Very short-lived brominated substances (VSLBr) are an important source of stratospheric bromine, an effective ozone destruction catalyst. However, the accurate estimation of the organic and inorganic partitioning of bromine and the input to the stratosphere remains uncertain. Here, we report near-tropopause measurements of organic brominated substances found over the tropical Pacific during the NASA Airborne Tropical Tropopause Experiment campaigns. We combine aircraft observations and a chemistry−climate model to quantify the total bromine loading injected to the stratosphere. Surprisingly, despite differences in vertical transport between the Eastern and Western Pacific, VSLBr (organic + inorganic) contribute approximately similar amounts of bromine [∼6 (4−9) parts per thousand] to the stratospheric input at the tropical tropopause. These levels of bromine cause substantial ozone depletion in the lower stratosphere, and any increases in future abundances (e.g., as a result of aquaculture) will lead to larger depletions.

We have performed numerical simulations of inertial particles in random model flows in the white-noise limit (at zero Kubo number, Ku = 0) and at finite Kubo numbers. Our results for the moments of relative inertial-particle velocities are in good agreement with recent theoretical results (Gustavsson and Mehlig 2011a) based on the formation of phase-space singularities in the inertialparticle dynamics (caustics). We discuss the relation between three recent approaches describing the dynamics and spatial distribution of inertial particles suspended in turbulent flows: caustic formation, real-space singularities of the deformation tensor and random uncorrelated motion. We discuss how the phaseand real-space singularities are related. Their formation is well understood in terms of a local theory. We summarise the implications for random uncorrelated motion.

A full Lagrangian method (FLM) is used in direct numerical simulations (DNS) of incompressible homogeneous isotropic and statistically stationary turbulent flow to measure the statistical properties of the segregation of small inertial particles advected with Stokes drag by the flow. Qualitative good agreement is observed with previous kinematic simulations (KS) (IJzermans, Meneguz & Reeks, J. Fluid Mech., vol. 653, 2010, pp. 99–136): in particular, the existence of singularities in the particle concentration field and a threshold value for the particle Stokes number $\mathit{St}$ above which the net compressibility of the particle concentration changes sign (from compression to dilation). A further KS analysis is carried out by examining the distribution in time of the compression of an elemental volume of particles, which shows that it is close to Gaussian as far as the third and fourth moments but non-Gaussian (within the uncertainties of the measurements) for higher-order moments when the contribution of singularities in the tails of the distribution increasingly dominates the statistics. Measurements of the rate of occurrence of singularities show that it reaches a maximum at $\mathit{St}\ensuremath{\sim} 1$, with the distribution of times between singularities following a Poisson process. Following the approach used by Fevrier, Simonin & Squires (J. Fluid Mech., vol. 553, 2005, pp. 1–46), we also measured the random uncorrelated motion (RUM) and mesoscopic components of the compression for $\mathit{St}= 1$ and show that the non-Gaussian highly intermittent part of the distribution of the compression is associated with the RUM component and ultimately with the occurrence of singularities. This result is consistent with the formation of caustics (Wilkinson et al. Phys. Fluids, vol. 19, 2007, p. 113303), where the activation of singularities precedes the crossing of trajectories (RUM).

The results presented here are part of a long-term study in which we analyse the segregation of inertial particles in turbulent flows using the so called full Lagrangian method (FLM) to evaluate the ‘compressibility’ of the particle phase along a particle trajectory. In the present work, particles are advected by Stokes drag in a random flow field consisting of counter-rotating vortices and in a flow field composed of 200 random Fourier modes. Both flows are incompressible and, like turbulence, have structure and a distribution of scales with finite lifetime. The compressibility is obtained by first calculating the deformation tensor Jij associated with an infinitesimally small volume of particles following the trajectory of an individual particle. The fraction of the initial volume occupied by the particles centred around a position x at time t is denoted by |J|, where J ≡ det(Jij) and Jij ≡ ∂xi(x0, t)/∂x0,j, x0 denoting the initial position of the particle. The quantity d〈ln|J|〉/dt is shown to be equal to the particle averaged compressibility of the particle velocity field 〈∇ · v〉, which gives a measure of the rate-of-change of the total volume occupied by the particle phase as a continuum. In both flow fields the compressibility of the particle velocity field is shown to decrease continuously if the Stokes number St (the dimensionless particle relaxation time) is below a threshold value Stcr, indicating that the segregation of particles continues indefinitely. We show analytically and numerically that the long-time limit of 〈∇ · v〉 for sufficiently small values of St is proportional to St2 in the flow field composed of random Fourier modes, and to St in the flow field consisting of counter-rotating vortices. If St > Stcr, however, the particles are ‘mixed’. The level of mixing can be quantified by the degree of random uncorrelated motion (RUM) of particles which is a measure of the decorrelation of the velocities of two nearby particles. RUM is zero for fluid particles and increases rapidly with the Stokes number if St > Stcr, approaching unity for St ≫ 1. The spatial averages of the higher-order moments of the particle number density are shown to diverge with time indicating that the spatial distribution of particles may be very intermittent, being associated with non-zero values of RUM and the occurrence of singularities in the particle velocity field. Our results are consistent with previous observations of the radial distribution function in Chun et al. (J. Fluid Mech., vol. 536, 2005, p. 219).

Abstract. Anthropogenic emissions from East Asia have increased over recent decades. These increases have led to changes in atmospheric composition as far afield as North America under the prevailing westerly winds. Here we show that, during Northern Hemisphere (NH) winter, pollution originating in East Asia also directly affects atmospheric composition in the deep tropics. We present observations of marked intra-seasonal variability in the anthropogenic tracer perchloroethene (C 2 Cl 4 ) collected at two locations in Borneo (117.84 • E, 4.98 • N and 118.00 • E, 4.22 • N) during the NH winter of 2008/2009. We use trajectories calculated with the Numerical Atmospheric-dispersion Modelling Environment to show that the observed enhancements in C 2 Cl 4 mixing ratio are caused by rapid meridional transport, in the form of "cold surges", from the relatively polluted East Asian land mass. In these events air masses can move from ∼35 • N to Borneo in 4 days. We then present data from the Monitoring Atmospheric Composition and Climate reanalysis which suggest that air masses high in C 2 Cl 4 may also contain levels of the pollutants carbon monoxide and ozone that are approximately double the typical "background" levels in Borneo. In addition to strengthening the meridional transport from the north, cold surges can enhance convection in Southeast Asia, and further trajectory calculations indicate that the polluted air masses can subsequently be lifted to the tropical upper troposphere. This suggests a potentially important connection between midlatitude pollution sources and the very low stratosphere.

The main field activities of the Coordinated Airborne Studies in the Tropics (CAST) campaign took place in the west Pacific during January–February 2014. The field campaign was based in Guam (13.5°N, 144.8°E), using the U.K. Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 atmospheric research aircraft, and was coordinated with the Airborne Tropical Tropopause Experiment (ATTREX) project with an unmanned Global Hawk and the Convective Transport of Active Species in the Tropics (CONTRAST) campaign with a Gulfstream V aircraft. Together, the three aircraft were able to make detailed measurements of atmospheric structure and composition from the ocean surface to 20 km. These measurements are providing new information about the processes influencing halogen and ozone levels in the tropical west Pacific, as well as the importance of trace-gas transport in convection for the upper troposphere and stratosphere. The FAAM aircraft made a total of 25 flights in the region between 1°S and 14°N and 130° and 155°E. It was used to sample at altitudes below 8 km, with much of the time spent in the marine boundary layer. It measured a range of chemical species and sampled extensively within the region of main inflow into the strong west Pacific convection. The CAST team also made ground-based measurements of a number of species (including daily ozonesondes) at the Atmospheric Radiation Measurement Program site on Manus Island, Papua New Guinea (2.1°S, 147.4°E). This article presents an overview of the CAST project, focusing on the design and operation of the west Pacific experiment. It additionally discusses some new developments in CAST, including flights of new instruments on board the Global Hawk in February–March 2015.

Preferential concentration of inertial particles in turbulence is studied numerically by evaluating the Lagrangian compressibility of the particle velocity field using the "full Lagrangian method." This is compared with the "mesoscopic Eulerian particle velocity field" both in a direct numerical simulation of turbulence and in a synthetic flow field. We demonstrate that the Lagrangian method, in contrast to the Eulerian, accurately predicts the compressibility of the particle velocity field even when the latter is characterized by singularities. In particular we use the method to evaluate the growth rates of spatial moments of the particle number density which reflect the fractal structure of segregation and the occurrence of singularities.

It is well known that encounters with moderate or severe turbulence can lead to passenger and crew injuries and incur high insurance costs for airlines. Atmospheric convection is thought to induce a significant proportion of turbulence experienced by commercial aircraft, but its relative importance over Europe and the northeastern Atlantic Ocean area has not yet been quantified in a systematic way. In this study, a new approach is developed to automatically detect turbulent events associated with convective sources. Observations of convection over Europe and the northeastern Atlantic were obtained from the Met Office Arrival Time Detection system (ATDnet) and from Meteosat Second Generation satellite imagery. The system is run for all in situ reports of turbulence received from a commercial airline for two 6-month periods (summer 2013 and summer 2014). It is found that, as a monthly average, 14% of all aircraft encounters with turbulence occur in the proximity of a convective storm. These findings are interpreted and discussed together with the limitations of the system and observations that were used in this study.