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Observed microphysical changes in Arctic mixed-phase clouds when transitioning from sea ice to open ocean

In situ airborne observations of cloud microphysics, aerosol properties, and thermodynamic structure over the transition from sea ice to ocean are presented from the Aerosol-Cloud Coupling And Climate Interactions in the Arctic (ACCACIA) campaign. A case study from 23 March 2013 provides a unique view of the cloud microphysical changes over this transition under cold-air outbreak conditions. Cloud base lifted and cloud depth increased over the transition from sea ice to ocean. Mean droplet number concentrations, Ndrop, also increased from 110 ± 36 cm−3 over the sea ice to 145 ± 54 cm−3 over the marginal ice zone (MIZ). Downstream over the ocean, Ndrop decreased to 63 ± 30 cm−3. This reduction was attributed to enhanced collision-coalescence of droplets within the deep ocean cloud layer. The liquid water content increased almost four fold over the transition and this, in conjunction with the deeper cloud layer, allowed rimed snowflakes to develop and precipitate out of cloud base downstream over the ocean. The ice properties of the cloud remained approximately constant over the transition. Observed ice crystal number concentrations averaged approximately 0.5–1.5 L−1, suggesting only primary ice nucleation was active; however, there was evidence of crystal fragmentation at cloud base over the ocean. Little variation in aerosol particle number concentrations was observed between the different surface conditions; however, some variability with altitude was observed, with notably greater concentrations measured at higher altitudes ( >  800 m) over the sea ice. Near-surface boundary layer temperatures increased by 13 °C from sea ice to ocean, with corresponding increases in surface heat fluxes and turbulent kinetic energy. These significant thermodynamic changes were concluded to be the primary driver of the microphysical evolution of the cloud. This study represents the first investigation, using in situ airborne observations, of cloud microphysical changes with changing sea ice cover and addresses the question of how the microphysics of Arctic stratiform clouds may change as the region warms and sea ice extent reduces.
Large-scale atmospheric circulation control on stable water isotopes in precipitation over the northwestern and southeastern Tibetan Plateau

The mid-latitude westerlies and South Asian Summer Monsoon (SASM) are two major atmospheric circulation systems influencing the Tibetan Plateau (TP). We report a seven-year (2007/2008–2013/2014) dataset of δ18O in precipitation (δ18Op) collected at three stations. Taxkorgan (TX) and Bulunkou (BLK) are located on the northwestern TP where westerly winds dominate while Lulang (LL) is situated on the southeastern TP where the SASM dominates. δ18O in precipitation (δ18Op) in northwestern TP varies with surface temperature (T) throughout the study period, and is depleted in 18O in precipitation during June to September when the monsoonal circulation enters the TP. Integration with model outputs suggests that large-scale atmospheric circulation plays a major role in isotopic seasonality in both regions. A teleconnection between precipitation on the northwestern TP and the El Niño-Southern Oscillation (ENSO) warm phase is suggested by changes in the relationship between δ18O and δD (e.g., reduced slope and weighted d-excess) in precipitation samples. These observations are indicative of a weakening of the mid-latitude westerly jet allowing local processes in the continental interior to become more dominant, thereby increasing the contribution of secondary evaporation from falling raindrops and kinetic fractionation. Under the conditions of a high Northern Annular Mode (NAM) the westerly jet is intensified over the southeastern TP which enhances local evaporation and continental recycling as revealed by a lower δD-δ18O slope and intercept, but higher d-excess average in contemporaneously collected precipitation samples. The significant correlation between T and δ18Op in the northwestern TP during various composite periods highlights a variation from 0.39 ‰ / ℃ (ENSO warm) to 0.77 ‰ / ℃ (high NAM), attributable to decreased (increased) water vapor availability over the northwestern TP during the ENSO warm (strong positive NAM) phase. ENSO cold and strong negative NAM phases show analogous effects on atmospheric circulation over both regions.
Particulate matter (PM) episodes at a suburban site in Hong Kong: evolution of PM characteristics and role of photochemistry in secondary aerosol formation

Episodes with high concentrations of particulate matter (PM) across the seasons were investigated during four 1-month campaigns at a suburban site in Hong Kong. High-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurements revealed that both regional transport and secondary formation contributed to high PM levels during the episodes at this site. Based on distinct meteorological conditions, episodes were categorized into three types: liquid water content (LWC), solar irradiance (IR), and long-range transport (LRT). Despite the difference in meteorological conditions, all episodes were characterized by a high fraction of sulfate (45–56 %) and organics (23–34 %). However, aerosols in LWC episodes were less aged, consisting of the lowest fraction of secondary organic aerosol (SOA) and the highest fraction of small particles. Large particles mixed internally while freshly formed small particles mixed externally in LWC episodes. Aerosols in LRT episodes, by contrast, were the most aged and consisted of the highest proportion of low-volatility oxygenated organic aerosol (LVOOA) and the lowest proportion of small particles. Both small and large particles mixed externally in LRT episodes. The highest proportion of semi-volatile oxygenated organic aerosol (SVOOA) and a medium proportion of small particles were observed in IR episodes. Both small and large particles were likely externally mixed during IR episodes. Furthermore, aerosols experienced the most dramatic size increase and diurnal variation, with a time lag between SVOOA and LVOOA and a gradual increase in carbon oxidation state (OSc ≈ 2 × O : C − H : C). Five out of 10 episodes were of the IR type, further reflecting the importance of this type of episode. The evolution of aerosol components in one particular episode of the IR type, which exhibited a clear land–sea breeze pattern, was examined in detail. Sulfate and SOA due to photochemical aging were very efficiently produced during the course of 6 h. The “less-oxidized” SOA (SVOOA) was initially formed at a higher rate than the “more-oxidized” SOA (LVOOA). The SVOOA transformed to LVOOA at the later stage of photochemical aging. This transformation was further supported by mass spectral analysis, which showed an increase in the most oxidized ion (CO2+) and decreases in moderately oxidized ones (C2H3O+, C3H3O+ and C3H5O+). By measuring the physical and chemical properties of PM in a highly time-resolved manner, the current study was able to demonstrate the dynamic and complex nature of PM transformation during high-PM episodes.
Aerosol arriving on the Caribbean island of Barbados: physical properties and origin

The marine aerosol arriving at Barbados (Ragged Point) was characterized during two 3-week long measurement periods in November 2010 and April 2011, in the context of the measurement campaign CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados). Through a comparison between ground-based and airborne measurements it was shown that the former are representative of the marine boundary layer at least up to cloud base. In general, total particle number concentrations (Ntotal) ranged from as low as 100  up to 800 cm−3, while number concentrations for cloud condensation nuclei (NCCN) at a supersaturation of 0.26 % ranged from some 10 to 600 cm−3. Ntotal and NCCN depended on the air mass origin. Three distinct types of air masses were found. One type showed elevated values for both Ntotal and NCCN and could be attributed to long-range transport from Africa, by which biomass burning particles from the Sahel region and/or mineral dust particles from the Sahara were advected. The second and third type both had values for NCCN below 200 cm−3 and a clear minimum in the particle number size distribution (NSD) around 70 to 80 nm (Hoppel minimum). While for one of these two types the accumulation mode was dominating (albeit less so than for air masses advected from Africa), the Aitken mode dominated the other and contributed more than 50 % of all particles. These Aitken mode particles likely were formed by new particle formation no more than 3 days prior to the measurements. Hygroscopicity of particles in the CCN size range was determined from CCN measurements to be κ  =  0.66 on average, which suggests that these particles contain mainly sulfate and do not show a strong influence from organic material, which might generally be the case for the months during which measurements were made. The average κ could be used to derive NCCN from measured number size distributions, showing that this is a valid approach to obtain NCCN. Although the total particulate mass sampled on filters was found to be dominated by Na+ and Cl−, this was found to be contributed by a small number of large particles ( >  500 nm, mostly even in the super-micron size range). Based on a three-modal fit, a sea spray mode observed in the NSDs was found to contribute 90 % to the total particulate mass but only 4 to 10 % to Ntotal and up to 15 % to NCCN. This is in accordance with finding no correlation between Ntotal and wind speed.
Residual Mean Circulation and Temperature Changes during the Evolution of Stratospheric Sudden Warming Revealed in MERRA

Residual mean circulation and temperature changes during the evolution of major stratospheric sudden warming (SSW) are investigated by composite analyses of 22 SSW events from 1979 to 2012 during the Northern Hemisphere winter (November–March) using four reanalysis data sets (MERRA, ERA-Interim, NCEP-NCAR, and JRA-55). The SSW events are classified as Type-1 or Type-2 based on the relative amplitude of planetary waves with zonal wavenumbers 1 and 2. The residual mean circulation induced by each forcing term in the Transformed Eulerian mean (TEM) momentum equation and the temperature advection associated with the circulation are calculated for both types of SSW, based on the generalized downward control principle using the MERRA data set. When ‘Lag = 0’ is defined as the day on which the wind reversal occurred at 60° N and 10 hPa, strong poleward and downward motion exists at Lag = −8 and Lag = −1 for Type-1 and at Lag = −3 for Type-2, which is induced primarily by the Eliassen–Palm flux divergence forcing (EPD). The poleward and downward motion is stronger for Type-2 than for Type-1. Gravity wave drag (GWD) produces a smaller contribution to the residual circulation than EPD. During the warming phase (at Lag = −2), strong temperature advection by the EPD induces primarily polar stratospheric warming. On the other hand, during the temperature recovery phase (at Lag = +2), anomalous negative temperature advection and diabatic cooling produce negative temperature tendency anomalies. Structures in the temperature tendency and temperature advection calculated using the MERRA data set are similar to those calculated using the ERA-Interim data set.
North African dust transport toward the western Mediterranean basin: atmospheric controls on dust source activation and transport pathways during June–July 2013

Dust transported from north African source region toward the Mediterranean basin and Europe is a ubiquitous phenomenon in the Mediterranean region. Winds formed by large-scale pressure gradients foster dust entrainment into the atmosphere over north African dust source regions and advection of dust downwind. The constellation of centers of high and low pressure determines wind speed and direction, and thus the chance for dust emission over northern Africa and transport toward the Mediterranean. We present characteristics of the atmospheric dust life cycle determining dust transport toward the Mediterranean basin with focus on the ChArMEx (Chemistry-Aerosol Mediterranean Experiment) special observation period in June and July 2013 using the atmosphere–dust model COSMO-MUSCAT (COSMO: COnsortium for Small-scale MOdeling; MUSCAT: MUltiScale Chemistry Aerosol Transport Model). Modes of atmospheric circulation are identified from empirical orthogonal function (EOF) analysis of the geopotential height at 850 hPa and compared to EOFs calculated from 1979–2015 ERA-Interim reanalysis. Two different phases are identified from the first EOF, which in total explain 45 % of the variance. They are characterized by the propagation of the subtropical ridge into the Mediterranean basin, the position of the Saharan heat low and the predominant Iberian heat low, and discussed illustrating a dipole pattern for enhanced (reduced) dust emission fluxes, stronger (weaker) meridional dust transport, and consequent increased (decreased) atmospheric dust concentrations and deposition fluxes. In the event of a predominant high-pressure zone over the western and central Mediterranean (positive phase), a hot spot in dust emission flux is evident over the Grand Erg Occidental, and a reduced level of atmospheric dust loading occurs over the western Mediterranean basin. The meridional transport in northward direction is reduced due to prevailing northerly winds. In case of a predominant heat low trough linking the Iberian and the Saharan heat low (negative phase), meridional dust transport toward the western Mediterranean is increased due to prevailing southerly winds resulting in an enhanced atmospheric dust loading over the western Mediterranean. Altogether, results from this study illustrate the relevance of knowing dust source location and characteristics in concert with atmospheric circulation. The study elaborates on the question of the variability of summertime dust transport toward the Mediterranean and Europe with regard to atmospheric circulation conditions controlling dust emission and transport routes of Saharan dust, exemplarily for the 2-month period of June–July 2013. Ultimately, outcomes from this study contribute to the understanding of the variance in dust transport into a populated region.
Global biogenic volatile organic compound emissions in the ORCHIDEE and MEGAN models and sensitivity to key parameters

A new version of the biogenic volatile organic compounds (BVOCs) emission scheme has been developed in the global vegetation model ORCHIDEE (Organizing Carbon and Hydrology in Dynamic EcosystEm), which includes an extended list of biogenic emitted compounds, updated emission factors (EFs), a dependency on light for almost all compounds and a multi-layer radiation scheme. Over the 2000–2009 period, using this model, we estimate mean global emissions of 465 Tg C yr−1 for isoprene, 107.5 Tg C yr−1 for monoterpenes, 38 Tg C yr−1 for methanol, 25 Tg C yr−1 for acetone and 24 Tg C yr−1 for sesquiterpenes. The model results are compared to state-of-the-art emission budgets, showing that the ORCHIDEE emissions are within the range of published estimates. ORCHIDEE BVOC emissions are compared to the estimates of the Model of Emissions of Gases and Aerosols from Nature (MEGAN), which is largely used throughout the biogenic emissions and atmospheric chemistry community. Our results show that global emission budgets of the two models are, in general, in good agreement. ORCHIDEE emissions are 8 % higher for isoprene, 8 % lower for methanol, 17 % higher for acetone, 18 % higher for monoterpenes and 39 % higher for sesquiterpenes, compared to the MEGAN estimates. At the regional scale, the largest differences between ORCHIDEE and MEGAN are highlighted for isoprene in northern temperate regions, where ORCHIDEE emissions are higher by 21 Tg C yr−1, and for monoterpenes, where they are higher by 4.4 and 10.2 Tg C yr−1 in northern and southern tropical regions compared to MEGAN. The geographical differences between the two models are mainly associated with different EF and plant functional type (PFT) distributions, while differences in the seasonal cycle are mostly driven by differences in the leaf area index (LAI). Sensitivity tests are carried out for both models to explore the response to key variables or parameters such as LAI and light-dependent fraction (LDF). The ORCHIDEE and MEGAN emissions are differently affected by LAI changes, with a response highly depending on the compound considered. Scaling the LAI by a factor of 0.5 and 1.5 changes the isoprene global emission by −21 and +8 % for ORCHIDEE and −15 and +7 % for MEGAN, and affects the global emissions of monoterpenes by −43 and +40 % for ORCHIDEE and −11 and +3 % for MEGAN. Performing a further sensitivity test, forcing ORCHIDEE with the MODIS LAI, confirms the high sensitivity of the ORCHIDEE emission module to LAI variation. We find that MEGAN is more sensitive to variation in the LDF parameter than ORCHIDEE. Our results highlight the importance and the need to further explore the BVOC emission estimate variability and the potential for using models to investigate the estimated uncertainties.
Emissions of NO, NO2 and PM from inland shipping

Particulate matter (PM) and nitrogen oxides NOx (NOx =  NO2+ NO) are key species for urban air quality in Europe and are emitted by mobile sources. According to European recommendations, a significant fraction of road freight should be shifted to waterborne transport in the future. In order to better consider this emission change pattern in future emission inventories, in the present study inland water transport emissions of NOx, CO2 and PM were investigated under real world conditions on the river Rhine, Germany, in 2013. An average NO2 ∕ NOx emission ratio of 0.08 ± 0.02 was obtained, which is indicative of ship diesel engines without exhaust gas aftertreatment systems. For all measured motor ship types and operation conditions, overall weighted average emission indices (EIs), as emitted mass of pollutant per kg burnt fuel of EINOx =  54 ± 4 g kg−1 and a lower limit EIPM1<mspace width="0.125em" linebreak="nobreak"/> ≥  2.0 ± 0.3 g kg−1, were obtained. EIs for NOx and PM1 were found to be in the range of 20–161 and ≥  0.2–8.1 g kg−1 respectively. A comparison with threshold values of national German guidelines shows that the NOx emissions of all investigated motor ship types are above the threshold values, while the obtained lower limit PM1 emissions are just under. To reduce NOx emissions to acceptable values, implementation of exhaust gas aftertreatment systems is recommended.
STEFLUX, a tool for investigating stratospheric intrusions: application to two WMO/GAW global stations

Stratospheric intrusion (SI) events are a topic of ongoing research, especially because of their ability to change the oxidation capacity of the troposphere and their contribution to tropospheric ozone levels. In this work, a novel tool called STEFLUX (Stratosphere-to-Troposphere Exchange Flux) is presented, discussed, and used to provide a first long-term investigation of SI over two global hot-spot regions for climate change and air pollution: the southern Himalayas and the central Mediterranean Basin. The main purpose of STEFLUX is to obtain a fast-computing and reliable identification of the SI events occurring at a specific location and during a specified time window. It relies on a compiled stratosphere-to-troposphere exchange (STE) climatology, which makes use of the ERA-Interim reanalysis dataset from the ECMWF, as well as a refined version of a well-established Lagrangian methodology. STEFLUX results are compared to the SI observations (SIO) at two high-mountain WMO/GAW global stations in these climate hot spots, i.e., the Nepal Climate Observatory-Pyramid (NCO-P, 5079 m a.s.l.) and Mt. Cimone (2165 m a.s.l.), which are often affected by SI events. Compared to the observational datasets at the two specific measurement sites, STEFLUX is able to detect SI events on a regional scale. Furthermore, it has the advantage of retaining additional information concerning the pathway of stratospheric-affected air masses, such as the location of tropopause crossing and other meteorological parameters along the trajectories. However, STEFLUX neglects mixing and dilution that air masses undergo along their transport within the troposphere. Therefore, the regional-scale STEFLUX events cannot be expected to perfectly reproduce the point measurements at NCO-P and Mt. Cimone, which are also affected by small-scale (orographic) circulations. Still, the seasonal variability in SI events according to SIO and STEFLUX agrees fairly well. By exploiting the fact that the ERA-Interim reanalysis extends back to 1979, the long-term climatology of SI events at NCO-P and Mt. Cimone is also assessed in this work. The analysis of the 35-year record at both stations denies the existence of any significant trend in the SI frequency, except for winter seasons at NCO-P. Furthermore, for the first time, by using the STEFLUX outputs, we investigate the potential impact of specific climate factors (i.e. ENSO, QBO, and solar activity) on SI frequency variability over the Mediterranean Basin and the Himalayas.
How do air ions reflect variations in ionising radiation in the lower atmosphere in a boreal forest?

Most of the ion production in the atmosphere is attributed to ionising radiation. In the lower atmosphere, ionising radiation consists mainly of the decay emissions of radon and its progeny, gamma radiation of the terrestrial origin as well as photons and elementary particles of cosmic radiation. These types of radiation produce ion pairs via the ionisation of nitrogen and oxygen as well as trace species in the atmosphere, the rate of which is defined as the ionising capacity. Larger air ions are produced out of the initial charge carriers by processes such as clustering or attachment to pre-existing aerosol particles. This study aimed (1) to identify the key factors responsible for the variability in ionising radiation and in the observed air ion concentrations, (2) to reveal the linkage between them and (3) to provide an in-depth analysis into the effects of ionising radiation on air ion formation, based on measurement data collected during 2003–2006 from a boreal forest site in southern Finland. In general, gamma radiation dominated the ion production in the lower atmosphere. Variations in the ionising capacity came from mixing layer dynamics, soil type and moisture content, meteorological conditions, long-distance transportation, snow cover attenuation and precipitation. Slightly similar diurnal patterns to variations in the ionising capacity were observed in air ion concentrations of the cluster size (0.8–1.7 nm in mobility diameters). However, features observed in the 0.8–1 nm ion concentration were in good connection to variations of the ionising capacity. Further, by carefully constraining perturbing variables, a strong dependency of the cluster ion concentration on the ionising capacity was identified, proving the functionality of ionising radiation in air ion production in the lower atmosphere. This relationship, however, was only clearly observed on new particle formation (NPF) days, possibly indicating that charges after being born underwent different processes on NPF days and non-event days and also that the transformation of newly formed charges to cluster ions occurred in a shorter timescale on NPF days than on non-event days.