Project description:Severe air pollution episodes have been frequent in China during the recent years. While high emissions are the primary reason for increasing pollutant concentrations, the ultimate cause for the most severe pollution episodes has remained unclear. Here we show that a high concentration of particulate matter (PM) will enhance the stability of an urban boundary layer, which in turn decreases the boundary layer height and consequently cause further increases in PM concentrations. We estimate the strength of this positive feedback mechanism by combining a new theoretical framework with ambient observations. We show that the feedback remains moderate at fine PM concentrations lower than about 200 μg m(-3), but that it becomes increasingly effective at higher PM loadings resulting from the combined effect of high surface PM emissions and massive secondary PM production within the boundary layer. Our analysis explains why air pollution episodes are particularly serious and severe in megacities and during the days when synoptic weather conditions stay constant.
Project description:Marine low clouds play an important role in the climate system, and their properties are sensitive to cloud condensation nuclei concentrations. While new particle formation represents a major source of cloud condensation nuclei globally, the prevailing view is that new particle formation rarely occurs in remote marine boundary layer over open oceans. Here we present evidence of the regular and frequent occurrence of new particle formation in the upper part of remote marine boundary layer following cold front passages. The new particle formation is facilitated by a combination of efficient removal of existing particles by precipitation, cold air temperatures, vertical transport of reactive gases from the ocean surface, and high actinic fluxes in a broken cloud field. The newly formed particles subsequently grow and contribute substantially to cloud condensation nuclei in the remote marine boundary layer and thereby impact marine low clouds.
Project description:Thermal turbulence is well known as a potent means to convey heat across space by a moving fluid. The existence of the boundary layers near the plates, however, bottlenecks its heat-exchange capability. Here, we conceptualize a mechanism of thermal vibrational turbulence that breaks through the boundary-layer limitation and achieves massive heat-transport enhancement. When horizontal vibration is applied to the convection cell, a strong shear is induced to the body of fluid near the conducting plates, which destabilizes thermal boundary layers, vigorously triggers the eruptions of thermal plumes, and leads to a heat-transport enhancement by up to 600%. We further reveal that such a vibration-induced shear can very efficiently disrupt the boundary layers. The present findings open a new avenue for research into heat transport and will also bring profound changes in many industrial applications where thermal flux through a fluid is involved and the mechanical vibration is usually inevitable.
Project description:The Kelvin-Helmholtz instability at the magnetospheric boundary plays a crucial role in solar wind-magnetosphere-ionosphere coupling, particle entry, and energization. The full extent of its impact has remained an open question due, in part, to global models without sufficient resolution to capture waves at higher latitudes. Using global magnetohydrodynamic simulations, we investigate an event when the Magnetospheric Multiscale (MMS) mission observed periodic low-frequency waves at the dawn-flank, high-latitude boundary layer. We show the layer to be unstable, even though the slow solar wind with the draped interplanetary magnetic field is seemingly unfavorable for wave generation. The simulated velocity shear at the boundary is thin ( ∼0.65RE ) and requires commensurately high spatial resolution. These results, together with MMS observations, confirm for the first time in fully three-dimensional global geometry that KH waves can grow in this region and thus can be an important process for energetic particle acceleration, dynamics, and transport.
Project description:The lifetime of reactive nitrogen and the production rate of reactive halogens in the marine boundary layer are strongly impacted by reactions occurring at aqueous interfaces. Despite the potential importance of the air-sea interface in serving as a reactive surface, few direct field observations are available to assess its impact on reactive nitrogen deposition and halogen activation. Here, we present direct measurements of the vertical fluxes of the reactant-product pair N2O5 and ClNO2 to assess the role of the ocean surface in the exchange of reactive nitrogen and halogens. We measure nocturnal N2O5 exchange velocities (Vex = -1.66 ± 0.60 cm s(-1)) that are limited by atmospheric transport of N2O5 to the air-sea interface. Surprisingly, vertical fluxes of ClNO2, the product of N2O5 reactive uptake to concentrated chloride containing surfaces, display net deposition, suggesting that elevated ClNO2 mixing ratios found in the marine boundary layer are sustained primarily by N2O5 reactions with aerosol particles. Comparison of measured deposition rates and in situ observations of N2O5 reactive uptake to aerosol particles indicates that N2O5 deposition to the ocean surface accounts for between 26% and 42% of the total loss rate. The combination of large Vex, N2O5 and net deposition of ClNO2 acts to limit NOx recycling rates and the production of Cl atoms by shortening the nocturnal lifetime of N2O5. These results indicate that air-sea exchange processes account for as much as 15% of nocturnal NOx removal in polluted coastal regions and can serve to reduce ClNO2 concentrations at sunrise by over 20%.
Project description:Long-term observations of the reactive chemical composition of the tropical marine boundary layer (MBL) are rare, despite its crucial role for the chemical stability of the atmosphere. Recent observations of reactive bromine species in the tropical MBL showed unexpectedly high levels that could potentially have an impact on the ozone budget. Uncertainties in the ozone budget are amplified by our poor understanding of the fate of NOx (= NO + NO2), particularly the importance of nighttime chemical NOx sinks. Here, we present year-round observations of the multiisotopic composition of atmospheric nitrate in the tropical MBL at the Cape Verde Atmospheric Observatory. We show that the observed oxygen isotope ratios of nitrate are compatible with nitrate formation chemistry, which includes the BrNO3 sink at a level of ca. 20 ± 10% of nitrate formation pathways. The results also suggest that the N2O5 pathway is a negligible NOx sink in this environment. Observations further indicate a possible link between the NO2/NOx ratio and the nitrogen isotopic content of nitrate in this low NOx environment, possibly reflecting the seasonal change in the photochemical equilibrium among NOx species. This study demonstrates the relevance of using the stable isotopes of oxygen and nitrogen of atmospheric nitrate in association with concentration measurements to identify and constrain chemical processes occurring in the MBL.
Project description:The sediments within fjords are critical components of the mid- to high-latitude coastal carbon (C) cycle, trapping and storing more organic carbon (OC) per unit area than other marine sedimentary environments. Located at the land-ocean transition, fjord sediments receive OC from both marine and terrestrial environments; globally, it has been estimated that 55%-62% of the OC held within modern fjord sediments originates from terrestrial environments. However, the mid-latitude fjords of the Northern Hemisphere have largely been omitted from these global compilations. Here we investigate the mechanism driving the distribution of OC originating from different sources within the sediments of 38 Scottish fjords. From an array of fjord characteristics, the tidal range and outer sill depth were identified as the main drivers governing the proportions of marine and terrestrial OC in the sediments. Utilizing this relationship, we estimate that on average 52% ± 10% of the OC held within the sediments of all Scotland's fjords is terrestrial in origin. These findings show that the Scottish fjords hold equivalent quantities of terrestrial OC as other global fjord systems. However, the analysis also highlights that the sediments within 29% of Scottish fjords are dominated by marine derived OC, which is driven by local fjord geomorphology and oceanography.
Project description:Summertime Arctic shipboard observations of oxygenated volatile organic compounds (OVOCs) such as organic acids, key precursors of climatically active secondary organic aerosol (SOA), are consistent with a novel source of OVOCs to the marine boundary layer via chemistry at the sea surface microlayer. Although this source has been studied in a laboratory setting, organic acid emissions from the sea surface microlayer have not previously been observed in ambient marine environments. Correlations between measurements of OVOCs, including high levels of formic acid, in the atmosphere (measured by an online high-resolution time-of-flight mass spectrometer) and dissolved organic matter in the ocean point to a marine source for the measured OVOCs. That this source is photomediated is indicated by correlations between the diurnal cycles of the OVOC measurements and solar radiation. In contrast, the OVOCs do not correlate with levels of isoprene, monoterpenes, or dimethyl sulfide. Results from box model calculations are consistent with heterogeneous chemistry as the source of the measured OVOCs. As sea ice retreats and dissolved organic carbon inputs to the Arctic increase, the impact of this source on the summer Arctic atmosphere is likely to increase. Globally, this source should be assessed in other marine environments to quantify its impact on OVOC and SOA burdens in the atmosphere, and ultimately on climate.
Project description:Heterogeneous uptake of hypoiodous acid (HOI), the dominant inorganic iodine species in the marine boundary layer (MBL), on sea-salt aerosol (SSA) to form iodine monobromide and iodine monochloride has been adopted in models with assumed efficiency. Recently, field measurements have reported a much faster rate of this recycling process than previously assumed in models. Here, we conduct global model simulations to quantify the range of effects of iodine recycling within the MBL, using Conventional, Updated, and Upper-limit coefficients. When considering the Updated coefficient, iodine recycling significantly enhances gaseous inorganic iodine abundance (∼40%), increases halogen atom production rates (∼40% in I, >100% in Br, and ∼60% in Cl), and reduces oxidant levels (-7% in O3, -2% in OH, and -4% in HO2) compared to the simulation without the process. We appeal for further direct measurements of iodine species, laboratory experiments on the controlling factors, and multiscale simulations of iodine heterogeneous recycling.
Project description:After the 2020 Lunar New Year, the Chinese government implemented a strict nationwide lockdown to inhibit the spread of the Coronavirus Disease 2019 (COVID-19). Despite the abrupt decreases in gaseous emissions caused by record-low anthropogenic activities, severe haze pollution occurred in northern China during the COVID lockdown. This paradox has attracted the attention of both the public and the scientific community. By analyzing comprehensive measurements of air pollutants, planetary boundary layer (PBL) height, and surface meteorology, we show that the severe air pollution episode over northern China coincided with the abnormally low PBL height, which had reduced by 45%, triggering strong aerosol-PBL interactions. After dynamical processes initiated the temperature inversion, the Beijing metropolitan area experienced a period with continuously shallow PBLs during the lockdown. This unprecedented event provided an experiment showcasing the role of meteorology, in particular aerosol-PBL interactions in affecting air quality.