Individual Plumes Research Articles

Inferring ion cluster lifetimes from energy-resolved mass spectra of an EMI-BF4 electrospray plume

The fragmentation of ion clusters within the accelerating fields of ionic liquid ion sources (ILISs) is well documented and degrades ILIS performance and lifetime. Some of the most popular ILIS liquids, such as EMI-BF4 (1-Ethyl-3-methylimidazolium tetrafluoroborate) and EMI-Im (1-Ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide), emit clusters with lifetimes as low as ∼1 ns. Studies of fragmentation within the accelerating field typically rely on measuring the plume energy distribution averaged over all plume species and comparing those measurements with numerical simulations to estimate ion cluster lifetimes. Here, for the first time, we estimate EMI-BF4 cluster lifetimes by analyzing the energy distributions of individual plume species. We use this novel analysis method to estimate mean lifetimes of positive EMI-BF4 ion clusters from previously published experimental data. We find that the mean lifetime ranges from τ=3.7ns to τ=124ns for [EMI+][EMI-BF4] dimers and ranges from τ=1.5ns to τ=23ns for [EMI+][EMI-BF4]2 trimers. Fitting those data to an analytical fragmentation model, we estimate the binding energy and temperature as ΔGS0=0.49eV and T=394K for dimers and ΔGS0=0.40eV and T=365K for trimers. Comparing our results with previous studies supports the conclusion that clusters are emitted with a wide distribution of internal energies, contrary to the common assumption of single internal energy for each species.

Satellite‐Based Surveys Reveal Substantial Methane Point‐Source Emissions in Major Oil & Gas Basins of North America During 2022–2023

AbstractUtilizing imaging spectroscopy technology to identify methane super‐emitters plays a vital role in mitigating methane emissions in the Oil & Gas (O&G) sector. While earlier research has uncovered significant point‐source methane emissions from O&G production in the US and Canada, which are key regions with large methane emissions, a comprehensive post‐COVID‐19 survey has been notably absent. Here, we perform a detailed survey of methane super‐emitters across multiple basins of North America (Marcellus Shale, Haynesville/Bossier Shale, Permian Basin and Montney Shale) using the new Chinese Gaofen5‐01A/02 (GF5‐01A/02) satellite measurements during 2022–2023. We detect 139 individual methane plumes emanating from 122 point sources, with flux rates ranging from 519 to 16,071 kg hr−1. These emissions exhibit a highly skewed and heavy‐tailed distribution, constituting approximately 23% of the flux inversion with TROPOMI in the sample region, with a range of 13%–40%. Moreover, we observe a 66.7% reduction in methane emissions in Permian Basin during COVID‐19, followed by fluctuations until spring 2023. By summer 2023, methane emissions rebound to twice their previous magnitude (1.68 ± 0.58 Tg a−1). Using these point‐source surveys, we further quantify a regional methane emission of 2.69 ± 0.86 Tg a−1 in Permian Basin. This estimation closely aligns with top‐down inversions (2.22 ± 0.40 Tg a−1) from TROPOMI. The upscale estimation underscores the effectiveness of high‐resolution remote sensing measurements in improving bottom‐up emissions inventories and refining regional methane emission assessments. Our results highlight the potential climate benefits derived from regular monitoring and specific remediation efforts focused on relatively few strong point‐source emissions.

A planar plume array emanating from an atmospheric pressure argon plasma jet employing floating electrodes

Large-scale plasma plumes downstream of plasma jets are in urgent need from a practical viewpoint. In this Letter, an argon plasma jet with floating electrodes is proposed to produce a large-scale planar plume array. Results indicate that with increasing peak voltage (Vp), the planar plume array elongates gradually and scales up in the lateral direction to an optimal value of 90.0 mm. There is only one discharge pulse per voltage half cycle, whose intensity and duration increase with increasing Vp. Moreover, there is a time lag between the initiations of individual plumes. Fast photography reveals that the planar plume array originates from the repeated process of some micro-discharge filaments stretching along the argon stream. By optical emission spectroscopy, the spatial distribution of plasma parameters is obtained, such as electron density, electron temperature, and gas temperature. At last, the planar plume array is employed to test the surface modification of polyethylene terephthalate, for which a uniform modification has been realized with a scan velocity of 1.0 cm/min. These results are of great significance for the development of large-scale atmospheric pressure plasma sources.

Impact of Dust Source Patchiness on the Existence of a Constant Dust Flux Layer During Aeolian Erosion Events

AbstractDust emission fluxes during wind soil erosion are usually estimated using a dust concentration vertical gradient, by assuming a constant dust flux layer between the surface and the dust measurement levels. Here, we investigate the existence of this layer during erosion events recorded in Iceland and Jordan. Size‐resolved dust fluxes were estimated at three levels between 2 and 4 m using the eddy‐covariance method. Dust fluxes were found mainly constant only between the two upper levels in Iceland, the lower dust flux being often stronger and richer in coarse particles, while dust fluxes in Jordan were nearly constant across all levels. The wind dynamics could not explain the absence of a constant dust flux layer in Iceland. We show that the presence of stationary dust source patches in Iceland, related to surface humidity, created a non‐uniform dust layer near the surface, named dust roughness sublayer (DRSL), where individual plumes behind each patch interact but do not fully mix. The lowest dust measurement level was probably located within this sublayer while the upper ones were located above, such that there the emitted dust became spatially well‐mixed. This explains near the surface in Iceland, the more intermittent dust concentration, its low correlation with the dust concentrations above, and the richer dust flux in coarse particles due to their lower deposition contribution. Our findings highlight the importance of estimating dust fluxes above a dust blending height whose characteristics depend on the dust source patchiness caused by surface humidity or the presence of sparse non‐erosive elements.

Application of Effective Conversion Rates between NO and NO2 in a Standard Airport Dispersion Model System

The NO/NO2/O3 reaction mechanism of the standard VDI 3783 Part 19 was coupled to the Lagrangian particle model LASAT and quasi-stationary, individual plumes were calculated for a point source under various conditions. First-order conversion rates between NO and NO2 were derived by fitting to these plumes and further simplified to sets of categorized conversion rates which depend on background NO2 concentration, atmospheric stability and time of the day. The rates were applied in the standard airport dispersion model system LASPORT and compared to measured NO2 concentrations at Los Angeles International Airport. The agreement between modelled and measured NO2 concentrations (weekly averages) and ratios NO2 over NOx at monitor stations dominated by airport emissions was in most cases better than a factor of 2 with a Pearson correlation coefficient of about 0.9 or above.

Numerical study on the onset of global-scale flow from individual buoyant plumes: Implications for indoor disease transmission

Transport of exhaled droplets and aerosol suspension is a main route for the transmission of highly infectious respiratory diseases. A poorly ventilated room, where human body heat drives the flow and the pathogen motion, is one such paradigmatic situation with an elevated risk of viral transmission. Here, we report a numerical study on human body heat-driven buoyancy convection in a slender rectangular geometry with the geometric size of 12 × 1 × 3 m3. Using large-scale three-dimensional simulations, we reveal how different spacings between human body heat sources can potentially spread pathogenic species between occupants in a room. Morphological transition in airflow takes place as the distance between human heat sources is varied, which shapes distinct patterns of disease transmission: For sufficiently large distance, individual buoyant plume creates a natural barrier, forming buoyant jets that block suspension spread between occupants. Thermal plumes exhibit significant individual effects. However, for small distances, a collective effect emerges and thermal plumes condense into superstructure, facilitating long-distance suspension transport via crossing between convection rolls. In addition, we quantify the impact of morphological transition on the transport of viral particles by introducing tracer particles. The quantitative analysis shows that under certain critical distances, the infection risk becomes significantly elevated due to this transition and collective behavior. Our findings highlight the importance of reasonable social distancing to reduce indoor cross-transmission of viral particles between people and provide new insights into the hidden transitional behavior of pathogen transmission in indoor environments.

Unpaved road particulate matter emission rates and vehicle-induced transient plume characteristics.

Particulate matter (PM) emitted from unpaved rural roads presents a potential inhalation hazard to people living and working near them. In the absence of site-specific exposure data, plume dispersion modeling can be used to predict ambient particulate concentrations in the vicinity of the unpaved roads. Hourly averaged PM10 concentrations were measured near a gravel road using an EPA reference method resulting in a geometric mean of 50 μg m-3. With these ambient concentrations, the AERMOD plume dispersion model was used to derive a PM emission factor of 444 g/VKT (grams per vehicle kilometer travelled). This result was lower than the emission factor calculated using the EPA's AP-42 guidance for unpaved roads (795 g/VKT). The transient nature of the plume of PM concentrations due to road traffic was also evaluated using a direct-reading instrument. Vehicle speed and wind speed were found to be significant determinants of PM concentration, average PM concentration, and total PM mass for each plume. Each vehicle produced an average concentration of 4096 μg m-3 over the duration of the plume. Therefore, residents near the road are potentially exposed to substantially higher short-term concentrations from individual plumes than would be indicated by hourly averages.

Fuel temperature and injection pressure influence on the cold start GDI sprays

Cold start in gasoline direct injection engines (GDI) is a critical issue that significantly impacts fuel consumption and emissions. Therefore, it is essential to investigate and improve the spray and air-fuel mixing processes during cold starts. This study employed a complimentary set of optical diagnostic techniques, including line-of-sight(extinction, Schlieren, and long-distance microscopy) and 3D computed tomography (CT), to characterize and understand the cold-start spray dynamics under various fuel temperature and injection pressure conditions. The experiments were conducted in a constant volume spray vessel and the fuel temperature was varied using a coolant circulator, with temperatures reaching as low as -7 °C to simulate cold-start conditions. The cold fuel exhibited longer liquid/vapor penetration lengths compared to hot fuel under low injection pressure conditions. This deterioration in spray characteristics was attributed to the attenuated fuel evaporation and reduced entrainment of ambient air. The 3D spray visualization obtained through the CT algorithm, particularly the cut plane images, revealed that plumes with low fuel temperatures had narrower individual plume widths, resulting in minimized plume-to-plume interaction. Microscopic imaging further confirmed this observation which showed separate plumes in the near-nozzle region for cold fuel conditions. Meanwhile, hot fuel under high injection pressure conditions exhibited complete plume collapsing, leading to a significant amount of liquid fuel remaining in the spray core. The liquid penetration reached 70 mm during the injection period, potentially can cause wall wetting on the piston top or cylinder wall. Based on the experimental findings, this study suggests the application of multiple injections with a moderate level of injection pressure for optimized engine performance and reduced emissions during cold starts.

Large-Scale Circulations and Dry Tropical Cyclones in Direct Numerical Simulations of Rotating Rayleigh–Bénard Convection

Abstract The organization of convection into relatively long-lived patterns of large spatial scales, like tropical cyclones, is a common feature of Earth’s atmosphere. However, many key aspects of convective aggregation and its relationship with tropical cyclone formation remain elusive. In this work, we simulate highly idealized setups of dry convection, inspired by the Rayleigh–Bénard system, to probe the effects of different thermal boundary conditions on the scale of organization of rotating convection, and on the formation of tropical cyclone–like structures. We find that in domains with sufficiently high aspect ratios, moderately turbulent (), moderately rotating () convection organizes more persistently and at larger scales when thermal boundary conditions constrain heat fluxes rather than temperatures. Furthermore, for some thermal boundary conditions with asymmetric heat fluxes, convection organizes into persistent vortices with the essential properties of mature tropical cyclones: a warm core, high axisymmetry, a strong azimuthal circulation, and substantially larger size than individual buoyant plumes. We argue that flux asymmetry results in a persistent and localized input of buoyancy, which allows spatially aggregated convection to sustain a warm core in a developing large-scale vortex. Crucially, the most intense and axisymmetric cyclone forms for setups where the bottom heat flux is enhanced by the nearby flow and the top boundary is insulating, as long as the convective Rossby number is higher than about 1. Our results demonstrate the great potential for dialogue between classical turbulence research and the study of convective aggregation and tropical cyclones. Significance Statement On Earth, atmospheric convection frequently organizes into large spatial patterns that persist for several days, like tropical cyclones. However, many aspects of this process of organization and its link to tropical cyclone formation are not fully understood. In this work, we use numerical simulations of simple setups of rotating convection without moisture to study the minimal conditions that produce large-scale convective organization, and the spontaneous formation of tropical cyclone–like structures. We find that the latter form more readily for a particular set of controlling parameters and thermal boundary conditions. Our approach seeks to narrow the disciplinary gap between tropical cyclone physics and traditional turbulence research, by bringing together methods, questions, and results that are of potential interest to both.

Influence of the Coriolis Force on Spreading of River Plumes

Wind is the main external force that governs the spreading of river plumes in the sea. Many previous studies demonstrated that the spreading direction of river plumes (especially small plumes) generally coincides with wind direction. At the same time, the majority of river plumes are strongly affected by the Coriolis force, which is also among the baseline knowledge about the plumes. In this study, we focus on the deflection of plumes from wind direction induced by the Coriolis force, which received little attention before. For this purpose, we analyzed an extensive set of Landsat 8 and Sentinel-2 satellite images of multiple small- and medium-sized river plumes at different parts of the World Ocean and synchronous wind reanalysis data. We demonstrated that the deflection angle is stable for individual river plumes for different wind directions, albeit with certain limitations related to wind speed and coastal morphology. Moreover, the deflection angle is similar for river plumes located at similar latitudes and varies from ~0° near the Equator to 15–25° in temperate zones and ~30° in polar zones. Finally, we derived a direct relation between latitude and the deflection angle. The obtained results contribute to our understanding of universal features of river plume dynamics, which is important for monitoring and forecasting of delivery and fate of fluvial water and river-borne matter in different coastal regions of the World Ocean.

Assessing the Impact of Self‐Lofting on Increasing the Altitude of Black Carbon in a Global Climate Model

AbstractBlack carbon (BC) absorbs solar radiation, increasing the buoyancy and vertical ascent of absorbing aerosol in the atmosphere. This self‐lofting process has been observed for individual plumes in the troposphere and lower stratosphere but here we show it occurring at broader scales through enhanced large‐scale ascent over BC‐rich regions. This is demonstrated in a pair of simulation using the UKESM1 Earth‐System model where BC aerosols were modeled either with or without the ability to absorb radiation. With absorption included the annual global mean concentration of BC in the upper troposphere and lower stratosphere (8–22 km) rose by up to 50% and the column loading over some remote oceanic regions more than doubled. The increase in aerosol height was particularly notable over the southeast Atlantic where biomass burning aerosol from Africa was elevated up to 1 km higher when their absorption was included. Similar effects were seen over the Arctic where the absorbing haze was transported in at higher levels and surface concentrations were halved. The absorption by BC also increased ascent over southern Asia, which tended to thicken the Asian brown cloud during the dry season but in the wet season enhancing ascent promoted deep convection and had the tendency to deplete the aerosol through wash‐out. We conclude that representing aerosol absorption accurately is important in simulating the vertical distribution, transport and abundance of aerosol in the Earth‐system that will affect their interactions with climate.

Mantle plume heat flux and surface motion periodicities and their implications for the growth of continental crust

About 40% of Earth's surface is covered by continental crust. It has been found that the global detrital zircon age distribution is dominated by multiple periodicities from <100 Myr to ∼800 Myr, suggesting that continental crust may have been produced periodically. However, what causes the periodic growth of continental crust remains unclear. Continental crust is produced mainly by arc magmatism at subduction zones and plume-induced magmatism. With 3D global mantle convection models, we investigate the long-term evolution of heat flux of mantle plumes and surface flow velocity, which can be respectively related to plume-induced magmatism and arc magmatism. About 10-30 plumes are present in our models, with significant spatial and temporal variations of heat flux for individual plumes. Both the temporal variations of the total plume heat flux and the root-mean-square (rms) of the surface velocity in our models have periodicities that decrease with the vigor of mantle convection. When extrapolated to conditions with Earth-like vigor of convection, the total plume heat flux and the rms of the surface velocity vary with periodic cycles of ∼90-200 Myr and ∼300 Myr, respectively. Therefore, the ∼90-200 Myr and the ∼300 Myr periodic cycles in the growth of continental crust as suggested by the global detrital zircon age distribution may be respectively caused by plume-induced magmatism and arc magmatism.

Volcanic Emissions, Plume Dispersion, and Downwind Radiative Impacts Following Mount Etna Series of Eruptions of February 21–26, 2021

AbstractDuring the extended activity of Mount Etna volcano in February–April 2021, three distinct paroxysmal events took place from February 21 to 26, which were associated with a very uncommon transport of the injected upper‐tropospheric plumes toward the north. Using a synergy of observations and modeling, we characterized the emissions and three‐dimensional dispersion for these three plumes, monitored their downwind distribution and optical properties, and estimated their radiative impacts at selected locations. With a satellite‐based source inversion, we estimate the emitted sulfur dioxide (SO2) mass at an integrated value of 55 kt and plumes injections at up to 12 km altitudes, which qualifies this series as an extreme event for Mount Etna. Then, we combine Lagrangian dispersion modeling, initialized with measured temporally resolved SO2 emission fluxes and altitudes, with satellite observations to track the dispersion of the three individual plumes. The transport toward the north allowed the height‐resolved downwind monitoring of the plumes at selected observatories in France, Italy, and Israel, using LiDARs and photometric aerosol observations. Volcanic‐specific aerosol optical depths (AODs) in the visible spectral range ranging from about 0.004 to 0.03 and local daily average shortwave radiative forcing (RF) ranging from about −0.2 to −1.2 W m−2 (at the top of atmosphere) and from about −0.2 to −3.0 W m−2 (at the surface) are found. The composition (possible presence of ash), AOD, and RF of the plume have a large inter‐plume and intra‐plume variability and thus depend strongly on the position of the sampled section of the plumes.

CO2 emissions retrieval from coal-fired power plants based on OCO-2/3 satellite observations and a Gaussian plume model

The CO2 emissions from coal-fired power plants are a major source of carbon emissions in China. However, the existing emission inventory does not accurately reflect current emissions because of a lag in the statistical data and the accuracy limit for emissions factor. This study aims to provide a method for estimating CO2 emissions from coal-fired power plants based on an improved Gaussian plume model and the Orbiting Carbon Observatory 2/3 satellite. We quantified CO2 emissions from six coal-fired power plants (>3000 MW) in China using 14 plumes from the OCO-2 (2014.09.06–2021.10.01) and OCO-3 (2019.08.06–2021.10.01) datasets. Four of the plumes are in good agreement with those from co-located the Tropospheric Monitoring Instrument measurements of co-emitted NO2. The estimated CO2 emissions ranged from 31.81 to 99.71 kt/d with correlation coefficient of 0.47–0.95. The uncertainty of individual plumes varied from 8% to 42% (1σ), with wind speed being the greatest source of uncertainty, and the average XCO2 enhancement of all power plants in this study is less than 1 ppm when the wind speed increases to about 10 m/s. After validation, our results show high agreement with the existing emission inventory. However, this study found that the Carbon Monitoring for Action may have underestimated the CO2 emissions from Tuoketuo due to the timing of the update, and carbon brief may have underestimated the emissions from Wujiaqu by ignoring the high emission factor of lignite. This study helps monitor and estimate important point source carbon emissions, which is not only a prerequisite for the power industry to carry out carbon reduction efforts, but also helps develop specific regional carbon reduction policies, which are important for reducing anthropogenic carbon emissions.

The isotopic origin of Lord Howe Island reveals secondary mantle plume twinning in the Tasman Sea

Thermochemical convective instabilities in the mantle, often referred to as mantle plumes, cause mantle melting that give rise to ocean island basalts (OIB) in intraplate settings. The array of radiogenic isotope signatures in global intraplate OIB indicate that although plumes are individual entities, they share enriched components that resemble various parts of subducted crust and a hypothetical mantle matrix termed “focal zone” (FOZO). Each plume is expected to rise with an individual buoyancy flux, thereby producing variable volumes of melting with some OIB forming subaerial islands, whereas others produce submarine volcanoes.Here, we report the first radiogenic isotope data (Sr, Nd, Pb and Hf) for lavas of Lord Howe Island (LHI) in the Tasman Sea, the most prominent subaerial expression of the hypothesised Lord Howe mantle plume. Major element data are consistent with a moderate degree of partial melting, and heavy rare earth element depletion indicates melting occurred in the presence of garnet, consistent with other global plume lavas. Radiogenic SrNd isotopic data are similar to those defining the relatively primitive FOZO component with no clear enriched mantle affinity. The nearby Tasmantid Seamounts are also sourced from a mantle plume, and have similar SrNd character. However, combined 208Pb/204Pb and 207Pb/204Pb vs 206Pb/204Pb ratios of LHI lavas are inconsistent with a FOZO-type source. Instead, Pb isotopes overlap with typical enriched mantle 1 (EM1) lavas (e.g., Pitcairn, Tristan da Cunha), trending slightly higher than the Northern Hemisphere Reference Line (NHRL). Hafnium isotopes follow trends observed in lavas of the archetypal EM1 Pitcairn-Gambier islands, and are partially decoupled from 143Nd/144Nd; this decoupling is rare among OIB. The combined element-isotope data indicate that LHI forms the most recent expression of a mantle plume track in the Tasman Sea. Albeit unique in its 208Pb*/206Pb* isotope code among global mantle plumes, the resemblance of LHI lavas with the spatially related and contemporaneous Taupo seamount of the parallel Tasmantid plume track in the Tasman sea supports a genetic relation of both plumes. The proposed common origin of the two parallel plume tracks requires a larger plume underpinning the Tasman sea with individual plume fingers rising towards the surface, possibly in a triple plume network considering the on-shore Cosgrove track in eastern Australia. The subaerial expression of LHI contrasts the submarine Tasmantid Seamounts; this expression is only possible due to the continental ribbon that forms the island's foundation, suggesting secondary plume fingers display similar low buoyancy fluxes. Plain language summaryLord Howe Island is predominantly composed of basaltic rocks, which are created when mantle underneath the crust melts and the subsequent magma rises to the surface and erupts out of a volcano. The chemical composition of these volcanic rocks can provide us with valuable information about geologic processes. Moreover, we can compare the composition of islands like Lord Howe to better investigate and understand volcanic networks that exist deep within the Earth. The composition of Lord Howe Island basalts was investigated for the first time using specialised instruments that can separate individual elements into different isotopes. The ratios of these different isotopes reflects the composition of the mantle source which can be enriched by the presence of subducted crustal rocks, oceanic rocks and sediments. Our data indicate the distinctive reservoir that Lord Howe Island samples were derived from is the same reservoir as that of the nearby Taupo Seamount volcano. We infer from this that a piece of ancient crust is stuck in the mantle, and the two volcanoes are sampling it. This study supports a theory of a large, linked volcanic network under the Tasman Sea, and adds to the growing body of research investigating ‘double-chain’ volcanism in the Pacific and Atlantic oceans.

Reconstructing volcanic radiative forcing since 1990, using a comprehensive emission inventory and spatially resolved sulfur injections from satellite data in a chemistry-climate model

Abstract. This paper presents model simulations of stratospheric aerosols with a focus on explosive volcanic eruptions. Using various (occultation and limb-based) satellite instruments, providing vertical profiles of sulfur dioxide (SO2) and aerosol extinction, we characterized the chemical and radiative influence of volcanic aerosols for the period between 1990 and 2019. We established an improved and extended volcanic SO2 emission inventory that includes more than 500 explosive volcanic eruptions reaching the upper troposphere and the stratosphere. Each perturbation identified was derived from the satellite data and incorporated as a three-dimensional SO2 plume into a chemistry-climate model without the need for additional assumptions about altitude distribution and eruption duration as needed for a “point source” approach. The simultaneous measurements of SO2 and aerosol extinction by up to four satellite instruments enabled a reliable conversion of extinction measurements into injected SO2. In the chemistry-climate model, the SO2 from each individual plume was converted into aerosol particles and their optical properties were determined. Furthermore, the aerosol optical depth (AOD) and the instantaneous radiative forcing on climate were calculated online. Combined with model improvements, the results of the simulations are consistent with the observations of the various satellites. Slight deviations between the observations and model simulations were found for the large volcanic eruption of Pinatubo in 1991 and cases where simultaneous satellite observations were not unique or too sparse. Weak- and medium-strength volcanic eruptions captured in satellite data and the Smithsonian database typically inject about 10 to 50 kt SO2 directly into the upper troposphere/lower stratosphere (UTLS) region or the sulfur species are transported via convection and advection. Our results confirm that these relatively minor eruptions, which occur quite frequently, can nevertheless contribute to the stratospheric aerosol layer and are relevant for the Earth's radiation budget. These minor eruptions cause a total global instantaneous radiative forcing of the order of −0.1 W m−2 at the top of the atmosphere (TOA) compared to a background stratospheric aerosol forcing of about −0.04 W m−2. Medium-strength eruptions injecting about 400 kt SO2 into the stratosphere or accumulation of consecutive smaller eruptions can lead to a total instantaneous forcing of about −0.3 W m−2. We show that it is critical to include the contribution of the extratropical lowermost stratospheric aerosol in the forcing calculations.

Understanding the potential of Sentinel-2 for monitoring methane point emissions

Abstract. The use of satellite instruments to detect and quantify methane emissions from fossil fuel production activities is highly beneficial to support climate change mitigation. Different hyperspectral and multispectral satellite sensors have recently shown potential to detect and quantify point-source emissions from space. The Sentinel-2 (S2) mission, despite its limited spectral design, supports the detection of large emissions with global coverage and high revisit frequency thanks to coarse spectral coverage of methane absorption lines in the shortwave infrared. Validation of S2 methane retrieval algorithms is instrumental in accelerating the development of a systematic and global monitoring system for methane point sources. Here, we develop a benchmarking framework for such validation. We first develop a methodology to generate simulated S2 datasets including methane point-source plumes. These benchmark datasets have been created for scenes in three oil and gas basins (Hassi Messaoud, Algeria; Korpeje, Turkmenistan; Permian Basin, USA) under different scene heterogeneity conditions and for simulated methane plumes with different spatial distributions. We use the simulated methane plumes to validate the retrieval for different flux rate levels and define a minimum detection threshold for each case study. The results suggest that for homogeneous and temporally invariant surfaces, the detection limit of the proposed S2 methane retrieval ranges from 1000 to 2000 kg h−1, whereas for areas with large surface heterogeneity and temporal variations, the retrieval can only detect plumes in excess of 500 kg h−1. The different sources of uncertainty in the flux rate estimates have also been examined. Dominant quantification errors are either wind-related or plume mask-related, depending on the surface type. Uncertainty in wind speed, both in the 10 m wind (U10) and in mapping U10 to the effective wind (Ueff) driving plume transport, is the dominant source of error for quantifying individual plumes in homogeneous scenes. For heterogeneous and temporally variant scenes, the surface structure underlying the methane plume affects the plume masking and can become a dominant source of uncertainty.

Linear Stochastic Analysis of the Partial Reversibility of Ensemble and Effective Dispersion in Heterogeneous Porous Media

AbstractMacrodispersion in heterogeneous formations is caused by spatial variability of the velocity field, making different parts of a plume experience different advective displacements. Differential advection interacts with diffusion, which hardly affects longitudinal ensemble dispersion (i.e., the spread of the ensemble‐averaged concentration) but determines effective dispersion, that is, the expected spread of individual plumes for point injections. The latter has been suggested as metric of solute mixing. Pure advection is fully reversible, whereas diffusion is completely irreversible. We quantify the partial reversibility of macrodispersion by analyzing the second central ensemble and effective spatial moments for advective‐diffusive transport in heterogeneous domains with flow reversal, applying linear stochastic theory to approximate the corresponding moments and comparing them to particle‐tracking random‐walk simulations in periodic media. Diffusion causes solute particles to deviate from their forward trajectories when flow is reversed. As long as advective memory dominates, both types of second central moments decrease during backward motion, then reach a minimum, and increase again. The reversibility is considerably bigger for ensemble than effective dispersion but the latter also shows partial reversibility, challenging its use as metric of mixing. The stronger diffusion is in comparison to advection, the less reversible dispersion becomes. After equally long times of forward and backward motion, the two types of second central moments differ, but to a much smaller extent than in pure forward motion. In realistic settings, the advective memory affects dispersion so strongly that the asymptotic regime is not reached before the plume center has returned to its origin.

Introducing the VIIRS-based Fire Emission Inventory version 0 (VFEIv0)

Abstract. A new open biomass burning inventory is presented that relies on the fire radiative power data from the Visible Infrared Imaging Radiometer Suite (VIIRS) on board the Suomi NPP satellite. This VIIRS-based Fire Emission Inventory (VFEI) provides emission data from early 2012 to 2019 for more than 40 species of gases and aerosols at spatial resolutions of around 500 m. We found that VFEI produces similar results when compared to other major inventories in many regions of the world. Additionally, we conducted regional simulations using VFEI with the Weather Research and Forecasting (WRF) model with chemistry (WRF-Chem) for Southern Africa (September 2016) and North America (July–August 2019). We compared aerosol optical depth (AOD) from the model against two observational datasets: the MODIS Multi-Angle Implementation of Atmospheric Correction (MAIAC) product and AErosol RObotic NETwork (AERONET) stations. Results showed good agreement between both simulations and the datasets, with mean AOD biases of around +0.03 for Southern Africa and −0.01 for North America. Both simulations were not only able to reproduce the AOD magnitudes accurately, but also the inter-diurnal variations of smoke concentration. In addition, we made use of the airborne data from the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES; Southern Africa) and the Fire Influence on Regional to Global Environments Experiment and Air Quality (FIREX-AQ; North America) campaigns to evaluate the simulations. In Southern Africa, results showed correlations higher than 0.77 when comparing carbon monoxide and black carbon. In North America, correlations were lower and biases higher. However, this is because the model was not able to reproduce the timing, shape, and location of individual plumes over complex terrain (Rocky Mountains) during the FIREX-AQ campaign period.

Assimilation of S5P/TROPOMI carbon monoxide data with the global CAMS near-real-time system

Abstract. The Tropospheric Monitoring Instrument (TROPOMI) on the Copernicus Sentinel 5 Precursor (S5P) satellite, launched in October 2017, provides a wealth of atmospheric composition data, including total columns of carbon monoxide (TCCO) at high horizontal resolution (5.5 km × 7 km). Near-real-time TROPOMI TCCO data have been monitored in the global data assimilation system of the Copernicus Atmosphere Monitoring Service (CAMS) since November 2018 to assess the quality of the data. The CAMS system already routinely assimilates TCCO data from the Measurement of Pollution in the Troposphere (MOPITT) instrument and the Infrared Atmospheric Sounding Interferometer (IASI) outside the polar regions. The assimilation of TROPOMI TCCO data in the CAMS system was tested for the period 6 July to 31 December 2021, i.e. after the TROPOMI algorithm update to version 02.02.00 in July 2021. By assimilating TROPOMI TCCO observations, the CAMS CO columns increase by on average 8 %, resulting in an improved fit to independent observations (IAGOS aircraft profiles and NDACC Fourier transform infrared (FTIR) tropospheric and total-column CO data) compared to a version of the CAMS system where only TCCO from MOPITT and IASI is assimilated. The largest absolute and relative changes from the assimilation of TROPOMI CO are found in the lower and middle troposphere, i.e. that part of the atmosphere that is not already well constrained by the assimilated TIR MOPITT and IASI data. The largest impact near the surface comes from clear-sky TROPOMI data over land, and additional vertical information comes from the retrievals of measurements in cloudy conditions. July and August 2021 saw record numbers of boreal wildfires over North America and Russia, leading to large amounts of CO being released into the atmosphere. The paper assesses the impact of TROPOMI CO assimilation on selected CO plumes more closely. While the CO column can be well constrained by the assimilation of TROPOMI CO data, and the fit to individual IAGOS CO profiles in the lower and middle troposphere is considerably improved, the TROPOMI CO columns do not provide further constraints on individual plumes that are transported across continents and oceans at altitudes above 500 hPa.