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Black carbon (BC) particles in the Arctic contribute to rapid warming of the Arctic by heating the atmosphere and snow and ice surfaces. Understanding the source contributions to Arctic BC is therefore important, but they are not well understood, especially those for atmospheric and snow radiative effects. Here we estimate simultaneously the source contributions of Arctic BC to near-surface and vertically integrated atmospheric BC mass concentrations (MBC_SRF and MBC_COL), BC deposition flux (MBC_DEP), and BC radiative effects at the top of the atmosphere and snow surface (REBC_TOA and REBC_SNOW), and show that the source contributions to these five variables are highly different. In our estimates, Siberia makes the largest contribution to MBC_SRF, MBC_DEP, and REBC_SNOW in the Arctic (defined as > 70° N), accounting for 70 %, 53 %, and 43 %, respectively. In contrast, Asia’s contributions to MBC_COL and REBC_TOA are largest, accounting for 38 % and 45 %, respectively. In addition, the contributions of biomass burning sources are larger (24−34 %) to MBC_DEP, REBC_TOA, and REBC_SNOW, which are highest from late spring to summer, and smaller (4.2−14 %) to MBC_SRF and MBC_COL, whose concentrations are highest from winter to spring. These differences in source contributions to these five variables are due to seasonal variations in BC emission, transport, and removal processes and solar radiation, as well as to differences in radiative effect efficiency (radiative effect per unit BC mass) among sources. Radiative effect efficiency varies by a factor of up to 4 among sources (1465−5439 W g–1) depending on lifetimes, mixing states, and heights of BC and seasonal variations of emissions and solar radiation. As a result, source contributions to radiative effects and mass concentrations (i.e., REBC_TOA and MBC_COL, respectively) are substantially different. The results of this study demonstrate the importance of considering differences in the source contributions of Arctic BC among mass concentrations, deposition, and atmospheric and snow radiative effects for accurate understanding of Arctic BC and its climate impacts.

This work demonstrated the first-ever cold-start operation of an ammonia (NH3)-fueled four-cylinder spark ignition engine with an on-board fuel reformer, applying autothermal reforming. In this system, an electrically heated NH3-air mixture was provided to a reforming catalyst and approximately 3 s was found to elapse between the start of engine rotation and the onset of combustion. Stable fast idle operation in conjunction with a cold start was realized with a H2-to-NH3 molar ratio of 2:1. Nearly zero NH3 emissions were achieved during cold start and fast idle until the engine warmed up, by adsorbing unburned NH3 passing through a three-way catalyst before the catalyst was sufficiently warmed up. The NH3 adsorption capacity of this system could be regenerated during the engine warm-up when the engine was running under lean conditions.

The Arctic region is sensitive to climate change and is warming faster than the global average. Aerosol particles change cloud properties by acting as cloud condensation nuclei and ice-nucleating particles, thus influencing the Arctic climate system. Therefore, understanding the aerosol particle properties in the Arctic is needed to interpret and simulate their influences on climate. In this study, we collected ambient aerosol particles using whole-air and PM10 inlets and residual particles of cloud droplets and ice crystals from Arctic low-level clouds (typically, all-liquid or mixed-phase clouds) using a counterflow virtual impactor inlet at the Zeppelin Observatory near Ny-Ålesund, Svalbard, within a time frame of 4 years. We measured the composition and mixing state of individual fine-mode particles in 239 samples using transmission electron microscopy. On the basis of their composition, the aerosol and cloud residual particles were classified as mineral dust, sea salt, K-bearing, sulfate, and carbonaceous particles. The number fraction of aerosol particles showed seasonal changes, with sulfate dominating in summer and sea salt increasing in winter. There was no measurable difference in the fractions between ambient aerosol and cloud residual particles collected at ambient temperatures above 0 ∘C. On the other hand, cloud residual samples collected at ambient temperatures below 0 ∘C had several times more sea salt and mineral dust particles and fewer sulfates than ambient aerosol samples, suggesting that sea spray and mineral dust particles may influence the formation of cloud particles in Arctic mixed-phase clouds. We also found that 43 % of mineral dust particles from cloud residual samples were mixed with sea salt, whereas only 18 % of mineral dust particles in ambient aerosol samples were mixed with sea salt. This study highlights the variety in aerosol compositions and mixing states that influence or are influenced by aerosol–cloud interactions in Arctic low-level clouds.

The terminal velocity of cloud drops and raindrops used in numerical model calculations can significantly affect weather predictions. Current formulations rely on laboratory experiments made in the 1940s and 1960s. Because these experiments were performed only at typical environmental conditions of 20°C and 1013 hPa, parameterizations have been introduced to deduce the terminal velocity aloft without rigorous evaluation. In this study, an incompressible two-phase flow direct numerical simulation model is used to calculate the free-falling motion of axisymmetric drops with diameters between 0.025 and 0.5 mm to study the terminal fall velocity. Simulated terminal fall velocities of free-falling drops at 20°C and 1013 hPa agree within 3.2% with the previous empirical parameterization (Beard formula), and 4.5% with existing laboratory data in the diameter range between 0.3 and 0.5 mm. The velocities converge to the analytic Hadamard–Rybczynski solution within 2% for small Reynolds numbers, demonstrating the robustness of our simulations. Simulations under various atmospheric conditions show that existing empirical parameterizations that account for the air density dependence of the terminal velocity have errors up to 11.8% under the conditions examined in this study. We propose a new empirical formula that describes the air density dependence of the terminal velocity. It is also shown that the falling speed of a small drop is not sensitive to shape oscillation, and the terminal velocity decreases by only less than 1.3% when the axis ratio increases by 12% with reduced surface tension. Internal circulation within falling drops is also presented and compared with previous studies.

During the PAMARCMiP 2018 campaign (March and April 2018) a proton-transfer-reaction mass spectrometer (PTR-MS) was deployed onboard the POLAR 5 research aircraft and sampled the High Arctic atmosphere under Arctic haze conditions. More than 100 compounds exhibited levels above 1 pmol/mol in at least 25% of the measurements. We used back trajectories and acetone mixing ratios to identify periods with and without long-range transport from continental sources.Air masses with continental influence contained elevated levels of compounds associated with (aged) biogenic emissions or aged anthropogenic pollution (e.g., methanol, peroxyacetylnitrate (PAN), acetone, acetic acid, methylethylketone (MEK), proprionic acid, and pentanone), but benzene – a marker for primary pollution – was not enhanced. Almost half of all positively detected compounds (>100) in the High Arctic atmosphere can be associated with terpene oxidation products. This constitutes a strong signature of biogenic terpenes and their oxidation products on the High Arctic atmosphere. Many of these compounds will condense and produce biogenic secondary organic aerosol (SOA) – a natural source of organic aerosol (OA) in addition to the aerosols that can be associated with anthropogenic pollution. Therefore, we hypothesize that biogenic SOA exerted significant control over the complex system of aerosols, clouds and longwave radiation in the pre-industrial Arctic winter, even though their role is likely marginal under contemporary polluted Arctic haze conditions. However, biogenic SOA may become an important factor in the future again, if biogenic emissions are enhanced due to climate change and if polluting technologies are (hopefully) phased out in the near future.During two flights, surface ozone depletion events (ODE) were observed that coincided with enhanced levels of acetone, and methylethylketone. There is evidence that ODEs may also be associated with the emission of biogenic ice-nucleating particles (INP) because the filter samples taken during these two flights exhibited enhanced levels of highly active ice-nucleating particles (INP).Both these processes, INP production in association with ozone depletion events, and the transport of biogenic SOA could require corrections in estimates of preindustrial radiative forcing (RF). If preindustrial RF has been stronger, the Arctic amplification would be even stronger than currently assumed.

Key Points: • First ever measurements with a high‐accuracy single‐particle soot photometer of black carbon (BC) concentrations in Arctic snowpack • Topography and BC emission flux strongly influenced latitudinal variations of mass concentrations and size distributions of BC • Measured BC mass concentrations 2–25 times lower than previously reported show the importance of revalidating climate models Black carbon (BC) deposited on snow lowers its albedo, potentially contributing to warming in the Arctic. Atmospheric distributions of BC and inorganic aerosols, which contribute directly and indirectly to radiative forcing, are also greatly influenced by depositions. To quantify these effects, accurate measurement of the spatial distributions of BC and ionic species representative of inorganic aerosols (ionic species hereafter) in snowpack in various regions of the Arctic is needed, but few such measurements are available. We measured mass concentrations of size-resolved BC (CMBC) and ionic species in snowpack by using a single-particle soot photometer and ion chromatography, respectively, over Finland, Alaska, Siberia, Greenland, and Spitsbergen during early spring in 2012–2016. Total BC mass deposited per unit area (DEPMBC) during snow accumulation periods was derived from CMBC and snow water equivalent (SWE). Our analyses showed that the spatial distributions of anthropogenic BC emission flux, total precipitable water, and topography strongly influenced latitudinal variations of CMBC, BC size distributions, SWE, and DEPMBC. The average size distributions of BC in Arctic snowpack shifted to smaller sizes with decreasing CMBC due to an increase in the removal efficiency of larger BC particles during transport from major sources. Our measurements of CMBC were lower by a factor of ~13 than previous measurements made with an Integrating Sphere/Integrating Sandwich spectrophotometer due mainly to interference from coexisting non-BC particles such as mineral dust. The SP2 data presented here will be useful for constraining climate models that estimate the effects of BC on the Arctic climate. Plain Language Summary Black carbon (BC) particles, commonly known as soot, are emitted from incomplete combustion of fossil fuels and biomass. They efficiently absorb solar radiation and thus heat the atmosphere. BC particles emitted at midlatitudes and in the Arctic are deposited onto snow in the Arctic, accelerating snowmelt in early spring by absorbing solar radiation. These processes contribute to warming in the Arctic. Calculations of this warming effect by using numerical models need to be validated by comparison with observed BC concentrations in snowpack. However, there are very few accurate records of concentrations of BC in snow because of technical difficulties in making these measurements. We developed a new laser-induced incandescence technique to measure BC concentrations in snowpack and applied it for the first time in six Arctic regions (Finland, Alaska, North and South Siberia, Greenland, and Spitsbergen). The BC concentrations we measured were highest in Finland and South Siberia, which are closer to large anthropogenic BC sources than the other regions, where our measured BC concentrations were much lower. On average, our BC concentrations were much lower than those previously measured by different techniques. Therefore, previous comparisons of modeled and observed BC concentrations need to be re-evaluated using the present data.

Ammonia-free emissions from an engine system fueled with ammonia and hydrogen during cold-start and warm-up periods are demonstrated. The fuels are supplied into a single-cylinder test engine under constant-speed conditions. The exhaust system consists of a redox catalyst followed by an in-line adsorber, the latter of which stores the ammonia that flows through the former. The results show that all adsorbers, H-ZSM-5, Cu-ZSM-5, and Pt-ZSM-5, can adsorb ammonia during cold-start conditions although the engine should be operated with retarded spark timing and a high hydrogen ratio because of low combustion efficiency at low coolant temperatures. Cu-ZSM-5 and Pt-ZSM-5 are regenerated after adsorption through their catalytic reactions without ammonia slip. Cu-ZSM-5, which has the largest adsorption capacity among the tested adsorbers, favors lean burn operation for regeneration. Pt-ZSM-5 has the advantage of simple regeneration control.

Long-term measurements of black carbon (BC) aerosols by filter-based absorption photometers with a heated inlet (COSMOS) in different regions have been useful in elucidating spatial variati...

Aeolian dusts serve as ice nucleating particles in mixed-phase clouds, and thereby alter the cloud properties and lifetime. Glacial outwash plains are thought to be a major dust source in cold, high latitudes. Due to the recent rapid and widespread retreat of glaciers, high-latitude dust emissions are projected to increase, especially in the Arctic region, which is highly sensitive to climate change. However, the potential contribution of high-latitude dusts to ice nucleation in Arctic low-level clouds is not well acknowledged. Here we show that glacial outwash sediments in Svalbard (a proxy for glacially sourced dusts) have a remarkably high ice nucleating ability under conditions relevant for mixed-phase cloud formation, as compared with typical mineral dusts. The high ice nucleating ability of the sediments is probably governed by the presence of small amounts of organic matter (

Black carbon (BC) aerosol deposited in and onto Arctic snow increases the snow's absorption of solar radiation and accelerates snowmelt. Concentrations of BC in the Arctic atmosphere and snow are controlled by wet deposition; however, details of this process are poorly understood owing to the scarcity of time-resolved measurements of BC in hydrometeors. We measured mass concentrations of BC in hydrometeors (CMBC) and in air (MBC) with 16% and 15% accuracies, respectively, at Ny-Ålesund, Svalbard during 2012–2019. Median monthly MBC and CMBC values showed similar seasonal variations, being high in winter-spring and low in summer. Median monthly BC wet deposition mass flux (FMBC) was highest in winter and lowest in summer, associated with seasonal patterns of CMBC and precipitation. Seasonally averaged BC size distributions in hydrometeors were similar except for summer. Measurements of MBC and CMBC in spring 2017 showed a size-independent removal efficiency, indicating that BC-containing particles were efficiently activated into cloud droplets. These observations at Ny-Ålesund were compared with observations at Barrow, Alaska, during 2013–2017. The near-surface MBC at Ny-Ålesund and Barrow had similar seasonal patterns; however, the two sites differed in CMBC and FMBC. In summer, CMBC was low at Ny-Ålesund but moderate at Barrow, likely reflecting differences in MBC in the lower troposphere. Seasonally averaged BC size distributions in hydrometeors were similar at both sites, suggesting that average BC size distributions are similar in the Arctic lower troposphere. The efficiency of BC removal tends to be size-independent during transport, leading to the observed similarity.

Long-term measurements of black carbon (BC) are warranted for investigating changes in its emission, transport, and deposition. However, depending on instrumentation, parameters related to BC such as aerosol absorption coefficient (babs) have been measured instead. Most ground-based measurements of babs in the Arctic have been made by filter-based absorption photometers, including multi-angle absorption photometers (MAAP), particle soot absorption photometers (PSAP), continuous light absorption photometer (CLAP), and Aethalometers. The measured babs can be converted to atmospheric mass concentrations of BC (MBC) by assuming the value of the mass absorption cross section (MAC = babs/MBC). However, the accuracy of conversion of babs to MBC has not been adequately assessed. Here, we introduce a systematic method for deriving MAC values from babs measured by these instruments and independently measured MBC. In this method, MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). COSMOS-derived MBC (MBC (COSMOS)) is traceable to a rigorously calibrated single particle soot photometer (SP2) and the absolute accuracy of MBC (COSMOS) has been demonstrated previously to be about 15 % in Asia and the Arctic. The necessary conditions for application of this method are a high correlation of the measured babs with independently measured MBC, and long-term stability of the correlation slope, which represents the MAC. In general, babs – MBC (COSMOS) correlations were high (r2 = 0.84–0.96 for hourly data) at Fukue in Japan, Barrow in Alaska, Ny-Ålesund in Svalbard, Pallastunturi in Finland, and Alert in Canada, and stable up to for 10 years. We successfully estimated MAC values (11.0–15.2 m2 g−1 at a wavelength of 550 nm) for these instruments and these MAC values can be used to obtain error-constrained estimates of MBC from babs measured at these sites even in the past, when COSMOS measurements were not made. Because the absolute values of MBC in these Arctic sites estimated by this method are consistent with each other, they are applicable to study spatial and temporal variation of MBC and to evaluate performance of numerical model calculations.

The 11th Symposium on Polar Science/Ordinary sessions: [OM] Polar Meteorology and Glaciology, Thu. 3 Dec.

The 11th Symposium on Polar Science/Special session: [S] Accelerating Arctic research: Recent progress and future prospect of Arctic research, Tue. 1 Dec.

The 11th Symposium on Polar Science/Special session: [S] Accelerating Arctic research: Recent progress and future prospect of Arctic research, Tue. 1 Dec.

To constrain uncertainties in radiative forcings associated with aerosol--cloud interactions, improved understanding of Arctic cloud formation is required, yet long-term measurements of the relevant cloud and aerosol properties remain sparse. We present the first long-term study of cloud residuals, i.e. particles that were involved in cloud formation, and ambient aerosol particles in Arctic low-level clouds measured at Zeppelin Observatory, Svalbard. A detailed evaluation of the ground-based counter-flow virtual impactor inlet system is also presented. Cloud residuals as small as 15 nm are routinely observed especially during the dark period and are potentially linked to ice, supporting prior work suggesting that classical droplet activation is not the only relevant process in the formation of Arctic low-level clouds. The reported measurements and findings provide a new basis for improving our understanding of Arctic clouds and for developing robust parameterisations of mixed-phase clouds in Earth system models.

Black carbon (BC) particles cause adverse health effects and contribute to the heating of the atmosphere by absorbing visible solar radiation. Efforts have been made to reduce BC emissions, especially in urban areas; however, long-term measurements of BC mass concentration (MBC) are very limited in Japan. We report MBC measurements conducted in Tokyo from 2003 to 2017, showing that MBC decreased by a factor of 3 from 2003 to 2010 and was stable from 2010 to 2017. Fine particulate concentrations (PM2.5) decreased by a much smaller factor during 2003–2010. The diurnal variations of BC size distributions suggest that the BC in Tokyo originates mainly from local sources, even after 2010. Our three-dimensional model calculations show that BC from the Asian continent contributes a small portion (about 20%) of the annual average MBC in the Kanto region of Japan, which includes Tokyo. This indicates that continued reduction of BC emissions inside Japan should be effective in further decreasing MBC.

Atmospheric iron affects the global carbon cycle by modulating ocean biogeochemistry through the deposition of soluble iron to the ocean. Iron emitted by anthropogenic (fossil fuel) combustion is a source of soluble iron that is currently considered less important than other soluble iron sources, such as mineral dust and biomass burning. Here we show that the atmospheric burden of anthropogenic combustion iron is 8 times greater than previous estimates by incorporating recent measurements of anthropogenic magnetite into a global aerosol model. This new estimation increases the total deposition flux of soluble iron to southern oceans (30–90 °S) by 52%, with a larger contribution of anthropogenic combustion iron than dust and biomass burning sources. The direct radiative forcing of anthropogenic magnetite is estimated to be 0.021 W m−2 globally and 0.22 W m−2 over East Asia. Our results demonstrate that anthropogenic combustion iron is a larger and more complex climate forcer than previously thought, and therefore plays a key role in the Earth system., As a source of soluble iron, anthropogenic combustion iron is considered less important than natural sources. Here, the authors combine new measurements with a global aerosol model and show the atmospheric burden of anthropogenic combustion iron to be 8 times greater than previous estimates.

This article presents a study of the mechanism that the lubricant oil droplet initiates low-speed pre-ignition in highly boosted downsized gasoline engines. Low-speed pre-ignition is a phenomenon that the fuel–air mixture ignites before the spark timing, leading to flame propagation that results in a heavy knock. The ignition of lubricant oil droplets is thought to be one possible mechanism for low-speed pre-ignition. However, the oil droplet ignition conditions are not yet well understood. First, the conditions under which a single oil droplet initiates the combustion of a fuel–air mixture were investigated using a rapid compression and expansion machine. When an initial droplet temperature was above 250 °C, the vaporized oil ignited before the gasoline–air mixture, in which case the combustion of the gasoline–air mixture around the droplet was initiated. The numerical results showed that the oil droplet temperature increases above 250 °C if the droplet is heated by burned gas remaining in the combustion chamber from the previous cycle. A direct-injection single-cylinder research engine was operated under the condition that no residual gas exists in the combustion chamber. In this case, no low-speed pre-ignition occurred even if gross indicated that mean effective pressure was 2.5 MPa. These results indicate that an oil droplet does not cause low-speed pre-ignition if any droplet flies into the combustion chamber unless it remains in the chamber over the exhaust stroke.

Long-term measurements of the light absorption coefficient (b(abs)) obtained with a particle soot absorption photometer (PSAP), b(abs) (PSAP), have been previously reported for Barrow, Alaska, and ...

Two years of continuous in situ measurements of Arctic low‐level clouds have been made at the Mount Zeppelin Observatory (78°56′N, 11°53′E), in Ny‐Alesund, Spitsbergen. The monthly median value of the cloud particle number concentration (Nc) showed a clear seasonal variation: Its maximum appeared in May–July (65 ± 8 cm−3), and it remained low between October and March (8 ± 7 cm−3). At temperatures warmer than 0 °C, a clear correlation was found between the hourly Nc values and the number concentrations of aerosols with dry diameters larger than 70 nm (N70), which are proxies for cloud condensation nuclei (CCN). When clouds were detected at temperatures colder than 0 °C, some of the data followed the summertime Nc to N70 relationship, while other data showed systematically lower Nc values. The lidar‐derived depolarization ratios suggested that the former (CCN‐controlled) and latter (CCN‐uncontrolled) data generally corresponded to clouds consisting of supercooled water droplets and those containing ice particles, respectively. The CCN‐controlled data persistently appeared throughout the year at Zeppelin. The aerosol‐cloud interaction index (ACI = dlnNc/(3dlnN70)) for the CCN‐controlled data showed high sensitivities to aerosols both in the summer (clean air) and winter–spring (Arctic haze) seasons (0.22 ± 0.03 and 0.25 ± 0.02, respectively). The air parcel model calculations generally reproduced these values. The threshold diameters of aerosol activation (Dact), which account for the Nc of the CCN‐controlled data, were as low as 30–50 nm when N70 was less than 30 cm−3, suggesting that new particle formation can affect Arctic cloud microphysics.

The Ninth Symposium on Polar Science/Ordinary sessions: [OM] Polar meteorology and glaciology, Wed. 5 Dec. / 3F Multipurpose Conference room, National Institute of Polar Research

We quantify the responses of aerosols to changes in emissions (sulfur dioxide, black carbon (BC), primary organic aerosol, nitrogen oxides (NOx), and volatile organic compounds) over East Asia by using simulations including gas-oxidant-aerosol coupling, organic aerosol (OA) formation, and BC aging processes. The responses of aerosols to NOx emissions are complex and are dramatically changed by simulating gas-phase chemistry and aerosol processes online. Reduction of NOx emissions by 50% causes a 30–40% reduction of oxidant (hydroxyl radical and ozone) concentrations and slows the formation of sulfate and OA by 20–30%. Because the response of OA to changes in NOx emissions is sensitive to the treatment of emission and oxidation of semivolatile and intermediate volatility organic compounds, reduction of the uncertainty in these processes is necessary to evaluate gas-oxidant-aerosol coupling accurately. Our simulations also show that the sensitivity of aerosols to changes in emissions is enhanced by 50–100% when OA formation and BC aging processes are resolved in the model. Sensitivity simulations show that the increase of NOx emissions from 1850 to 2000 explains 70% (40%) of the enhancement of aerosol mass concentrations (direct radiative effects) over East Asia during that period through enhancement of oxidant concentrations and that this estimation is sensitive to the representation of OA formation and BC aging processes. Our results demonstrate the importance of simultaneous simulation of gas-oxidant-aerosol coupling and detailed aerosol processes. The impact of NOx emissions on aerosol formation will be a key to formulating effective emission reduction strategies such as BC mitigation and aerosol reduction policies in East Asia.

An improved understanding of the variations in the mass concentration and size distribution of black carbon (BC) in the free troposphere (FT) over East Asia, where BC emissions are very high, is needed to reliably estimate the radiative forcing of BC in climate models. We measured these parameters and the carbon monoxide (CO) concentration by conducting the Aerosol Radiative Forcing in East Asia (A-FORCE) 2013W aircraft campaign in East Asia in winter 2013 and compared these data with measurements made in the same region in spring 2009. The median BC concentrations in the FT originating from North China (NC) and South China (SC) showed different seasonal variations, which were primarily caused by variations in meteorological conditions. CO concentrations above the background were much higher in SC than in NC in both seasons, suggesting a more active upward transport of CO. In SC, precipitation greatly increased from winter to spring, leading to an increased wet deposition of BC. As a result, the median BC concentration in the FT was highest in SC air in winter. This season and region were optimal for the effective transport of BC from the planetary boundary layer to the FT. The count median diameters of the BC size distributions generally decreased with altitude via wet removal during upward transport. The altitude dependence of the BC size distributions was similar in winter and spring, in accord with the similarity in the BC mixing state. The observed BC concentrations and microphysical properties will be useful for evaluating the performance of climate models.