative humidity (RH), and a CCN counter was used to measure the particle activation. SOA-particles were CCN active with critical diameters of e.g. 100 nm and 55 nm at super-saturations of 0.4% and 1.1%, respectively. But only slight hygroscopic growth with hygroscopic growth factors ≤1.05 was observed at RH<98% RH. At RH>98%, the hygroscopic growth increased stronger than would be expected if a constant hygroscopicity parameter for the particle/droplet solution was assumed. An increase of the hygroscopicity parameter by a factor of 4–6 was observed in the RH-range from below 90% to 99.6%, and this increase continued for increasingly diluted particle solutions for activating particles. This explains an observation already made in the past: that the relation between critical super-saturation and dry diameter for activation is steeper than what would be expected for a constant value of the hygroscopicity. Combining measurements of hygroscopic growth and activation, it was found that the surface tension that has to be assumed to interpret the measurements consistently is greater than 55 mN/m, possibly close to that of pure water, depending on the different SOA-types produced, and therefore only in part accounts for the discrepancy between hygroscopic growth and CCN activity observed for SOA particles in the past.
The Ron Brown cruise during ACE‐Asia (March–April 2001) encountered complex aerosol that at times was dominated by marine, polluted, volcanic, and dust aerosols. Average total light scattering ...coefficients (σsp for Dp <10 μm, relative humidity (RH) = 19%, and λ = 550 nm) ranged from 23 (marine) to 181 Mm−1 (dust). Aerosol hygroscopicity ranged from deliquescent with hysteresis (marine frequently and polluted variably) to hygroscopic without hysteresis (volcanic) to nearly hygrophobic (dust‐dominated). Average deliquescence and crystallization RH were 77 ± 2% and 42 ± 3%, respectively. The ambient aerosol was typically on the upper branch of the hysteresis loop for marine and polluted air masses and the lower branch for dust‐dominated aerosols. Average f(RH = ambient), defined as σsp (RH = ambient)/σsp (RH = 19%), ranged from 1.25 (dust) to 2.88 (volcanic). Average h(RH ∼60%), defined as f(RH)upper branch/f(RH)lower branch, were 1.6, 1.3, 1, and 1.25 for marine, polluted, volcanic, and dust, demonstrating an importance of hysteresis to optical properties. Hemispheric backscatter fraction (b) at ambient RH ranged from 0.077 (marine) to 0.111 (dust), while single scattering albedo (ω) at ambient RH ranged from 0.94 (dust and polluted) to 0.99 (marine).
We examine the observed relationships between molar volume (the ratio of molar mass and density) and cloud condensation nuclei (CCN) activity for sufficiently soluble organic compounds found in ...atmospheric particulate matter. Our data compilation includes new CCN data for certain carbohydrates and oligoethylene glycols, as well as published data for organic compounds. We compare predictions of CCN activity using water activities based on Raoult's law and Flory‐Huggins theory to observations. The Flory‐Huggins water activity expression, with an assumed surface tension of pure water, generally predicts CCN activity within a factor of two over the full range of molar volumes considered. CCN activity is only weakly dependent on molar volume for values exceeding 600 cm3 mol−1, and the diminishing sensitivity to molar volume, combined with the significant scatter in the data, limits the accuracy with which molar volume can be inferred from CCN measurements.
As part of the Fire Lab at Missoula Experiments (FLAME) in 2006–2007, we examined hygroscopic properties of particles emitted from open combustion of 33 select biomass fuels. Measurements of ...humidification growth factors for subsaturated water relative humidity (RH) conditions were made with a hygroscopic tandem differential mobility analyzer (HTDMA) for dry particle sizes of 50, 100 and 250 nm. Results were then fit to a single-parameter model to obtain the hygroscopicity parameter, κ. Particles in freshly emitted biomass smoke exhibited a wide range of hygroscopicity (individual modes with 0
Ice‐nucleating particles (INPs) are required for initial ice crystal formation in clouds at temperatures warmer than about −36°C and thus play a crucial role in cloud and precipitation formation. ...Biomass burning has been found to be a source of INPs in previous studies and is also a major contributor to atmospheric black carbon (BC) concentrations. This study focuses on isolating the BC contribution to the INP population associated with biomass combustion. Emissions of condensation mode INPs from a number of globally relevant biomass fuels were measured at −30°C and above water saturation as fires progressed from ignition to extinguishment in a laboratory setting. Number emissions of INPs were found to be highest during intense flaming combustion (modified combustion efficiency > 0.95). Overall, combustion emissions from 13 of 22 different biomass fuel types produced measurable INP concentrations for at least one replicate experiment. On average, all burns that produced measureable INPs had higher combustion efficiency, which is associated with higher BC emissions, than those that did not produce measureable INPs. Across all burns that produced measureable INPs, concentrations ranged from 0.1 to 10 cm−3, and the median emission factor was about 2 × 107 INPs per kilogram of fuel burned. For a subset of the burns, the contribution of refractory black carbon (rBC) to INP concentrations was determined by removing rBC via laser‐induced incandescence. Reductions in INPs of 0–70% were observed, indicating an important contribution of rBC particles to INP concentrations for some burns, especially marsh grasses.
Key Points
Fires emit ice‐nucleating particles
Black carbon contributes to the INPs emitted from fires
Fire emissions have lower ice‐nucleating efficiency than other sources
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