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Turbulence vertical structure of the boundary layer during the afternoon transition

We investigate the decay of planetary boundary layer (PBL) turbulence in the afternoon, from the time the surface buoyancy flux starts to decrease until sunset. Dense observations of mean and turbulent parameters were acquired during the Boundary Layer Late Afternoon and Sunset Turbulence (BLLAST) field experiment by several meteorological surface stations, sounding balloons, radars, lidars and two aircraft during the afternoon transition. We analysed a case study based on some of these observations and large-eddy simulation (LES) data focusing on the turbulent vertical structure throughout the afternoon transition. The decay of turbulence is quantified through the temporal and vertical evolution of (1) the turbulence kinetic energy (TKE), (2) the characteristic length scales of turbulence and (3) the shape of the turbulence spectra. A spectral analysis of LES data, airborne and surface measurements is performed in order to characterize the variation in the turbulent decay with height and study the distribution of turbulence over eddy size. This study highlights the LES ability to reproduce the turbulence evolution throughout the afternoon. LESs and observations agree that the afternoon transition can be divided in two phases: (1) a first phase during which the TKE decays at a low rate, with no significant change in turbulence characteristics, and (2) a second phase characterized by a larger TKE decay rate and a change in spectral shape, implying an evolution of eddy size distribution and energy cascade from low to high wave number. The changes observed either in TKE decay (during the first phase) or in the vertical wind spectra shape (during the second phase of the afternoon transition) occur first in the upper region of the PBL. The higher within the PBL, the stronger the spectra shape changes.
Black carbon concentrations and mixing state in the Finnish Arctic

Atmospheric aerosol composition was measured using a Single Particle Soot Photometer (SP2) in the Finnish Arctic during winter 2011–2012. The Sammaltunturi measurement site at the Pallas GAW (Global Atmosphere Watch) station receives air masses from different source regions including the Arctic Ocean and continental Europe. The SP2 provides detailed information about mass distributions and mixing state of refractory black carbon (rBC). The measurements showed widely varying rBC mass concentrations (0–120 ng m−3), which were related to varying contributions of different source regions and aerosol removal processes. The rBC mass was log-normally distributed showing a relatively constant rBC core mass mean diameter with an average of 194 nm (75–655 nm sizing range). On average, the number fraction of particles containing rBC was 0.24 (integrated over 350–450 nm particle diameter range) and the average particle diameter to rBC core volume equivalent diameter ratio was 2.0 (averaged over particles with 150–200 nm rBC core volume equivalent diameters). These average numbers mean that the observed rBC core mass mean diameter is similar to those of aged particles, but the observed particles seem to have unusually high particle to rBC core diameter ratios. Comparison of the measured rBC mass concentration with that of the optically detected equivalent black carbon (eBC) using an Aethalometer and a MAAP showed that eBC was larger by a factor of five. The difference could not be fully explained without assuming that only a part of the optically detected light absorbing material is refractory and absorbs light at the wavelength used by the SP2. Finally, climate implications of five different black carbon mixing state representations were compared using the Mie approximation and simple direct radiative forcing efficiency calculations. These calculations showed that the observed mixing state means significantly lower warming effect or even a net cooling effect when compared with that of a homogenous aerosol containing the same amounts of black carbon and non-absorbing material.
Long-term real-time measurements of aerosol particle composition in Beijing, China: seasonal variations, meteorological effects, and source analysis

High concentrations of fine particles (PM2.5) are frequently observed during all seasons in Beijing, China, leading to severe air pollution and human health problems in this megacity. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) species (sulfate, nitrate, ammonium, chloride, and organics) in Beijing using an Aerodyne Aerosol Chemical Speciation Monitor for 1 year, from July 2011 to June 2012. This is the first long-term, highly time-resolved (~ 15 min) measurement of fine particle composition in China. The seasonal average (±1σ) mass concentration of NR-PM1 ranged from 52 (±49) μg m−3 in the spring season to 62 (±49) μg m−3 in the summer season, with organics being the major fraction (40–51 %), followed by nitrate (17–25 %) and sulfate (12–17 %). Organics and chloride showed pronounced seasonal variations, with much higher concentrations in winter than in the other seasons, due to enhanced coal combustion emissions. Although the seasonal variations of secondary inorganic aerosol (SIA, i.e., sulfate + nitrate + ammonium) concentrations were not significant, higher contributions of SIA were observed in summer (57–61 %) than in winter (43–46 %), indicating that secondary aerosol production is a more important process than primary emissions in summer. Organics presented pronounced diurnal cycles that were similar among all seasons, whereas the diurnal variations of nitrate were mainly due to the competition between photochemical production and gas–particle partitioning. Our data also indicate that high concentrations of NR-PM1 (> 60 μg m−3) are usually associated with high ambient relative humidity (RH) (> 50 %) and that severe particulate pollution is characterized by different aerosol composition in different seasons. All NR-PM1 species showed evident concentration gradients as a function of wind direction, generally with higher values associated with wind from the south, southeast or east. This was consistent with their higher potential as source areas, as determined by potential source contribution function analysis. A common high potential source area, located to the southwest of Beijing along the Taihang Mountains, was observed during all seasons except winter, when smaller source areas were found. These results demonstrate a high potential impact of regional transport from surrounding regions on the formation of severe haze pollution in Beijing.
Airborne measurements of new particle formation in the free troposphere above the Mediterranean Sea during the HYMEX campaign

While atmospheric new particle formation (NPF) has been observed in various environments and was found to contribute significantly to the total aerosol particle concentration, the production of new particles over open seas is poorly documented in the literature. Nucleation events were detected and analysed over the Mediterranean Sea using two condensation particle counters and a scanning mobility particle sizer on board the ATR-42 research aircraft during flights conducted between 11 September and 4 November 2012 in the framework of the HYMEX (HYdrological cycle in Mediterranean EXperiment) project. The main purpose of the present work was to characterize the spatial extent of the NPF process, both horizontally and vertically. Our findings show that nucleation is occurring over large areas above the Mediterranean Sea in all air mass types. Maximum concentrations of particles in the size range 5–10 nm (N5–10) do not systematically coincide with lower fetches (time spent by the air mass over the sea before sampling), and significant N5–10 values are found for fetches between 0 and 60 h depending on the air mass type. These observations suggest that nucleation events could be more influenced by local precursors originating from emission processes occurring above the sea, rather than linked to synoptic history. Vertical soundings were performed, giving the opportunity to examine profiles of the N5–10 concentration and to analyse the vertical extent of NPF. Our observations demonstrate that the process could be favoured above 1000 m, i.e. frequently in the free troposphere, and more especially between 2000 and 3000 m, where the NPF frequency is close to 50 %. This vertical distribution of NPF might be favoured by the gradients of several atmospheric parameters, together with the mixing of two air parcels, which could also explain the occurrence of the process at preferential altitudes. In addition, increased condensation sinks collocated with high concentrations of small particles suggest the occurrence of NPF events promoted by inputs from the boundary layer, most probably associated with convective clouds and their outflow. After their formation, particles slowly grow at higher altitudes to diameters of at least 30 nm while not being greatly depleted or affected by coagulation. Our analysis of the particle size distributions suggests that particle growth could decrease with increasing altitude.
Deuterium excess in the atmospheric water vapour of a Mediterranean coastal wetland: regional vs. local signatures

Stable isotopes of water vapour represent a powerful tool for tracing atmospheric vapour origin and mixing processes. Laser spectrometry recently allowed high time-resolution measurements, but despite an increasing number of experimental studies, there is still a need for a better understanding of the isotopic signal variability at different time scales. We present results of in situ measurements of δ18O and δD during 36 consecutive days in summer 2011 in atmospheric vapour of a Mediterranean coastal wetland exposed to high evaporation (Camargue, Rhône River delta, France). The mean composition of atmospheric vapour (δv) is δ18O = −14.66 &permil; and δD = − 95.4 &permil;, with data plotting clearly above the local meteoric water line on a δ18O-δD plot, and an average deuterium excess (d) of 21.9 &permil;. Important diurnal d variations are observed, and an hourly time scale analysis is necessary to interpret the main processes involved in its variability. After having classified the data according to air mass back trajectories, we analyse the average daily cycles relating to the two main meteorological situations, i.e. air masses originating from North Atlantic Ocean and Mediterranean Sea. In both situations, we show that diurnal fluctuations are driven by (1) the influence of local evaporation, culminating during daytime, and leading to an increase in absolute water vapour concentration associated to a δv enrichment and d increase; (2) vertical air mass redistribution when the Planetary Boundary Layer collapses in the evening, leading to a d decrease, and (3) dew formation during the night, producing a δv depletion with d remaining stable. Using a two-component mixing model, we calculate the average composition of the locally evaporated vapour (δE). We find higher d(E) under North Atlantic air mass conditions, which is consistent with lower humidity conditions. We also suggest that δv measured when the PBL collapses is the most representative of a regional signal. Strong, cold and dry winds coming from the north bring an isotopically depleted vapour, while light, warm and wet winds coming from the south bring an isotopically enriched vapour. Under northern conditions, a strong advection rate dilutes the contribution of the locally evaporated vapour (δE) to the ambient moisture (δv). The higher d values measured under northern conditions, compared to the Mediterranean situation, thus results from the combination of a higher d in both local and regional vapour. This depiction of typical daily cycles of water vapour isotopic composition can be used as a framework for further quantitative analyses of vapour sources during specific days.
In situ formation and spatial variability of particle number concentration in a European megacity

Ambient particle number size distributions were measured in Paris, France, during summer (1–31 July 2009) and winter (15 January to 15 February 2010) at three fixed ground sites and using two mobile laboratories and one airplane. The campaigns were part of the Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation (MEGAPOLI) project. New particle formation (NPF) was observed only during summer on approximately 50 % of the campaign days, assisted by the low condensation sink (about 10.7 ± 5.9 × 10−3 s−1). NPF events inside the Paris plume were also observed at 600 m altitude onboard an aircraft simultaneously with regional events identified on the ground. Increased particle number concentrations were measured aloft also outside of the Paris plume at the same altitude, and were attributed to NPF. The Paris plume was identified, based on increased particle number and black carbon concentration, up to 200 km away from the Paris center during summer. The number concentration of particles with diameters exceeding 2.5 nm measured on the surface at the Paris center was on average 6.9 ± 8.7 × 104 and 12.1 ± 8.6 × 104 cm−3 during summer and winter, respectively, and was found to decrease exponentially with distance from Paris. However, further than 30 km from the city center, the particle number concentration at the surface was similar during both campaigns. During summer, one suburban site in the NE was not significantly affected by Paris emissions due to higher background number concentrations, while the particle number concentration at the second suburban site in the SW increased by a factor of 3 when it was downwind of Paris.
Towards a first classification of aerosol shrinkage events

This work presents for the first time a classification of shrinkage events based on the aerosol processes that precede them. To this end, 3.5 years of continuous measurements (from 2009 to 2012) of aerosol size distributions, obtained with a Scanning Mobility Particle Sizer (SMPS) at an urban background site in Southern Europe, have been interpreted. 48 shrinkage events were identified and analysed, all occurring during spring and summer when the atmospheric conditions are more favourable for their development. In this study the shrinkage events took place mostly towards the end of the day, and their occurrence could be associated to atmospheric dilution conditions and a reduction in photochemical activity. The shrinkage rate (SR) varied between −1.0 and −11.1 nm h−1 (average value of −4.7 ± 2.6 nm h−1). Changes in particle concentrations corresponding to the nucleation and Aitken modes were detected, whereby an increase in the number of particles in the nucleation mode often coincided with a reduction in the Aitken mode. The accumulation mode did not undergo significant changes during these processes. In addition, in some cases, a dilution of the total particle number concentration in the ambient air was observed. Following the proposed methodology, three groups of events have been identified: Group I (NPF + shrinkage), Group II (aerosol growth process + shrinkage) and Group III (pure shrinkage events). The largest number of shrinkage events has been observed in the absence of prior processes, i.e. pure shrinkage events, followed by Group I events and finally Group II events. Although this analysis has confirmed that the triggering of shrinkage events is clearly linked to the atmospheric situation and the characteristics of the measurement area, this classification may contribute to a better understanding of the processes involved and the features that characterize shrinkage events.
Effect of tropical cyclones on the tropical tropopause parameters observed using COSMIC GPS RO data

Tropical cyclones (TCs) are deep convective synoptic-scale systems that play an important role in modifying the thermal structure, tropical tropopause parameters and hence also modify stratosphere–troposphere exchange (STE) processes. In the present study, high vertical resolution and high accuracy measurements from COSMIC Global Positioning System (GPS) radio occultation (RO) measurements are used to investigate and quantify the effect of tropical cyclones that occurred over Bay of Bengal and Arabian Sea in the last decade on the tropical tropopause parameters. The tropopause parameters include cold-point tropopause altitude (CPH) and temperature (CPT), lapse-rate tropopause altitude (LRH) and temperature (LRT) and the thickness of the tropical tropopause layer (TTL), that is defined as the layer between convective outflow level (COH) and CPH, obtained from GPS RO data. From all the TC events, we generate the mean cyclone-centred composite structure for the tropopause parameters and removed it from the climatological mean obtained from averaging the GPS RO data from 2002 to 2013. Since the TCs include eye, eye walls and deep convective bands, we obtained the tropopause parameters based on radial distance from the cyclone eye. In general, decrease in the CPH in the eye is noticed as expected. However, as the distance from the cyclone eye increases by 300, 400, and 500 km, an enhancement in CPH (CPT) and LRH (LRT) is observed. Lowering of CPH (0.6 km) and LRH (0.4 km) values with coldest CPT and LRT (2–3 K) within a 500 km radius of the TC centre is noticed. Higher (2 km) COH leading to the lowering of TTL thickness (2–3 km) is clearly observed. There are multiple tropopause structures in the profiles of temperature obtained within 100 km from the centre of the TC. These changes in the tropopause parameters are expected to influence the water vapour transport from the troposphere to the lower stratosphere, and ozone from the lower stratosphere to the upper troposphere, hence influencing STE processes.
Statistical exploration of gaseous elemental mercury (GEM) measured at Cape Point from 2007 to 2011

The authors evaluated continuous high-resolution gaseous elemental mercury (GEM) data from the Cape Point Global Atmosphere Watch (CPT GAW) station with different statistical analysis techniques. GEM data were evaluated by cluster analysis and the results indicated that two clusters, separated at 0.904 ng m−3, existed. The air mass history for the two-cluster solution was investigated by means of back-trajectory analysis. The air mass back-trajectory net result showed lower GEM concentrations originating from the sparsely populated semi-arid interior of South Africa and the marine environment, whereas higher GEM concentrations originated predominately along the coast of South Africa that most likely coincide with trade routes and industrial activities in urban areas along the coast. Considering the net result from the air mass back-trajectories, it is evident that not all low GEM concentrations are from marine origin, and similarly, not all high GEM concentrations have a terrestrial origin. Equations were developed by means of multi-linear regression (MLR) analysis that allowed for the estimation and/or prediction of atmospheric GEM concentrations from other atmospheric parameters measured at the CPT GAW station. These equations also provided some insight into the relation and interaction of GEM with other atmospheric parameters. Both measured and MLR calculated data confirm a decline in GEM concentrations at CPT GAW over the period evaluated.
Technical Note: A proposal for ice nucleation terminology

Terminology dealing with ice nucleation in the atmosphere, in biological systems, and in other areas has not kept pace with the growth of empirical evidence and the development of new ideas over recent decades. Ambiguities and misinterpretations could be seen in the literature. This paper offers a set of definitions for various terms in common use, adds some qualifications, and introduces some new ones. Input has been received on the interpretation of various terms from a fair number of researchers; diverse views have been accommodated with some success. It is anticipated that the terminology proposed here will be helpful both to those who adopt it and to those who wish to explain a different perspective.