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We present the results of idealized numerical experiments to examine the difference between tropical cyclone evolution in three-dimensional (3-D) and axisymmetric (AX) model configurations. We focus on the prototype problem for intensification, which considers the evolution of an initially unsaturated AX vortex in gradient-wind balance on an <i>f</i> plane. Consistent with findings of previous work, the mature intensity in the 3-D model is reduced relative to that in the AX model. In contrast with previous interpretations invoking barotropic instability and related horizontal mixing processes as a mechanism detrimental to the spin-up process, the results indicate that 3-D eddy processes associated with vortical plume structures can assist the intensification process by contributing to a radial contraction of the maximum tangential velocity and to a vertical extension of tangential winds through the depth of the troposphere. These plumes contribute significantly also to the azimuthally averaged heating rate and the corresponding azimuthal-mean overturning circulation. <br><br> The comparisons show that the resolved 3-D eddy momentum fluxes above the boundary layer exhibit counter-gradient characteristics during a key spin-up period, and more generally are not solely diffusive. The effects of these eddies are thus not properly represented by the subgrid-scale parameterizations in the AX configuration. The resolved eddy fluxes act to support the contraction and intensification of the maximum tangential winds. The comparisons indicate fundamental differences between convective organization in the 3-D and AX configurations for meteorologically relevant forecast timescales. While the radial and vertical gradients of the system-scale angular rotation provide a hostile environment for deep convection in the 3-D model, with a corresponding tendency to strain the convective elements in the tangential direction, deep convection in the AX model does not suffer this tendency. Also, since during the 3-D intensification process the convection has not yet organized into annular rings, the azimuthally averaged heating rate and radial gradient thereof is considerably less than that in the AX model. This lack of organization results broadly in a slower intensification rate in the 3-D model and leads ultimately to a weaker mature vortex after 12 days of model integration. While azimuthal mean heating rates in the 3-D model are weaker than those in the AX model, local heating rates in the 3-D model exceed those in the AX model and at times the vortex in the 3-D model intensifies more rapidly than AX. Analyses of the 3-D model output do not support a recent hypothesis concerning the key role of small-scale vertical mixing processes in the upper-tropospheric outflow in controlling the intensification process. <br><br> In the 3-D model, surface drag plays a particularly important role in the intensification process for the prototype intensification problem on meteorologically relevant timescales by helping foster the organization of convection in azimuth. There is a radical difference in the behaviour of the 3-D and AX simulations when the surface drag is reduced or increased from realistic values. Borrowing from ideas developed in a recent paper, we give a partial explanation for this difference in behaviour. <br><br> Our results provide new qualitative and quantitative insight into the differences between the asymmetric and symmetric dynamics of tropical cyclones and would appear to have important consequences for the formulation of a fluid dynamical theory of tropical cyclone intensification and mature intensity. In particular, the results point to some fundamental limitations of strict axisymmetric theory and modelling for representing the azimuthally averaged behaviour of tropical cyclones in three dimensions.
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The objective of this paper is to deliver the most accurate ozone (O<sub>3</sub>) and carbon monoxide (CO) climatology for the pure troposphere only, i.e. exclusively from the ground to the dynamical tropopause on an individual profile basis. The results (profiles and columns) are derived solely from the <b>M</b>easurements of <b>OZ</b>one and water vapour by in-service <b>Al</b>rbus air<b>C</b>raft programme (MOZAIC) over 15 years (1994–2009). The study, focused on the northern mid-latitudes [24–50° N] and [119° W–140° E], includes more than 40 000 profiles over 11 sites to give a quasi-global zonal picture. Considering all the sites, the pure tropospheric column peak-to-peak seasonal cycle ranges are 23.7–43.2 DU for O<sub>3</sub> and 1.7–6.9 × 10 <sup>18</sup> molecules cm<sup>−2</sup> for CO. The maxima of the seasonal cycles are not in phase, occurring in February–April for CO and May–July for O<sub>3</sub>. The phase shift is related to the photochemistry and OH removal efficiencies. The purely tropospheric seasonal profiles are characterized by a typical autumn–winter/spring–summer O<sub>3</sub> dichotomy (except in Los Angeles, Eastmed – a cluster of Cairo and Tel Aviv – and the regions impacted by the summer monsoon) and a summer–autumn/winter–spring CO dichotomy. We revisit the boundary-layer, mid-tropospheric (MT) and upper-tropospheric (UT) partial columns using a~new monthly varying MT ceiling. Interestingly, the seasonal cycle maximum of the UT partial columns is shifted from summer to spring for O<sub>3</sub> and to very early spring for CO. Conversely, the MT maximum is shifted from spring to summer and is associated with a summer (winter) MT thickening (thinning). Lastly, the pure tropospheric seasonal cycles derived from our analysis are consistent with the cycles derived from spaceborne measurements, the correlation coefficients being <i>r</i>=0.6–0.9 for O<sub>3</sub> and <i>r</i>>0.9 for CO. The cycles observed from space are nevertheless greater than MOZAIC for O<sub>3</sub> (by 9–18 DU) and smaller for CO (up to 1 × 10 <sup>18</sup> molecules cm<sup>−2</sup>). The larger winter O<sub>3</sub> difference between the two data sets suggests probable stratospheric contamination in satellite data due to the tropopause position. The study underlines the importance of rigorously discriminating between the stratospheric and tropospheric reservoirs and avoiding use of a~monthly averaged tropopause position without this strict discrimination in order to assess the pure O<sub>3</sub> and CO tropospheric trends.
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Light absorbing organic carbon, often called brown carbon, has the potential to significantly contribute to the visible light-absorption budget, particularly at shorter wavelengths. Currently, the relative contributions of particulate brown carbon to light absorption, as well as the sources of brown carbon, are poorly understood. With this in mind size-resolved direct measurements of brown carbon were made at both urban (Atlanta), and rural (Yorkville) sites in Georgia. Measurements in Atlanta were made at both a representative urban site and a road-side site adjacent to a main highway. Fine particle absorption was measured with a multi-angle absorption photometer (MAAP) and seven-wavelength Aethalometer, and brown carbon absorption was estimated based on Mie calculations using direct size-resolved measurements of chromophores in solvents. Size-resolved samples were collected using a cascade impactor and analyzed for water-soluble organic carbon (WSOC), organic and elemental carbon (OC and EC), and solution light-absorption spectra of water and methanol extracts. Methanol extracts were more light-absorbing than water extracts for all size ranges and wavelengths. Absorption refractive indices of the organic extracts were calculated from solution measurements for a range of wavelengths and used with Mie theory to predict the light absorption by fine particles comprised of these components, under the assumption that brown carbon and other aerosol components were externally mixed. For all three sites, chromophores were predominately in the accumulation mode with an aerodynamic mean diameter of 0.5 μm, an optically effective size range resulting in predicted particle light absorption being a factor of 2 higher than bulk solution absorption. Mie-predicted brown carbon absorption at 350 nm contributed a significant fraction (20 to 40%) relative to total light absorption, with the highest contributions at the rural site where organic to elemental carbon ratios were highest. Brown carbon absorption, however, was highest by the roadside site due to vehicle emissions. The direct size-resolved measurement of brown carbon in solution definitively shows that it is present and optically important in the near-UV range in both a rural and urban environment during the summer when biomass burning emissions are low. These results allow estimates of brown carbon aerosol absorption from direct measurements of chromophores in aerosol extracts.
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Unique measurements of vertical size-resolved aerosol particle concentrations, trace gas concentrations and meteorological data were obtained during the Arctic Summer Cloud Ocean Study (ASCOS, <a href="http://www.ascos.se"target="_blank"> www.ascos.se</a>), an International Polar Year project aimed at establishing the processes responsible for formation and evolution of low-level clouds over the high Arctic summer pack ice. The experiment was conducted from on board the Swedish icebreaker <i>Oden</i>, and provided both ship- and helicopter-based measurements. This study focuses on the vertical helicopter profiles and onboard measurements obtained during a three-week period when <i>Oden</i> was anchored to a drifting ice floe, and sheds light on the characteristics of Arctic aerosol particles and their distribution throughout the lower atmosphere. <br><br> Distinct differences in aerosol particle characteristics within defined atmospheric layers are identified. Within the lowermost couple hundred metres, transport from the marginal ice zone (MIZ), condensational growth and cloud processing develop the aerosol population. During two of the four representative periods defined in this study, such influence is shown. At altitudes above about 1 km, long-range transport occurs frequently. However, only infrequently does large-scale subsidence descend such air masses to become entrained into the mixed layer in the high Arctic, and therefore long-range transport plumes are unlikely to directly influence low-level stratiform cloud formation. Nonetheless, such plumes can influence the radiative balance of the planetary boundary layer (PBL) by influencing formation and evolution of higher clouds, as well as through precipitation transport of particles downwards. New particle formation was occasionally observed, particularly in the near-surface layer. We hypothesize that the origin of these ultrafine particles could be in biological processes, both primary and secondary, within the open leads between the pack ice and/or along the MIZ. In general, local sources, in combination with upstream boundary-layer transport of precursor gases from the MIZ, are considered to constitute the origin of cloud condensation nuclei (CCN) particles and thus be of importance for the formation of interior Arctic low-level clouds during summer, and subsequently, through cloud influences, for the melting and freezing of sea ice.
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Observation shows that eastern China experienced an interdecadal shift in the summer precipitation during the second half of the 20th century. The summer precipitation increased in the middle and lower reaches of the Yangtze River valley, whereas it decreased in northern China. Here we use a coupled ocean–atmosphere general circulation model and multi-ensemble simulations to show that the interdecadal shift is mainly caused by the anthropogenic forcing. The rapidly increasing greenhouse gases induce a notable Indian Ocean warming, causing a westward shift of the western Pacific subtropical high (WPSH) and a southward displacement of the East Asia westerly jet (EAJ) on an interdecadal timescale, leading to more precipitation in Yangtze River valley. At the same time the surface cooling effects from the stronger convection, higher precipitation and rapidly increasing anthropogenic aerosols contribute to a reduced summer land–sea thermal contrast. Due to the changes in the WPSH, the EAJ and the land–sea thermal contrast, the East Asian summer monsoon weakened resulting in drought in northern China. Consequently, an anomalous precipitation pattern started to emerge over eastern China in the late 1970s. According to the model, the natural forcing played an opposite role in regulating the changes in WPSH and EAJ, and postponed the anthropogenically forced climate changes in eastern China. The Indian Ocean sea surface temperature is crucial to the response, and acts as a bridge to link the external forcings and East Asian summer climate together on a decadal and longer timescales. Our results further highlight the dominant roles of anthropogenic forcing agents in shaping interdecadal changes of the East Asian climate during the second half of the 20th century.
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Stratosphere-to-troposphere transport (STT) results in air masses of stratospheric origin intruding into the free troposphere. Once in the free troposphere, ozone (O<sub>3</sub>)-rich stratospheric air can be transported and mixed with tropospheric air masses, contributing to the tropospheric O<sub>3</sub> budget. Evidence of STT can be identified based on the differences in the trace gas composition of the two regions. Because O<sub>3</sub> is present in such large quantities in the stratosphere compared to the troposphere, it is frequently used as a tracer for STT events. <br><br> This work reports on airborne in situ measurements of O<sub>3</sub> and other trace gases during two STT events observed over California, USA. The first, on 14 May 2012, was associated with a cutoff low, and the second, on 5 June 2012, occurred during a post-trough, building ridge event. In each STT event, airborne measurements identified high O<sub>3</sub> within the stratospheric intrusion, which were observed as low as 3 km above sea level. During both events the stratospheric air mass was characterized by elevated O<sub>3</sub> mixing ratios and reduced carbon dioxide (CO<sub>2</sub>) and water vapor. The reproducible observation of reduced CO<sub>2</sub> within the stratospheric air mass supports the use of non-conventional tracers as an additional method for detecting STT. A detailed meteorological analysis of each STT event is presented, and observations are interpreted with the Realtime Air Quality Modeling System (RAQMS). The implications of the two STT events are discussed in terms of the impact on the total tropospheric O<sub>3</sub> budget and the impact on air quality and policy-making.
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Long-term measurements of particle number size distributions were carried out both at an urban background site (Peking University, PKU) and a regional Global Atmospheric Watch station (Shangdianzi, SDZ) from March to November in 2008. In total, 52 new particle formation (NPF) events were observed simultaneously at both sites, indicating that this is a regional phenomenon in the North China Plain. On average, the mean condensation sink value before the nucleation events started was 0.025 s<sup>−1</sup> in the urban environment, which was 1.6 times higher than that at regional site. However, higher particle formation and growth rates were observed at PKU (10.8 cm<sup>−3</sup> s<sup>−1</sup> and 5.2 nm h<sup>−1</sup>) compared with those at SDZ (4.9 cm<sup>−3</sup> </sup> s<sup>−1</sup> and 4.0 nm h<sup>−1</sup>). These results implied that precursors were much more abundant in the polluted urban environment. Different from the observations in cleaner environments, the background conditions of the observed particle homogeneous nucleation events in the North China Plain could be characterized as the co-existing of a stronger source of precursor gases and a higher condensational sink of pre-existing aerosol particles. Secondary aerosol formation following nucleation events results in an increase of particle mass concentration, particle light scattering coefficient, and cloud condensation nuclei (CCN) number concentration, with consequences on visibility, radiative effects, and air quality. Typical regional NPF events with significant particle nucleation rates and subsequent particle growth over a sufficiently long time period at both sites were chosen to investigate the influence of NPF on the number concentration of "potential" CCN. As a result, the NPF and the subsequent condensable growth increased the CCN number concentration in the North China Plain by factors in the range from 5.6 to 8.7. Moreover, the potential contribution of anthropogenic emissions to the CCN number concentration was more than 50%, to which more attention should be drawn in regional and global climate modeling, especially in the polluted urban areas.
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Climatic effects of newly-formed atmospheric secondary aerosol particles are to a large extent determined by their condensational growth rates. However, all the vapours condensing on atmospheric nanoparticles and growing them to climatically relevant sizes are not identified yet and the effects of particle phase processes on particle growth rates are poorly known. Besides sulfuric acid, organic compounds are known to contribute significantly to atmospheric nanoparticle growth. In this study a particle growth model MABNAG (Model for Acid-Base chemistry in NAnoparticle Growth) was developed to study the effect of salt formation on nanoparticle growth, which has been proposed as a potential mechanism lowering the equilibrium vapour pressures of organic compounds through dissociation in the particle phase and thus preventing their evaporation. MABNAG is a model for monodisperse aqueous particles and it couples dynamics of condensation to particle phase chemistry. Non-zero equilibrium vapour pressures, with both size and composition dependence, are considered for condensation. The model was applied for atmospherically relevant systems with sulfuric acid, one organic acid, ammonia, one amine and water in the gas phase allowed to condense on 3–20 nm particles. The effect of dissociation of the organic acid was found to be small under ambient conditions typical for a boreal forest site, but considerable for base-rich environments (gas phase concentrations of about 10<sup>10</sup> cm<sup>−3</sup> for the sum of the bases). The contribution of the bases to particle mass decreased as particle size increased, except at very high gas phase concentrations of the bases. The relative importance of amine versus ammonia did not change significantly as a function of particle size. While our results give a reasonable first estimate on the maximum contribution of salt formation to nanoparticle growth, further studies on, e.g. the thermodynamic properties of the atmospheric organics, concentrations of low-volatility organics and amines, along with studies investigating the applicability of thermodynamics for the smallest nanoparticles are needed to truly understand the acid-base chemistry of atmospheric nanoparticles.
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In situ measurements of carbon monoxide (CO) and ozone (O<sub>3</sub>) at the Pico Mountain Observatory (PMO) located in the Azores, Portugal, are analyzed together with results from an atmospheric chemical transport model (GEOS-Chem) and satellite remote sensing data (AIRS (Atmospheric Infrared Sounder) for CO, and TES (Tropospheric Emission Spectrometer) for O<sub>3</sub>) to examine the evolution of free-troposphere CO and O<sub>3</sub> over the North Atlantic for 2001–2011. GEOS-Chem captured the seasonal cycles for CO and O<sub>3</sub> well but significantly underestimated the mixing ratios of CO, particularly in spring. Statistically significant (using a significance level of 0.05) decreasing trends were found for both CO and O<sub>3</sub> based on harmonic regression analysis of the measurement data. The best estimates of the possible trends for CO and O<sub>3</sub> measurements are −0.31 ± 0.30 (2-σ) ppbv yr<sup>−1</sup> and −0.21 ± 0.11 (2-σ) ppbv yr<sup>−1</sup>, respectively. Similar decreasing trends for both species were obtained with GEOS-Chem simulation results. The most important factor contributing to the decreases in CO and O<sub>3</sub> at PMO over the past decade is the decline in anthropogenic emissions from North America, which more than compensate for the impacts from increasing Asian emissions. It is likely that climate change in the past decade has also affected the intercontinental transport of O<sub>3</sub>.
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A comprehensive general circulation model including ice supersaturation is used to estimate the climate impact of aviation induced contrails. The model uses a realistic aviation emissions inventory for 2006 to initiate contrails, and allows them to evolve consistently with the model hydrologic cycle. <br><br> The radiative forcing from linear contrails is very sensitive to the diurnal cycle. For linear contrails, including the diurnal cycle of air traffic reduces the estimated radiative forcing by 29%, and for contrail cirrus estimates, the radiative forcing is reduced by 25%. Estimated global radiative forcing from linear contrails is 0.0031 ± 0.0005 Wm<sup>−2</sup>. The linear contrail radiative forcing is found to exhibit a strong diurnal cycle. The contrail cirrus radiative forcing is less sensitive to the diurnal cycle of flights. The estimated global radiative forcing from contrail cirrus is 0.013 ± 0.01 Wm<sup>−2</sup>. Over regions with the highest air traffic, the regional effect can be as large as 1 Wm<sup>−2</sup>.