Size distribution measurements of wildfire smoke-influences aerosol at Yosemite National Park

Dec 2004.Includes bibliographical references.Sponsored by National Park Service H2380040002 to 04-56

Influences on the fraction of hydrophobic and hydrophilic black carbon in the atmosphere

Black carbon (BC) is a short term climate forcer that directly warms the atmosphere, slows convection, and hinders quantification of the effect of greenhouse gases on climate change. The atmospheric lifetime of BC particles with respect to nucleation scavenging in clouds is controlled by their ability to serve as cloud condensation nuclei (CCN). To serve as CCN under typical conditions, hydrophobic BC particles must acquire hygroscopic coatings. However, the quantitative relationship between coatings and hygroscopic properties for ambient BC particles is not known nor is the time scale for hydrophobic-to-hydrophilic conversion. Here we introduce a method for measuring the hygroscopicity of externally and internally mixed BC particles by coupling a single particle soot photometer with a humidified tandem differential mobility analyzer. We test this technique using uncoated and coated laboratory generated model BC compounds and apply it to characterize the hygroscopicity distribution of ambient BC particles. From these data we derive that the observed number fraction of BC that is CCN active at 0.2% supersaturation is generally low in an urban area near sources and that it varies with the trajectory of the airmass. We anticipate that our method can be combined with measures of air parcel physical and photochemical age to provide the first quantitative estimates for characterizing hydrophobic-to-hydrophilic conversion rates in the atmosphere.Peer reviewe

Aerosol Mass and Optical Properties, Smoke Influence on O\u3csub\u3e3\u3c/sub\u3e, and High NO\u3csub\u3e3\u3c/sub\u3e Production Rates in a Western U.S. City Impacted by Wildfires

Evaluating our understanding of smoke from wild and prescribed fires can benefit from downwind measurements that include inert tracers to test production and transport and reactive species to test chemical mechanisms. We characterized smoke from fires in coniferous forest fuels for \u3e1,000 hr over two summers (2017 and 2018) at our Missoula, Montana, surface station and found a narrow range for key properties. ΔPM2.5/ΔCO was 0.1070 ± 0.0278 (g/g) or about half the age-independent ratios obtained at free troposphere elevations (0.2348 ± 0.0326). The average absorption Ångström exponent across both years was 1.84 ± 0.18, or about half the values available for very fresh smoke. Brown carbon (BrC) was persistent (~50% of absorption at 401 nm) in both years, despite differences in smoke age. ΔBC/ΔCO doubled from 2017 to 2018, but the average across 2 years was within 33% of recent airborne measurements, suggesting low sampling bias among platforms. Switching from a 1.0 to a 2.5 micron cutoff increased the mass scattering and mass absorption coefficients, suggesting often overlooked supermicron particles impact the optical properties of moderately aged smoke. O3 was elevated ~6 ppb on average over a full diurnal period when wildfire smoke was present, and smoke-associated O3 increases were highest (~9 pbb) at night, suggesting substantial upwind production. NOx was mostly local in origin. NOx spurred high rates of NO3 production, including in the presence of wildfire smoke (up to 2.44 ppb hr−1) and at least one nighttime BrC secondary formation event that could have impacted next-day photochemistry

The interaction of frictional slip and adhesion for a stiff sphere on a compliant substrate

How friction affects adhesion is addressed. The problem is considered in the context of a very stiff sphere adhering to a compliant, isotropic, linear elastic substrate, and experiencing adhesion and frictional slip relative to each other. The adhesion is considered to be driven by very large attractive tractions between the sphere and the substrate that can act only at very small distances between them. As a consequence, the adhesion behavior can be represented by the Johnson-Kendall-Roberts model, and this is assumed to prevail also when frictional slip is occurring. Frictional slip is considered to be resisted by a uniform, constant shear traction at the slipping interface, a model that is considered to be valid for small asperities and for compliant elastomers in contact with stiff material. A model for the interaction of friction and adhesion, known to agree with some experimental data, is utilized. This model is due to Johnson, and its adhesion-friction interaction is assumed to stem, upon shrinkage of the contact area, from a postulated reversible energy release associated with frictional slip. This behavior is considered to arise from surface microstructures generated or eliminated by frictional slip, where these microstructures store some elastic strain energy in a reversible manner. The associated reversible energy release rate is derived from the energy exchanges that occur in the system. The Johnson model, and an asymptotic analysis of it for small amounts of frictional slip, is shown to be consistent with the reversible energy release rate that we identify.Comment: 11 page

In situ measurements of trace gases, PM, and aerosol optical properties during the 2017 NW US wildfire smoke event

In mid-August through mid-September of 2017 a major wildfire smoke and haze episode strongly impacted most of the NW US and SW Canada. During this period our ground-based site in Missoula, Montana, experienced heavy smoke impacts for ∼ 500h (up to 471μ-3 hourly average PM2.5). We measured wildfire trace gases, PM2.5 (particulate matter ≤2.5μm in diameter), and black carbon and submicron aerosol scattering and absorption at 870 and 401nm. This may be the most extensive real-time data for these wildfire smoke properties to date. Our range of trace gas ratios for δNH3 δCO and δC2H4 δCO confirmed that the smoke from mixed, multiple sources varied in age from ∼ 2-3h to ∼ 1-2 days. Our study-average δCH4 δCO ratio (0.166±0.088) indicated a large contribution to the regional burden from inefficient smoldering combustion. Our δBC δCO ratio (0.0012±0.0005) for our ground site was moderately lower than observed in aircraft studies (∼ 0.0015) to date, also consistent with a relatively larger contribution from smoldering combustion. Our δBC δPM2.5 ratio (0.0095±0.0003) was consistent with the overwhelmingly non-BC (black carbon), mostly organic nature of the smoke observed in airborne studies of wildfire smoke to date. Smoldering combustion is usually associated with enhanced PM emissions, but our δPM2.5 δCO ratio (0.126±0.002) was about half the δPM1.0 δCO measured in fresh wildfire smoke from aircraft (∼ 0.266). Assuming PM2.5 is dominated by PM1, this suggests that aerosol evaporation, at least near the surface, can often reduce PM loading and its atmospheric/air-quality impacts on the timescale of several days. Much of the smoke was emitted late in the day, suggesting that nighttime processing would be important in the early evolution of smoke. The diurnal trends show brown carbon (BrC), PM2.5, and CO peaking in the early morning and BC peaking in the early evening. Over the course of 1 month, the average single scattering albedo for individual smoke peaks at 870nm increased from ∼ 0.9 to ∼ 0.96. B/scat401 B/scat870 was used as a proxy for the size and photochemical age of the smoke particles, with this interpretation being supported by the simultaneously observed ratios of reactive trace gases to CO. The size and age proxy implied that the Ångström absorption exponent decreased significantly after about 10h of daytime smoke aging, consistent with the only airborne measurement of the BrC lifetime in an isolated plume. However, our results clearly show that non-BC absorption can be important in typical regional haze and moderately aged smoke, with BrC ostensibly accounting for about half the absorption at 401nm on average for our entire data set

Airborne observations of aerosol microphysical properties and particle ageing processes in the troposphere above Europe

In-situ measurements of aerosol microphysical properties were performed in May 2008 during the EUCAARI-LONGREX campaign. Two aircraft, the FAAM BAe-146 and DLR Falcon 20, operated from Oberpfaffenhofen, Germany. A comprehensive data set was obtained comprising the wider region of Europe north of the Alps throughout the whole tropospheric column. Prevailing stable synoptic conditions enabled measurements of accumulating emissions inside the continental boundary layer reaching a maximum total number concentration of 19 000 particles cm<sup>−3</sup> stp. Ultra-fine particles as indicators for nucleation events were observed within the boundary layer during high pressure conditions and after updraft of emissions induced by frontal passages above 8 km altitude in the upper free troposphere. Aerosol ageing processes during air mass transport are analysed using trajectory analysis. The ratio of particles containing a non-volatile core (250 °C) to the total aerosol number concentration was observed to increase within the first 12 to 48 h from the particle source from 50 to 85% due to coagulation. Aged aerosol also features an increased fraction of accumulation mode particles of approximately 40% of the total number concentration. The presented analysis provides an extensive data set of tropospheric aerosol microphysical properties on a continental scale which can be used for atmospheric aerosol models and comparisons of satellite retrievals

Evolution of trace gases and particles emitted by a chaparral fire in California

Biomass burning (BB) is a major global source of trace gases and particles. Accurately representing the production and evolution of these emissions is an important goal for atmospheric chemical transport models. We measured a suite of gases and aerosols emitted from an 81 hectare prescribed fire in chaparral fuels on the central coast of California, US on 17 November 2009. We also measured physical and chemical changes that occurred in the isolated downwind plume in the first ~4 h after emission. The measurements were carried out onboard a Twin Otter aircraft outfitted with an airborne Fourier transform infrared spectrometer (AFTIR), aerosol mass spectrometer (AMS), single particle soot photometer (SP2), nephelometer, LiCor CO_2 analyzer, a chemiluminescence ozone instrument, and a wing-mounted meteorological probe. Our measurements included: CO_2; CO; NO_x; NH_3; non-methane organic compounds; organic aerosol (OA); inorganic aerosol (nitrate, ammonium, sulfate, and chloride); aerosol light scattering; refractory black carbon (rBC); and ambient temperature, relative humidity, barometric pressure, and three-dimensional wind velocity. The molar ratio of excess O_3 to excess CO in the plume (ΔO_3/ΔCO) increased from −5.13 (±1.13) × 10^(−3) to 10.2 (±2.16) × 10^(−2) in ~4.5 h following smoke emission. Excess acetic and formic acid (normalized to excess CO) increased by factors of 1.73 ± 0.43 and 7.34 ± 3.03 (respectively) over the same time since emission. Based on the rapid decay of C_2H_4 we infer an in-plume average OH concentration of 5.27 (±0.97) × 10^6 molec cm^(−3), consistent with previous studies showing elevated OH concentrations in biomass burning plumes. Ammonium, nitrate, and sulfate all increased over the course of 4 h. The observed ammonium increase was a factor of 3.90 ± 2.93 in about 4 h, but accounted for just ~36% of the gaseous ammonia lost on a molar basis. Some of the gas phase NH_3 loss may have been due to condensation on, or formation of, particles below the AMS detection range. NO_x was converted to PAN and particle nitrate with PAN production being about two times greater than production of observable nitrate in the first ~4 h following emission. The excess aerosol light scattering in the plume (normalized to excess CO_2) increased by a factor of 2.50 ± 0.74 over 4 h. The increase in light scattering was similar to that observed in an earlier study of a biomass burning plume in Mexico where significant secondary formation of OA closely tracked the increase in scattering. In the California plume, however, ΔOA/ΔCO_2 decreased sharply for the first hour and then increased slowly with a net decrease of ~20% over 4 h. The fraction of thickly coated rBC particles increased up to ~85% over the 4 h aging period. Decreasing OA accompanied by increased scattering/particle coating in initial aging may be due to a combination of particle coagulation and evaporation processes. Recondensation of species initially evaporated from the particles may have contributed to the subsequent slow rise in OA. We compare our results to observations from other plume aging studies and suggest that differences in environmental factors such as smoke concentration, oxidant concentration, actinic flux, and RH contribute significantly to the variation in plume evolution observations

An elementary 1-dimensional model for a solid state lithium-ion battery with a single ion conductor electrolyte and a lithium metal negative electrode

As noted above, this contribution is dedicated to Norman Fleck on the occasion of his 60th birthday. I have spent many happy hours in collaboration with Norman, and it has been highly productive, educational, rewarding and enjoyable to do so. I look forward to further interactions with him on the subject of this paper, lithium-ion batteries. This work was funded by the University of California, Santa Barbara and by the University of Aberdeen.Peer reviewedPostprin