Significant Vertical Difference in Aerosol Chemistry Within Urban Boundary Layer Triggered by Cold‐Air Pool: Insights From Simultaneous Mountain‐Valley Measurements

Impact of aerosol-boundary layer interactions on PM2.5 pollution during cold air pool events in a semi-arid urban basin

Cold-air pooling is an important topoclimatic process that creates temperature inversions with the coldest air at the lowest elevations. Incomplete understanding of sub-canopy spatiotemporal cold-air pooling dynamics and associated ecological impacts hinders predictions and conservation actions related to climate change and cold-dependent species and functions. To determine if and how cold-air pooling influences forest composition, we characterized the frequency, strength, and temporal dynamics of cold-air pooling in the sub-canopy at local to regional scales in New England, USA. We established a network of 48 plots along elevational transects and continuously measured sub-canopy air temperatures for 6-10 months (depending on site). We then estimated overstory and understory community temperature preferences by surveying tree composition in each plot and combining these data with known species temperature preferences. We found that cold-air pooling was frequent (19-43% seasonal occurrences) and that sites with the most frequent inversions displayed inverted forest composition patterns across slopes with more cold-adapted species, namely conifers, at low instead of high elevations. We also observed both local and regional variability in cold-air pooling dynamics, revealing that while cold-air pooling is common, it is also spatially complex. Our study, which uniquely focused on broad spatial and temporal scales, has revealed some rarely reported cold-air pooling dynamics. For instance, we discovered frequent and strong temperature inversions that occurred across seasons and in some locations were most frequent during the daytime, likely affecting forest composition. Together, our results show that cold-air pooling is a fundamental ecological process that requires integration into modeling efforts predicting future forest vegetation patterns under climate change, as well as greater consideration for conservation strategies identifying potential climate refugia for cold-adapted species.

This overview summarizes the objectives of the Aerosol Characterization Experiments (ACEs) of the International Global Atmospheric Chemistry (IGAC) project and the research strategy implemented in the second of this series of experiments (ACE-2). ACE-2 took place from 16 June to 24 July 1997, over the sub-tropical North-East Atlantic. It provided an opportunity to study the properties, processes and effects of contrasting aerosol types in this region, including background marine and anthropogenic pollution aerosol in the marine boundary layer (MBL), and background aerosol and mineral dust in the overlaying free troposphere (FT). The major achievements of ACE-2 include:(a) identification of entrainment, in-cloud scavenging and coagulation as the major processes transforming a pollution aerosol transported within the MBL; (b) the first documentation of the indirect radiative effect of aerosols at the scale of a cloud ensemble in continental pollution outflow; (c) observation of a wide range in the contribution of organic material to the sub-micron aerosol mass, with possibly the highest contribution in the free tropospheric; (d) improved understanding of the role of condensing HCl, HNO3 and NH3 as a growth mechanism of sub-micron aerosols in polluted air masses advecting over the ocean. A close connection was observed between meteorological factors (such as horizontal and vertical wind speed, boundary layer development, entrainment, humidity fields) and aerosol and cloud characteristics. In the ACE-2 region, these meteorological factors, rather than aerosol microphysics and chemistry, often dominated the shaping of the aerosol size distribution and/or their effect on radiation and clouds. The ACE-2 data presently analyzed provide a qualitative, and in many cases a quantitative understanding of the complex gas/aerosol/cloud system in the sub-tropical marine environment. This will guide future model development. Some major data sets are still to be analyzed.

Some of the world’s valleys are famous for having particularly cold microclimates. The La Brevine valley, in the Swiss Jura Mountains, holds the record for the lowest temperature ever measured in an inhabited location in Switzerland. We studied cold air pools (CAPs) in this valley during the winter of 2014–2015 using 44 temperature data loggers distributed between 1033 and 1293 m asl. Our goals were to (i) describe the climatic conditions under which CAPs form in the valley, (ii) examine the spatial configuration and the temperature structure of the CAPs and (iii) quantify how often temperature inversions occur in winter using long-term series of temperature from the valley floor. Our results show that CAPs occurred every second night, on average, during the winter of 2014–2015 and were typically formed under cloudless, windless and high-pressure conditions. Strong temperature inversions up to 28 °C were detected between the valley floor and the surrounding hills. The spatial temperature structure of the CAPs varies among the different inversion days, with the upper boundary of the cold pool generally situated at about 1150 m asl. Although mean temperatures have increased in this area over the period 1960–2015 in connection with climate change, the occurrences of extreme cold temperatures did not decrease in winter and are highly correlated with the North Atlantic Oscillation and the East Atlantic indices. This suggests that CAPs in sheltered valleys are largely decoupled from the free atmosphere temperature and will likely continue to occur in the next decades under warmer conditions.

The main aim of this paper is to explore the potential of combining measurements from fixed- and rotary-wing remotely piloted aircraft systems (RPAS) to complement data sets from radio soundings as well as ship and sea-ice-based instrumentation for atmospheric boundary layer (ABL) profiling. This study represents a proof-of-concept of RPAS observations in the Antarctic sea-ice zone. We present first results from the RV Polarstern Antarctic winter expedition in the Weddell Sea in June–August 2013, during which three RPAS were operated to measure temperature, humidity and wind; a fixed-wing small unmanned meteorological observer (SUMO), a fixed-wing meteorological mini-aerial vehicle, and an advanced mission and operation research quadcopter. A total of 86 RPAS flights showed a strongly varying ABL structure ranging from slightly unstable temperature stratification near the surface to conditions with strong surface-based temperature inversions. The RPAS observations supplement the regular upper air soundings and standard meteorological measurements made during the campaign. The SUMO and quadcopter temperature profiles agree very well and, excluding cases with strong temperature inversions, 70% of the variance in the difference between the SUMO and quadcopter temperature profiles can be explained by natural, temporal, temperature fluctuations. Strong temperature inversions cause the largest differences, which are induced by SUMO’s high climb rates and slow sensor response. Under such conditions, the quadcopter, with its slower climb rate and faster sensor, is very useful in obtaining accurate temperature profiles in the lowest 100 m above the sea ice. Keywords: Remotely piloted aircraft systems; unmanned aerial vehicles; Weddell Sea; polar meteorology; Antarctic; boundary layer meteorology. (Published: 8 October 2015) To access the supplementary material for this article, please see supplementary files in the column to the right (under Article Tools). Citation: Polar Research 2015, 34 , 25651, http://dx.doi.org/10.3402/polar.v34.25651

The interactions of aerosols and planetary boundary layer and its critical impacts on environment, weather and climate is a hot issue in the atmospheric environment field at present. The coupled chemical–boundary interactions that drive severe haze events are less understood due to the limited comprehensive vertical measurements，especially for valley cities, in which the formation and development of haze pollution are more complicated and unique. High ozone concentrations promote the formation of nitrate in the nocturnal residual layer, but this phenomenon has not been confirmed and quantified by direct observation. Here, gaseous pollutants, water-soluble ions in PM2.5 and meteorological factors were simultaneously observed in the stable boundary layer (SBL), residual layer (RL) and mixing layer (ML) in a typical valley city in Northern China. Strong photochemical formation was found in the upper ML during the daytime. At night, nitrate formation was weak due to poor reaction conditions with low ozone and relative humidity (RH) in the SBL near ground level. However, enhanced reaction conditions were observed in the RL, which was associated with the increased precursors transported by the upward valley breeze during the daytime and the increased humidity caused by the temperature reduction; the increased relative humidity and precursors in turn promoted nitrate formation. The mixing down of nitrate from the RL contributes 70% of the surface-level nitrate in the next morning. This vertical feedback, together with the pollutant-trapped terrain, constitutes a key mechanism that links boundary evolution, mountain-valley breeze and nitrate formation in the valley city. This mechanism is self-amplifying, leading to faster chemical production, accumulation, and more severe haze pollution，which was significant to air quality in the valley or basin cities in the world.

The effect of cross-scale modulation of synoptic systems by the cold air pool on autumn nighttime rainfall over Hainan Island

Air quality in China has been continuously improved since the implementation of “Atmospheric Pollution Prevention and Control Action Plan” in 2013. However, the mass concentrations of fine particles particularly in Beijing, Tianjin and Hebei are still much higher than the National Ambient Air Quality Standard (35 μg m−3 as an annual average), and severely polluted events also occur occasionally in autumn and winter seasons. In recent years, Chinese research scientists have made significant progresses in vertical measurements of air pollution, formation mechanisms and source apportionment of atmospheric aerosol, and also the interactions between aerosol and atmospheric boundary layer, which greatly support the scientific prevention and control of atmospheric pollution. Despite this, many questions on atmospheric pollution have not been well addressed yet. This paper first summarizes the recent research progresses in vertical measurements of air pollution in China, in particular, the measurements from the research platform of the Beijing 325 m meteorological tower. In addition to the routine long-term measurements of boundary layer (turbulence, CO2 and H2O flux) and meteorological parameters (temperature, relative humidity, wind speed and wind direction) at 7 and 15 heights, respectively, this platform can have simultaneous real-time measurements of aerosol particle composition (organics, sulfate, nitrate, ammonium, chloride, and black carbon), gaseous species (CO, SO2, and O3), particle number size distributions, and optical properties (extinction and absorption coefficients) at ground level and 260 m, and also the continuously vertical measurements from ground to 260 m using the tower container equipped with specific instruments. Then, the vertical differences of aerosol composition in different seasons in Beijing, and their interactions with boundary layer are discussed. Also, the response of aerosol chemistry to regional source emission control are elucidated based on vertical measurements during the Asia-Pacific Economic Conference (APEC) summit in 2014 and the 70th anniversary parade in 2015. This paper also reviews the latest research progress on formation mechanisms of secondary inorganic aerosol (nitrate and sulfate) and secondary organic aerosol, and the life cycles of severe haze events in China. In particular, the heterogeneous formation of sulfate during severe haze episodes strongly depends on pH values of aerosol liquid water content. While techniques for direct measurements of aerosol particle pH are essential yet challenging, laboratory experiments are more needed now to prove the hypothesis of sulfate formation mechanisms. Compared with inorganic species, the formation and evolutionary mechanisms of secondary organic aerosol (SOA) are far more complex in polluted environments, and their roles in haze formation need to be better characterized. Finally, this paper lists some future recommendations for air pollution measurements (e.g., from long-term to vertical measurements in terms of significant emission changes in the near future), formation mechanism of secondary aerosol, and molecular composition and physical and chemical properties (phase, volatility, oxidation state, etc.) of organic aerosol.

Alpine valleys are rarely closed systems, implying that the atmospheric boundary layer of a particular valley is influenced by the surrounding terrain and large-scale flows. A detailed characterisation and quantification of these effects is required in order to design appropriate parameterisation schemes for complex terrains. The focus of this work is to improve the understanding of the effects of surrounding terrain (plains, valleys or tributaries) on the heat and mass budgets of the stable boundary layer of a valley, under dry and weak large-scale wind conditions. Numerical simulations using idealised and real frameworks are performed to meet this goal. Several idealised terrains (configurations) were considered: an infinitely long valley (i.e. two-dimensional), and upstream valleys opening either on a plain (valley-plain), on a wider valley (draining) or on a narrower valley (pooling). In three-dimensional valleys, two main regimes can be identified for all configurations: a transient regime, before the down-valley flow develops, followed by a quasi-steady regime, when the down-valley flow is fully developed. The presence of a downstream valley reduces the along-valley temperature difference, therefore leading to weaker down-valley flows. As a result, the duration of the transient regime increases compared to the respective valley-plain configuration. Its duration is longest for pooling configuration. For strong pooling the along-valley temperature difference can reverse, forcing up-valley flows from the narrower towards the wider valley. In this regime, the volume-averaged cooling rate is found maximum and its magnitude dependent on the configuration considered. Therefore pooling and draining induce colder and deeper boundary layers than the respective valley-plain configurations. In the quasi-steady regime the cooling rate is smaller than in the transient regime, and almost independent of the configuration considered. Indeed, as the pooling character is more pronounced, the warming contribution from advection to the heat budget decreases because of weaker down-valley flows, and so does the cooling contribution from the surface sensible heat flux. The mass budget of the valley boundary layer was found to be controlled by a balance between the convergence of downslope flows at the boundary layer top and the divergence of down-valley flows along the valley axis, with negligible contributions of subsidence far from the slopes. The mass budget highlighted the importance of the return current above the down-valley flow, which may contribute significantly to the inflow of air at the top of the boundary layer. A case-study of a persistent cold-air pool event which occurred in February 2015 in the Arve River Valley during the intensive observation period 1 of the PASSY-2015 field campaign, allowed to quantify the effects of neighbouring valleys on the heat and mass budgets of a real valley atmosphere. The cold-air pool persisted because of warm air advection at the valley top, associated with the passage of an upper-level ridge over Europe. The contributions from each tributary valley to the mass and heat budgets of the valley atmosphere were found to vary from day to day within the persistent stage of the cold-air pool, depending on the large-scale flow. Tributary flows had significant impact on the height of the inversion layer and the strength of the cold-air pool, transporting a significant amount of mass within the valley atmosphere throughout the night. The strong stratification of the near-surface atmosphere prevented the tributary flows from penetrating down to the valley floor. The evolution of the large-scale flow during the episode had a profound impact on the near-surface circulation of the valley. The channelling of the large-scale flow at night, can lead to the decrease of the horizontal temperature difference driving the near-surface down-valley flow, favouring the stagnation of the air close to the ground.

It has long been known that the urban surface energy balance is different to that of a rural surface, and that heating of the urban surface after sunset gives rise to the Urban Heat Island (UHI). Less well known is how flow and turbulence structure above the urban surface are changed during different phases of the urban boundary layer (UBL). This paper presents new observations above both an urban and rural surface and investigates how much UBL structure deviates from classical behaviour. A 5-day, low wind, cloudless, high pressure period over London, UK, was chosen for analysis, during which there was a strong UHI. Boundary layer evolution for both sites was determined by the diurnal cycle in sensible heat flux, with an extended decay period of approximately 4 h for the convective UBL. This is referred to as the “Urban Convective Island” as the surrounding rural area was already stable at this time. Mixing height magnitude depended on the combination of regional temperature profiles and surface temperature. Given the daytime UHI intensity of \(1.5\,^\circ \mathrm{C}\), combined with multiple inversions in the temperature profile, urban and rural mixing heights underwent opposite trends over the period, resulting in a factor of three height difference by the fifth day. Nocturnal jets undergoing inertial oscillations were observed aloft in the urban wind profile as soon as the rural boundary layer became stable: clear jet maxima over the urban surface only emerged once the UBL had become stable. This was due to mixing during the Urban Convective Island reducing shear. Analysis of turbulent moments (variance, skewness and kurtosis) showed “upside-down” boundary layer characteristics on some mornings during initial rapid growth of the convective UBL. During the “Urban Convective Island” phase, turbulence structure still resembled a classical convective boundary layer but with some influence from shear aloft, depending on jet strength. These results demonstrate that appropriate choice of Doppler lidar scan patterns can give detailed profiles of UBL flow. Insights drawn from the observations have implications for accuracy of boundary conditions when simulating urban flow and dispersion, as the UBL is clearly the result of processes driven not only by local surface conditions but also regional atmospheric structure.

<p><strong>Abstract.</strong> The vertical distribution in the physical and chemical properties of submicron aerosol has been characterised across northern India for the first time using airborne in situ measurements. This study focusses primarily on the Indo-Gangetic Plain, a low-lying area in the north of India which commonly experiences high aerosol mass concentrations prior to the monsoon season. Data presented are from the UK Facility for Airborne Atmospheric Measurements BAe-146 research aircraft that performed flights in the region during the 2016 pre-monsoon (11 and 12 June) and monsoon (30 June to 11 July) seasons.</p> <p>Inside the Indo-Gangetic Plain boundary layer, organic matter dominated the submicron aerosol mass (43 %) followed by sulfate (29 %), ammonium (14 %), nitrate (7 %) and black carbon (7 %). However, outside the Indo-Gangetic Plain, sulfate was the dominant species, contributing 44 % to the total submicron aerosol mass in the boundary layer, followed by organic matter (30 %), ammonium (14 %), nitrate (6 %) and black carbon (6 %). Chlorine mass concentrations were negligible throughout the campaign. Black carbon mass concentrations were higher inside the Indo-Gangetic Plain (2 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>) compared to outside (1 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>). Nitrate appeared to be controlled by thermodynamic processes, with increased mass concentration in conditions of lower temperature and higher relative humidity. Increased mass and number concentrations were observed inside the Indo-Gangetic Plain and the aerosol was more absorbing in this region, whereas outside the Indo-Gangetic Plain the aerosol was larger in size and more scattered in nature, suggesting greater dust presence, especially in north-western India. The aerosol composition remained largely similar as the monsoon season progressed, but the total aerosol mass concentrations decreased by <span class="inline-formula">∼50</span> % as the rainfall arrived; the pre-monsoon average total mass concentration was 30 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span> compared to a monsoon average total mass concentration of 10–20 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>. However, this mass concentration decrease was less noteworthy (<span class="inline-formula">∼20</span> %–30 %) over the Indo-Gangetic Plain, likely due to the strength of emission sources in this region. Decreases occurred in coarse mode aerosol, with the fine mode fraction increasing with monsoon arrival. In the aerosol vertical profile, inside the Indo-Gangetic Plain during the pre-monsoon, organic aerosol and absorbing aerosol species dominated in the lower atmosphere (<span class="inline-formula"><1.5</span> km), with sulfate, dust and other scattering aerosol species enhanced in an elevated aerosol layer above 1.5 km with maximum aerosol height <span class="inline-formula">∼6</span> km. The elevated concentration of dust at altitudes <span class="inline-formula">>1.5</span> km is<span id="page5616"/> a clear indication of dust transport from the Great Indian Desert, also called the Thar Desert, in north-western India. As the monsoon progressed into this region, the elevated aerosol layer diminished, the aerosol maximum height reduced to <span class="inline-formula">∼2</span> km. The dust and sulfate-dominated aerosol layer aloft was removed upon monsoon arrival, highlighted by an increase in fine mode fraction throughout the profile.</p>

Wintertime cold air pools (CAPs) are common across the Western United States and result in cold, dense air trapped in valley basins. The CAPs are characterized by a stable atmospheric boundary layer, leading to cold air and low wind speeds. While CAP formation occurs nightly, the CAP conditions can persist into daytime and often last for multiple days (i.e., persistent cold air pool or PCAP), resulting in poor air quality in populated areas. The presence and strength of CAPs can be calculated using data from radiosondes, surface weather stations at varying elevations, and indirectly through air pollution monitors. Because vertical profile data are often limited to twice daily radiosondes, and are spatially sparse, numerical models can be a useful substitute. This work uses the European Centre for Medium-Range Weather Forecasts (ECMWFs) Reanalysis v5 (ERA) atmospheric reanalysis to provide data to classify wintertime CAP events without radiosonde observations. An automated CAP classification method using ERA outputs is evaluated using afternoon radiosonde observations in six cities (Salt Lake City, Utah; Reno, Nevada; Boise, Idaho; Denver, Colorado; Las Vegas, Nevada; Medford, and Oregon). Using this CAP determination method, days with CAP events are analyzed in 13 locations, 6 with radiosonde observations and 7 without, including the Central valley of California. The CAP classification method is evaluated at these 13 locations across the Western US over the study period of 2000–2022. The results show that the ERA model performs similarly to the radiosonde observations when used to identify CAP events. Therefore, ERA can be used to provide a reasonable estimate of CAP conditions when radiosonde data are unavailable. Providing consistent CAP classifications across space and time are necessary for regional scale CAP studies, such as human health effects modeling over large spatial and temporal scales.

The chemical composition of nonrefractory submicron aerosol particles was measured at the Puy‐de‐Dôme (PUY) station (1,465 m a.s.l) during 2015 using a Time‐of‐Flight Aerosol Chemical Speciation Monitor (ToF‐ACSM). These aerosol chemistry measurements are combined with online black carbon (BC) measurements to provide an overview of the submicron aerosol composition. Averaged over the entire year, and normalized to standard temperature and pressure, organic aerosol (OA) dominates the PM1 concentration during all seasons and within all air mass types (2.12 ± 1.73 µgm−3), and is responsible for summertime increases in aerosol concentration. Highest mass concentrations were measured during the summer, when air masses were arriving over mainland Europe and lowest in the winter months (when most air masses were of Atlantic origin). OA source apportionment was performed separately during each season, using the Source Finder (SoFi) interface for the multilinear engine. The PUY site, situated at 1,465 m a.s.l, although mainly sampling in the atmospheric boundary layer, it is sometimes sampling in the lower free troposphere (FT), providing the opportunity to identify the characteristics of FT aerosol. In order to accurately identify these sampling periods, the methodology described in Farah et al. (2018), during the same time period (2015/2016), was applied to the data. During this period, FT air masses are sampled approximately 20% of the time. This work provides, on one hand, a description of long‐term aerosol chemical properties at a remote regional site in central Europe and, on the other hand a characteristic chemical signature of FT aerosols over this region. This data can be used to improve our understanding of the transport and aging properties of aerosols at regional observation sites.

Abstract. Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environments against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce the plume structure and location fairly well both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirm the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicates that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated by about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%), and inorganic aerosol fraction (40%) including nitrate (8%), sulfate (22%) and ammonium (10%). The secondary organic aerosols (SOA) represent 12% of the total aerosol mass, while the mineral dust accounts for 8%. The comparison demonstrates the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However, for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given.

Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.