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Speciated atmospheric mercury on haze and non-haze days in an inland city in China

Long-term continuous measurements of speciated atmospheric mercury were conducted from July 2013 to June 2014 in Hefei, a midlatitude inland city in eastern central China that experiences frequent haze pollution. The mean concentrations (±standard deviation) of gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM) and particle-bound mercury (PBM) were 3.95 ± 1.93 ng m−3, 2.49 ± 2.41 and 23.3 ± 90.8 pg m−3, respectively, on non-haze days, and 4.74 ± 1.62 ng m−3, 4.32 ± 8.36 and 60.2 ± 131.4 pg m−3, respectively, on haze days. Potential source contribution function (PSCF) analysis suggested that atmospheric mercury pollution on haze days was caused primarily by local emissions, instead of via long-range transport. The poorer mixing conditions on haze days also favored the accumulation of atmospheric mercury. Compared to GEM and GOM, PBM was especially sensitive to haze pollution. The mean PBM concentration on haze days was 2.5 times that on non-haze days due to elevated concentrations of particulate matter. PBM also showed a clear seasonal trend; its concentration was the highest in fall and winter, decreased rapidly in spring and was the lowest in summer, following the same order in the frequency of haze days in different seasons. On both non-haze and haze days, GOM concentrations remained low at night, but increased rapidly just before sunrise, which could be due to diurnal variation in air exchange between the boundary layer and free troposphere. However, non-haze and haze days showed different trends in daytime GEM and GOM concentrations. On non-haze days, GEM and GOM declined synchronously through the afternoon, probably due to the retreat of the free tropospheric air as the height of the atmospheric boundary layer increases. In contrast, on haze days, GOM and GEM showed opposite trends with the highest GOM and lowest GEM observed in the afternoon, suggesting the occurrence of photochemical oxidation. This is supported by simple box-model calculations, which showed that oxidation of GEM to GOM does occur and that the transport of free tropospheric GOM alone is not large enough to account for the observed increase in daytime GOM. Our results further postulate that NO2 aggregation with the HgOH intermediate may be a potential mechanism for the enhanced production of GOM during daytime.
Regional and seasonal radiative forcing by perturbations to aerosol and ozone precursor emissions

Predictions of temperature and precipitation responses to changes in the anthropogenic emissions of climate forcers require the quantification of the radiative forcing exerted by those changes. This task is particularly difficult for near-term climate forcers like aerosols, methane, and ozone precursors because their short atmospheric lifetimes cause regionally and temporally inhomogeneous radiative forcings. This study quantifies specific radiative forcing, defined as the radiative forcing per unit change in mass emitted, for eight near-term climate forcers as a function of their source regions and the season of emission by using dedicated simulations by four general circulation and chemistry-transport models. Although differences in the representation of atmospheric chemistry and radiative processes in different models impede the creation of a uniform dataset, four distinct findings can be highlighted. Firstly, specific radiative forcing for sulfur dioxide and organic carbon are stronger when aerosol–cloud interactions are taken into account. Secondly, there is a lack of agreement on the sign of the specific radiative forcing of volatile organic compound perturbations, suggesting they are better avoided in climate mitigation strategies. Thirdly, the strong seasonalities of the specific radiative forcing of most forcers allow strategies to minimise positive radiative forcing based on the timing of emissions. Finally, European and shipping emissions exert stronger aerosol specific radiative forcings compared to East Asia where the baseline is more polluted. This study can therefore form the basis for further refining climate mitigation options based on regional and seasonal controls on emissions. For example, reducing summertime emissions of black carbon and wintertime emissions of sulfur dioxide in the more polluted regions is a possible way to improve air quality without weakening the negative radiative forcing of aerosols.
The magnitude of the snow-sourced reactive nitrogen flux to the boundary layer in the Uintah Basin, Utah, USA

Reactive nitrogen (Nr  =  NO, NO2, HONO) and volatile organic carbon emissions from oil and gas extraction activities play a major role in wintertime ground-level ozone exceedance events of up to 140 ppb in the Uintah Basin in eastern Utah. Such events occur only when the ground is snow covered, due to the impacts of snow on the stability and depth of the boundary layer and ultraviolet actinic flux at the surface. Recycling of reactive nitrogen from the photolysis of snow nitrate has been observed in polar and mid-latitude snow, but snow-sourced reactive nitrogen fluxes in mid-latitude regions have not yet been quantified in the field. Here we present vertical profiles of snow nitrate concentration and nitrogen isotopes (δ15N) collected during the Uintah Basin Winter Ozone Study 2014 (UBWOS 2014), along with observations of insoluble light-absorbing impurities, radiation equivalent mean ice grain radii, and snow density that determine snow optical properties. We use the snow optical properties and nitrate concentrations to calculate ultraviolet actinic flux in snow and the production of Nr from the photolysis of snow nitrate. The observed δ15N(NO3−) is used to constrain modeled fractional loss of snow nitrate in a snow chemistry column model, and thus the source of Nr to the overlying boundary layer. Snow-surface δ15N(NO3−) measurements range from −5 to 10 ‰ and suggest that the local nitrate burden in the Uintah Basin is dominated by primary emissions from anthropogenic sources, except during fresh snowfall events, where remote NOx sources from beyond the basin are dominant. Modeled daily averaged snow-sourced Nr fluxes range from 5.6 to 71  ×  107 molec cm−2 s−1 over the course of the field campaign, with a maximum noontime value of 3.1  ×  109 molec cm−2 s−1. The top-down emission estimate of primary, anthropogenic NOx in Uintah and Duchesne counties is at least 300 times higher than the estimated snow NOx emissions presented in this study. Our results suggest that snow-sourced reactive nitrogen fluxes are minor contributors to the Nr boundary layer budget in the highly polluted Uintah Basin boundary layer during winter 2014.
Single-particle investigation of summertime and wintertime Antarctic sea spray aerosols using low-Z particle EPMA, Raman microspectrometry, and ATR-FTIR imaging techniques

Two aerosol samples collected at King Sejong Korean scientific research station, Antarctica, on 9 December 2011 in the austral summer (sample S1) and 23 July 2012 in the austral winter (sample S2), when the oceanic chlorophyll a levels on the collection days of the samples were quite different, by ∼  19 times (2.46 vs. 0.13 µg L−1, respectively), were investigated on a single-particle basis using quantitative energy-dispersive electron probe X-ray microanalysis (ED-EPMA), called low-Z particle EPMA, Raman microspectrometry (RMS), and attenuated total reflection Fourier transform infrared (ATR-FTIR) imaging techniques to obtain their characteristics based on the elemental chemical compositions, molecular species, and mixing state. X-ray analysis showed that the supermicron summertime and wintertime Antarctic aerosol samples have different elemental chemical compositions, even though all the individual particles analyzed were sea spray aerosols (SSAs); i.e., the contents of C, O, Ca, S, and Si were more elevated, whereas Cl was more depleted, for sample S1 than for sample S2. Based on qualitative analysis of the chemical species present in individual SSAs by the combined application of RMS and ATR-FTIR imaging, different organic species were observed in samples S1 and S2; i.e., Mg hydrate salts of alanine were predominant in samples S1 and S2, whereas Mg salts of fatty acids internally mixed with Mg hydrate salts of alanine were significant in sample S2. Although CaSO4 was observed significantly in both samples S1 and S2, other inorganic species, such as Na2SO4, NaNO3, Mg(NO3)2, SiO2, and CH3SO3Mg, were observed more significantly in sample S1, suggesting that those compounds may be related to the higher phytoplankton activity in summer.
Spatiotemporal variability and contribution of different aerosol types to the aerosol optical depth over the Eastern Mediterranean

This study characterizes the spatiotemporal variability and relative contribution of different types of aerosols to the aerosol optical depth (AOD) over the Eastern Mediterranean as derived from MODIS (Moderate Resolution Imaging Spectroradiometer) Terra (March 2000–December 2012) and Aqua (July 2002–December 2012) satellite instruments. For this purpose, a 0.1° × 0.1° gridded MODIS dataset was compiled and validated against sun photometric observations from the AErosol RObotic NETwork (AERONET). The high spatial resolution and long temporal coverage of the dataset allows for the determination of local hot spots like megacities, medium-sized cities, industrial zones and power plant complexes, seasonal variabilities and decadal averages. The average AOD at 550 nm (AOD550) for the entire region is ∼ 0.22 ± 0.19, with maximum values in summer and seasonal variabilities that can be attributed to precipitation, photochemical production of secondary organic aerosols, transport of pollution and smoke from biomass burning in central and eastern Europe and transport of dust from the Sahara and the Middle East. The MODIS data were analyzed together with data from other satellite sensors, reanalysis projects and a chemistry–aerosol-transport model using an optimized algorithm tailored for the region and capable of estimating the contribution of different aerosol types to the total AOD550. The spatial and temporal variability of anthropogenic, dust and fine-mode natural aerosols over land and anthropogenic, dust and marine aerosols over the sea is examined. The relative contribution of the different aerosol types to the total AOD550 exhibits a low/high seasonal variability over land/sea areas, respectively. Overall, anthropogenic aerosols, dust and fine-mode natural aerosols account for ∼ 51, ∼ 34 and ∼ 15 % of the total AOD550 over land, while, anthropogenic aerosols, dust and marine aerosols account ∼ 40, ∼ 34 and ∼ 26 % of the total AOD550 over the sea, based on MODIS Terra and Aqua observations.
On the 18-day quasi-periodic oscillation in the ionosphere

The presence and persistence of an 18-day quasi-periodic oscillation in the ionospheric electron density variations were studied. The data of lower ionosphere (radio-wave absorption at equivalent frequency near 1 MHz), middle and upper ionosphere (critical frequencies f0E and f0F2) for the period 1970–1990 have been used in the analysis. Also, solar and geomagnetic activity data (the sunspot numbers Rz and solar radio flux F10.7 cm, and aN index respectively) were used to compare the time variations of the ionospheric with the solar and geomagnetic activity data. Periodogram, complex demodulation, auto- and cross-correlation analysis have been used. It was found that 18-day quasi-periodic oscillation exists and persists in the temporal variations of the ionospheric parameters under study with high level of correlation and mean period of 18–19 days. The time variation of the amplitude of the 18-day quasi-periodic oscillation in the ionosphere seems to be modulated by the long-term solar cycle variations. Such oscillations exist in some solar and geomagnetic parameters and in the planetary wave activity of the middle atmosphere. The high similarities in the amplitude modulation, long-term amplitude variation, period range between the oscillation of investigated parameters and the global activity of oscillation suggests a possible solar influence on the 18-day quasi-periodic oscillation in the ionosphere.
Quasi-periodic precipitation with periods between 40 and 60 minutes

Intervals of periodic enhancements of E-region electron density have been found in EISCAT (European Incoherent SCATter) data. The periods are typically between 40 and 60 min. The phenomenon is observed during relatively quiet times, though after geomagnetic disturbances; it may last up to 6 h. The events can occur at all times of day with a maximum probability in the MLT morning sector. Using the EISCAT database from recent years, the statistical characteristics of these events, and their relation to magnetospheric conditions defined by the Dst index and the d.c. electric field perpendicular to B= have been derived. The latitudinal extent is found to be several degrees, but the longitudinal extent is not known. It is concluded that these events are due to the periodically modulated flux of electron precipitation controlled by oscillations in the magnetospheric tail.
Predicting geomagnetic storms from solar-wind data using time-delay neural networks

We have used time-delay feed-forward neural networks to compute the geomagnetic-activity index Dst one hour ahead from a temporal sequence of solar-wind data. The input data include solar-wind density n, velocity V and the southward component Bz of the interplanetary magnetic field. Dst is not included in the input data. The networks implement an explicit functional relationship between the solar wind and the geomagnetic disturbance, including both direct and time-delayed non-linear relations. In this study we especially consider the influence of varying the temporal size of the input-data sequence. The networks are trained on data covering 6600 h, and tested on data covering 2100 h. It is found that the initial and main phases of geomagnetic storms are well predicted, almost independent of the length of the input-data sequence. However, to predict the recovery phase, we have to use up to 20 h of solar-wind input data. The recovery phase is mainly governed by the ring-current loss processes, and is very much dependent on the ring-current history, and thus also the solar-wind history. With due consideration of the time history when optimizing the networks, we can reproduce 84% of the Dst variance.
Response of ionospheric electric fields to variations in the interplanetary magnetic field

The STARE system (Scandinavian Twin Auroral Radar Experiment) provides estimates of electron drift velocities, and hence also of the electric field in the high-latitude E-region ionosphere between 65 and 70 degrees latitude. The occurrence of drift velocities larger than about 400 m/s (equivalent to an electric field of 20 mV/m) have been correlated with the magnitude of the Interplanetary Magnetic Field (IMF) components Bz and By at all local times. Observation days have been considered during which both southward (Bz<0) and northward (Bz>0) IMF occurred. The occurrence of electric fields larger than 20 mV/m increases with increases in Bz magnitudes when Bz<0. It is found that the effects of southward IMF continue for some time following the northward turnings of the IMF. In order to eliminate such residual effects for Bz<0, we have, in the second part of the study, considered those days which were characterized by a pure northward IMF. The occurrence is considerably lower during times when Bz>0, than during those when Bz is negative. These results are related to the expansion and contraction of the auroral oval. The different percentage occurrences of large electric field for By>0 and By<0 components of the IMF during times when Bz>0, clearly display a dawn-dusk asymmetry of plasma flow in the ionosphere. The effects of the time-varying solar-wind speed, density, IMF fluctuations, and magnetospheric substorms on the occurrence of auroral-backscatter observations are also discussed.
The formation of electron-temperature hot spots in the main ionospheric trough by the internal processes

A mathematical model of the convecting high-latitude ionosphere is described which produces three-dimensional distributions of electron density, positive-ion velocity and electron and ion temperatures at the F-layer altitudes. The results of simulation of the behaviour of the high-latitude ionosphere, in particular, the heat regime of the F-layer, are presented and analysed. From our study, it was found that electron-temperature hot spots in the main ionospheric trough can arise owing to internal ionospheric processes, and not due to effects of any external causes. Three conditions, to be satisfied simultaneously, are necessary for the formation of the considered electron-temperature hot spots: first, low values of electron density; second, solar illumination of the upper F region and darkness of the lower F region; third, low values of neutral-component densities. These conditions are valid in the main ionospheric trough near the terminator on the nightside when the density of the neutral atmosphere is not high. The physical processes which lead to the formation of the electron-temperature hot spots are the heat transfer from the upper into the lower F region, the reduced heat capacity of electron gas and the weakened cooling of electron gas due to inelastic collisions with neutral atoms and molecules. Also investigated is the influence of seasonal and solar-activity variations on the efficiency of the identified mechanism responsible for the formation of the electron temperature peaks in the main ionospheric trough by the internal processes.