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The volatility of organic aerosols (OA) has emerged as a property of primary importance in understanding their atmospheric life cycle, and thus abundance and transport. However, quantitative estimates of the thermodynamic (volatility, water solubility) and kinetic parameters dictating ambient-OA gas-particle partitioning, such as saturation concentrations (<i>C</i><sup>∗</sup>), enthalpy of evaporation (Δ<i>H</i><sub>vap</sub>), and evaporation coefficient (<i>γ</i><sub>e</sub>), are highly uncertain. Here, we present measurements of ambient-OA volatility at two sites in the southeastern US, one at a rural setting in Alabama dominated by biogenic volatile organic compounds (BVOCs) as part of the Southern Oxidant and Aerosol Study (SOAS) in June–July 2013, and another at a more anthropogenically influenced urban location in North Carolina during October–November 2013. These measurements applied a dual-thermodenuder (TD) system, in which temperature and residence times are varied in parallel to constrain equilibrium and kinetic aerosol volatility properties. Gas-particle partitioning parameters were determined via evaporation kinetic model fits to the dual-TD observations. OA volatility parameter values derived from both datasets were similar despite the fact that measurements were collected in distinct settings and seasons. The OA volatility distributions also did not vary dramatically over the campaign period or strongly correlate with OA components identified via positive matrix factorization of aerosol mass spectrometer data. A large portion (40–70 %) of measured ambient OA at both sites was composed of very-low-volatility organics (<i>C</i><sup>∗</sup> ≤ 0.1 µg m<sup>−3</sup>). An effective Δ<i>H</i><sub>vap</sub> of bulk OA of ∼ 80–100 kJ mol<sup>−1</sup> and a <i>γ</i><sub>e</sub> value of ∼ 0.5 best describe the evaporation observed in the TDs. This range of Δ<i>H</i><sub>vap</sub> values is substantially higher than that typically assumed for simulating OA in atmospheric models (30–40 kJ mol<sup>−1</sup>). TD data indicate that <i>γ</i><sub>e</sub> is on the order of 0.1 to 0.5, indicating that repartitioning timescales for atmospheric OA are on the order of several minutes to an hour under atmospheric conditions. The OA volatility distributions resulting from fits were compared to those simulated in the Weather, Research and Forecasting model with Chemistry (WRF/Chem) with a current treatment of secondary organic aerosol (SOA) formation. The substantial fraction of low-volatility material observed in our measurements is largely missing from simulations, and OA mass concentrations are underestimated. The large discrepancies between simulations and observations indicate a need to treat low-volatility OA in atmospheric models. Volatility parameters extracted from ambient measurements enable evaluation of emerging treatments for OA (e.g., secondary OA using the volatility basis set or formed via aqueous chemistry) in atmospheric models.
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Geotail energetic particle, magnetic field data and plasma observations (EPIC, MGF and CPI experiments) have been examined for a number of energetic particle bursts in the distant tail (120Re<|X<sub>GSM</sub>|< 130 Re), associated with moving magnetic field structures, following substorm onsets. The features obtained from this data analysis are consistent with the distant magnetotail dynamics determined first by ISEE3 observations and explained in terms of the neutral line model. At the onset of the bursts, before plasma sheet entrance, energetic electrons appear as a field-aligned beam flowing in the tailward direction, followed by anisotropic ions. Within the flux rope region, suprathermal ions exhibit a convective anisotropy, which allows determination of the plasma flow velocity, assuming that the anisotropy arises from the Compton-Getting effect. The velocities thus determined in the plasma sheet are estimated to be 200–650 km/s, and compare favourably with the velocities derived from the CPI electron and proton experiment. The estimated length of magnetic field structures varies between 28 and 56 Re and depends on the strength of the westward electrojet intensification. Finally, the three structures reported here show clear magnetic field signatures of flux rope topology. The existence of a strong magnetic field aligned approximately along the Y-axis and centred on the north-to-south excursion of the field, and the bipolar signature in both <i>B</i>y and/or <i>B</i>z components, is consistent with the existence of closed field lines extending from Earth and wrapping around the core of the flux rope structure.<br><br><b>Key words.</b> Magnetospheric configuration and dynamics · Magnetotail
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This study examines the adequacy of the existing Brewer network to supplement other networks from the ground and space to detect SO<sub>2</sub> plumes of volcanic origin. It was found that large volcanic eruptions of the last decade in the Northern Hemisphere have a positive columnar SO<sub>2</sub> signal seen by the Brewer instruments located under the plume. It is shown that a few days after the eruption the Brewer instrument is capable of detecting significant columnar SO<sub>2</sub> increases, exceeding on average 2 DU relative to an unperturbed pre-volcanic 10-day baseline, with a mean close to 0 and <i>σ</i> = 0.46, as calculated from the 32 Brewer stations under study. Intercomparisons with independent measurements from the ground and space as well as theoretical calculations corroborate the capability of the Brewer network to detect volcanic plumes. For instance, the comparison with OMI (Ozone Monitoring Instrument) and GOME-2 (Global Ozone Monitoring Experiment-2) SO<sub>2</sub> space-borne retrievals shows statistically significant agreement between the Brewer network data and the collocated satellite overpasses in the case of the Kasatochi eruption. Unfortunately, due to sparsity of satellite data, the significant positive departures seen in the Brewer and other ground networks following the Eyjafjallajökull, Bárðarbunga and Nabro eruptions could not be statistically confirmed by the data from satellite overpasses. A model exercise from the MACC (Monitoring Atmospheric Composition and Climate) project shows that the large increases in SO<sub>2</sub> over Europe following the Bárðarbunga eruption in Iceland were not caused by local pollution sources or ship emissions but were clearly linked to the volcanic eruption. Sulfur dioxide positive departures in Europe following Bárðarbunga could be traced by other networks from the free troposphere down to the surface (AirBase (European air quality database) and EARLINET (European Aerosol Research Lidar Network)). We propose that by combining Brewer data with that from other networks and satellites, a useful tool aided by trajectory analyses and modelling could be created which can also be used to forecast high SO<sub>2</sub> values both at ground level and in air flight corridors following future eruptions.
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The mechanism of generation of internal gravity waves (IGW) by mesoscale turbulence in the troposphere is considered. The equations that describe the generation of waves by hydrodynamic sources of momentum, heat and mass are derived. Calculations of amplitudes, wave energy fluxes, turbulent viscosities, and accelerations of the mean flow caused by IGWs generated in the troposphere are made. A comparison of different mechanisms of turbulence production in the atmosphere by IGWs shows that the nonlinear destruction of a primary IGW into a spectrum of secondary waves may provide additional dissipation of nonsaturated stable waves. The mean wind increases both the effectiveness of generation and dissipation of IGWs propagating in the direction of the wind. Competition of both effects may lead to the dominance of IGWs propagating upstream at long distances from tropospheric wave sources, and to the formation of eastward wave accelerations in summer and westward accelerations in winter near the mesopause.
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Few studies have investigated nocturnal new particle formation (NPF) events, and none of them were conducted in urban environments. Nocturnal NPF can potentially be a significant source of particles in urban areas, and studying them would improve our understanding of nucleation mechanisms. To address this, our study was conducted in an urban environment to investigate the physical characteristics of NPF events, with a particular focus on nocturnal events and the differences between them and the daytime NPF events. Particle number size distribution (PNSD) was measured for 2 weeks at each of 25 sites across an urban environment. A new method was proposed to automatically categorise NPF events based on growth rate (GR) in order to remove the bias related to the manual procedure. Out of 219 observed events, 118 and 101 were categorised into class I and II respectively and 73 happened during the nighttime which included more than 30 % of the events. GR and condensation sink (CS) were calculated and a slight negative relationship between GR and CS was observed. Nocturnal events displayed higher GRs compared to daylight ones which were on average about 10 %. Back trajectory analysis was also conducted to estimate the locations of the sources of daylight and nocturnal precursors. While the precursors related to daylight events originated from different locations with no particular pattern, back-trajectory analysis showed many air masses associated with nocturnal NPF events were transported from over the ocean. Overall, nocturnal NPF events were found to be a significant source of particles in the studied environment with different physical characteristics and/or sources compared to daylight events.
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Reducing insolation has been proposed as a geoengineering response to global warming. Here we present the results of climate model simulations of a unique Geoengineering Model Intercomparison Project Testbed experiment to investigate the benefits and risks of a scheme that would brighten certain oceanic regions. The National Center for Atmospheric Research CESM CAM4-Chem global climate model was modified to simulate a scheme in which the albedo of the ocean surface is increased over the subtropical ocean gyres in the Southern Hemisphere. In theory, this could be accomplished using a stable, nondispersive foam, comprised of tiny, highly reflective microbubbles. Such a foam has been developed under idealized conditions, although deployment at a large scale is presently infeasible. We conducted three ensemble members of a simulation (G4Foam) from 2020 through to 2069 in which the albedo of the ocean surface is set to 0.15 (an increase of 150 %) over the three subtropical ocean gyres in the Southern Hemisphere, against a background of the RCP6.0 (representative concentration pathway resulting in +6 W m<sup>−2</sup> radiative forcing by 2100) scenario. After 2069, geoengineering is ceased, and the simulation is run for an additional 20 years. Global mean surface temperature in G4Foam is 0.6 K lower than RCP6.0, with statistically significant cooling relative to RCP6.0 south of 30° N. There is an increase in rainfall over land, most pronouncedly in the tropics during the June–July–August season, relative to both G4SSA (specified stratospheric aerosols) and RCP6.0. Heavily populated and highly cultivated regions throughout the tropics, including the Sahel, southern Asia, the Maritime Continent, Central America, and much of the Amazon experience a statistically significant increase in precipitation minus evaporation. The temperature response to the relatively modest global average forcing of −1.5 W m<sup>−2</sup> is amplified through a series of positive cloud feedbacks, in which more shortwave radiation is reflected. The precipitation response is primarily the result of the intensification of the southern Hadley cell, as its mean position migrates northward and away from the Equator in response to the asymmetric cooling.
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Numerical simulations are presented of the ion distribution functions seen by middle-altitude spacecraft in the low-latitude boundary layer (LLBL) and cusp regions when reconnection is, or has recently been, taking place at the equatorial magnetopause. From the evolution of the distribution function with time elapsed since the field line was opened, both the observed energy/observation-time and pitch-angle/energy dispersions are well reproduced. Distribution functions showing a mixture of magnetosheath and magnetospheric ions, often thought to be a signature of the LLBL, are found on newly opened field lines as a natural consequence of the magnetopause effects on the ions and their flight times. In addition, it is shown that the extent of the source region of the magnetosheath ions that are detected by a satellite is a function of the sensitivity of the ion instrument . If the instrument one-count level is high (and/or solar-wind densities are low), the cusp ion precipitation detected comes from a localised region of the mid-latitude magnetopause (around the magnetic cusp), even though the reconnection takes place at the equatorial magnetopause. However, if the instrument sensitivity is high enough, then ions injected from a large segment of the dayside magnetosphere (in the relevant hemisphere) will be detected in the cusp. Ion precipitation classed as LLBL is shown to arise from the low-latitude magnetopause, irrespective of the instrument sensitivity. Adoption of threshold flux definitions has the same effect as instrument sensitivity in artificially restricting the apparent source region<br><br><b>Key words.</b> Low-latitude boundary layer · Cusp regions · Open magnetosphere model · Mid-altitudes
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In situ single particle analysis of ice particle residuals (IPRs) and out-of-cloud aerosol particles was conducted by means of laser ablation mass spectrometry during the intensive INUIT-JFJ/CLACE campaign at the high alpine research station Jungfraujoch (3580 m a.s.l.) in January–February 2013. During the 4-week campaign more than 70 000 out-of-cloud aerosol particles and 595 IPRs were analyzed covering a particle size diameter range from 100 nm to 3 µm. The IPRs were sampled during 273 h while the station was covered by mixed-phase clouds at ambient temperatures between −27 and −6 °C. The identification of particle types is based on laboratory studies of different types of biological, mineral and anthropogenic aerosol particles. The outcome of these laboratory studies was characteristic marker peaks for each investigated particle type. These marker peaks were applied to the field data. In the sampled IPRs we identified a larger number fraction of primary aerosol particles, like soil dust (13 ± 5 %) and minerals (11 ± 5 %), in comparison to out-of-cloud aerosol particles (2.4 ± 0.4 and 0.4 ± 0.1 %, respectively). Additionally, anthropogenic aerosol particles, such as particles from industrial emissions and lead-containing particles, were found to be more abundant in the IPRs than in the out-of-cloud aerosol. In the out-of-cloud aerosol we identified a large fraction of aged particles (31 ± 5 %), including organic material and secondary inorganics, whereas this particle type was much less abundant (2.7 ± 1.3 %) in the IPRs. In a selected subset of the data where a direct comparison between out-of-cloud aerosol particles and IPRs in air masses with similar origin was possible, a pronounced enhancement of biological particles was found in the IPRs.
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Stratosphere–troposphere coupling is investigated in relation to middle atmospheric subtropical jet (MASTJ) variations in boreal winter. An exceptional strengthening of the MASTJ occurred in association with a sudden equatorward shift of the stratospheric polar night jet (PNJ) in early December 2011. This abrupt transformation of the MASTJ and PNJ had no apparent relation to the upward propagation of planetary waves from the troposphere. The impact of this stratospheric event penetrated into the troposphere in two regions: in the northern polar region and the tropics. Due to the strong MASTJ, planetary waves at higher latitudes were deflected and trapped in the northern polar region. Trapping of the planetary waves resulted in amplification of zonal wave number 1 component, which appeared in the troposphere as the development of a trough over the Atlantic sector and a ridge over the Eurasian sector. A strong MASTJ also suppressed the equatorward propagation of planetary waves, which resulted in weaker tropical stratospheric upwelling and produced anomalous warming in the tropical stratosphere. In the tropical tropopause layer (TTL), however, sublimation of ice clouds kept the temperature change minor. In the troposphere, an abrupt termination of a Madden–Julian Oscillation (MJO) event occurred following the static stability increase in the TTL. This termination suggests that the stratospheric event affected the convective episode in the troposphere.
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The interaction between the factors of the quasi-biennial oscillation (QBO) and the 11-year solar cycle is considered as an separate factor influencing the interannual January-March variations of total ozone over Northeastern Europe. Linear correlation analysis and the running correlation method are used to examine possible connections between ozone and solar activity at simultaneous moment the QBO phase. Statistically significant correlations between the variations of total ozone in February and, partially, in March, and the sunspot numbers during the different phases of QBO are found. The running correlation method between the ozone and the equatorial zonal wind demonstrates a clear modulation of 11-y solar signal for February and March. Modulation is clearer if the QBO phases are defined at the level of 50 hPa rather than at 30 hPa. The same statistical analyses are conducted also for possible connections between the index of stratospheric circulation <i>C</i><sub>1</sub> and sunspot numbers considering the QBO phase. Statistically significant connections are found for February. The running correlations between the index <i>C</i><sub>1</sub> and the equatorial zonal wind show the clear modulation of 11-y solar signal for February and March. Based on the obtained correlations between the interannual variations of ozone and index <i>C</i><sub>1</sub>, it may be concluded that a connection between solar cycle – QBO – ozone occurs through the dynamics of stratospheric circulation.
