Modelling trends in OH radical concentrations using generalized additive models

During the TORCH campaign a zero dimensional box model based on the Master Chemical Mechanism was used to model concentrations of OH radicals. The model provided a close overall fit to measured concentrations but with some significant deviations. In this research, an approach was established for applying Generalized Additive Models (GAM) to atmospheric concentration data. Two GAM models were fitted to OH radical concentrations using TORCH data, the first using measured OH data and the second using MCM model results. GAM models with five smooth functions provided a close fit to the data with 78% of the deviance explained for measured OH and 83% for modelled OH. The GAM model for measured OH produced substantially better predictions of OH concentrations than the original MCM model results. The diurnal profile of OH concentration was reproduced and the predicted mean diurnal OH concentration was only 0.2% less than the measured concentration compared to 16.3% over-estimation by the MCM model. Photolysis reactions were identified as most important in explaining concentrations of OH. The GAM models combined both primary and secondary pollutants and also anthropogenic and biogenic species to explain changes in OH concentrations. Differences identified in the dependencies of modelled and measured OH concentrations, particularly for aromatic and biogenic species, may help to understand why the MCM model predictions sometimes disagree with measurements of atmospheric species

Enhancement of marine cloud albedo via controlled sea spray injections: a global model study of the influence of emission rates, microphysics and transport

Modification of cloud albedo by controlled emission of sea spray particles into the atmosphere has been suggested as a possible geoengineering option to slow global warming. Previous global studies have imposed changes in cloud drop concentration in low level clouds to explore the radiative and climatic effects. Here, we use a global aerosol transport model to quantify how an imposed flux of sea spray particles affects the natural aerosol processes, the particle size distribution, and concentrations of cloud drops. We assume that the proposed fleet of vessels emits sea spray particles with a wind speed-dependent flux into four regions of persistent stratocumulus cloud off the western coasts of continents. The model results show that fractional changes in cloud drop number concentration (CDNC) vary substantially between the four regions because of differences in wind speed (which affects the spray efficiency of the vessels), transport and particle deposition rates, and because of variations in aerosols from natural and anthropogenic sources. Using spray emission rates comparable to those implied by previous studies we find that the predicted CDNC changes are very small (maximum 20%) and in one of the four regions even negative. The weak or negative effect is because the added particles suppress the in-cloud supersaturation and prevent existing aerosol particles from forming cloud drops. A scenario with five times higher emissions (considerably higher than previously assumed) increases CDNC on average by 45–163%, but median concentrations are still below the 375 cm<sup>−3</sup> assumed in previous studies. An inadvertent effect of the spray emissions is that sulphur dioxide concentrations are suppressed by 1–2% in the seeded regions and sulphuric acid vapour by 64–68% due to chemical reactions on the additional salt particles. The impact of this suppression on existing aerosol is negligible in the model, but should be investigated further in the real environment so that inadvertent impacts can be excluded

Fourier mode dynamics for the nonlinear Schroedinger equation in one-dimensional bounded domains

We analyze the 1D focusing nonlinear Schr\"{o}dinger equation in a finite interval with homogeneous Dirichlet or Neumann boundary conditions. There are two main dynamics, the collapse which is very fast and a slow cascade of Fourier modes. For the cubic nonlinearity the calculations show no long term energy exchange between Fourier modes as opposed to higher nonlinearities. This slow dynamics is explained by fairly simple amplitude equations for the resonant Fourier modes. Their solutions are well behaved so filtering high frequencies prevents collapse. Finally these equations elucidate the unique role of the zero mode for the Neumann boundary conditions

The impact of the 1783-1784 AD Laki eruption on global aerosol formation processes and cloud condensation nuclei

The 1783–1784 AD Laki flood lava eruption commenced on 8 June 1783 and released 122 Tg of sulphur dioxide gas over the course of 8 months into the upper troposphere and lower stratosphere above Iceland. Previous studies have examined the impact of the Laki eruption on sulphate aerosol and climate using general circulation models. Here, we study the impact on aerosol microphysical processes, including the nucleation of new particles and their growth to cloud condensation nuclei (CCN) using a comprehensive Global Model of Aerosol Processes (GLOMAP). Total particle concentrations in the free troposphere increase by a factor ~16 over large parts of the Northern Hemisphere in the 3 months following the onset of the eruption. Particle concentrations in the boundary layer increase by a factor 2 to 5 in regions as far away as North America, the Middle East and Asia due to long-range transport of nucleated particles. CCN concentrations (at 0.22% supersaturation) increase by a factor 65 in the upper troposphere with maximum changes in 3-month zonal mean concentrations of ~1400 cm<sup>−3</sup> at high northern latitudes. 3-month zonal mean CCN concentrations in the boundary layer at the latitude of the eruption increase by up to a factor 26, and averaged over the Northern Hemisphere, the eruption caused a factor 4 increase in CCN concentrations at low-level cloud altitude. The simulations show that the Laki eruption would have completely dominated as a source of CCN in the pre-industrial atmosphere. The model also suggests an impact of the eruption in the Southern Hemisphere, where CCN concentrations are increased by up to a factor 1.4 at 20° S. Our model simulations suggest that the impact of an equivalent wintertime eruption on upper tropospheric CCN concentrations is only about one-third of that of a summertime eruption. The simulations show that the microphysical processes leading to the growth of particles to CCN sizes are fundamentally different after an eruption when compared to the unperturbed atmosphere, underlining the importance of using a fully coupled microphysics model when studying long-lasting, high-latitude eruptions

The response of precipitation to aerosol through riming and melting in deep convective clouds

We have used a 2-D axisymmetric, non-hydrostatic, bin-resolved cloud model to examine the impact of aerosol changes on the development of mixed-phase convective clouds. We have simulated convective clouds from four different sites (three continental and one tropical marine) with a wide range of realistic aerosol loadings and initial thermodynamic conditions (a total of 93 different clouds). It is found that the accumulated precipitation responds very differently to changing aerosol in the marine and continental environments. For the continental clouds, the scaled total precipitation reaches a maximum for aerosol that produce drop numbers at cloud base between 180–430 cm<sup>−3</sup> when other conditions are the same. In contrast, all the tropical marine clouds show an increase in accumulated precipitation and deeper convection with increasing aerosol loading. For continental clouds, drops are rapidly depleted by ice particles shortly after the onset of precipitation. The precipitation is dominantly produced by melting ice particles. The riming rate increases with aerosol when the loading is very low, and decreases when the loading is high. Peak precipitation intensities tend to increase with aerosol up to drop concentrations (at cloud base) of ~500 cm<sup>−3</sup> then decrease with further aerosol increases. This behaviour is caused by the initial transition from warm to mixed-phase rain followed by reduced efficiency of mixed-phase rain at very high drop concentrations. The response of tropical marine clouds to increasing aerosol is different to, and larger than, that of continental clouds. In the more humid tropical marine environment with low cloud bases we find that accumulated precipitation increases with increasing aerosol. The increase is driven by the transition from warm to mixed-phase rain. Our study suggests that the response of deep convective clouds to aerosol will be an important contribution to the spatial and temporal variability in cloud microphysics and precipitation

Designing arrays of Josephson junctions for specific static responses

We consider the inverse problem of designing an array of superconducting Josephson junctions that has a given maximum static current pattern as function of the applied magnetic field. Such devices are used for magnetometry and as Terahertz oscillators. The model is a 2D semilinear elliptic operator with Neuman boundary conditions so the direct problem is difficult to solve because of the multiplicity of solutions. For an array of small junctions in a passive region, the model can be reduced to a 1D linear partial differential equation with Dirac distribution sine nonlinearities. For small junctions and a symmetric device, the maximum current is the absolute value of a cosine Fourier series whose coefficients (resp. frequencies) are proportional to the areas (resp. the positions) of the junctions. The inverse problem is solved by inverse cosine Fourier transform after choosing the area of the central junction. We show several examples using combinations of simple three junction circuits. These new devices could then be tailored to meet specific applications.Comment: The article was submitted to Inverse Problem

Effects of boundary layer particle formation on cloud droplet number and changes in cloud albedo from 1850 to 2000

We use a global aerosol microphysics model to estimate the effect of particle formation through activation nucleation in the boundary layer (BL) on cloud droplet number concentration (CDNC) on global and regional scales. The calculations are carried out for years 1850 and 2000 using historical emissions inventories for primary particles and aerosol precursor gases. Predicted CDNC in 2000 are in good agreement with in-situ observations when activation nucleation is included. We find that BL particle formation increases global annual mean CDNC by approximately the same relative amount in both years (16.0% in 1850 and 13.5% in 2000). As a result, global mean changes in cloud albedo are similar with and without BL particle formation. However, there are substantial regional effects of up to 50% enhancement or suppression of the 1850–2000 albedo change. Over most modern-day polluted northern hemisphere regions, including BL particle formation scheme suppresses the 1850–2000 increase in CDNC and cloud albedo because BL particle formation is already large in 1850. Over the Arctic the albedo change is suppressed by 23% in the annual mean and by 43% in summer when BL particle formation is taken into account. The albedo change of the persistent stratocumulus cloud deck west of Chile is enhanced by 49%

Factors controlling Arctic denitrification in cold winters of the 1990s

International audienceDenitrification of the Arctic winter stratosphere has been calculated using a 3-D microphysical model for the winters 1994/95, 1995/96, 1996/97 and 1999/2000. Denitrification is assumed to occur through the sedimentation of low number concentrations of large nitric acid trihydrate (NAT) particles, as observed extensively in 1999/2000. We examine whether the meteorological conditions that allowed NAT particles to grow to the very large sizes observed in 1999/2000 also occurred in the other cold winters. The results show that winter 1999/2000 had conditions that were optimum for denitrification by large NAT particles, which are a deep concentric cold pool and vortex. Under these conditions, NAT particles can circulate in the cold pool for several days, reaching several micrometres in radius and leading to a high downward flux of nitric acid. The other winters had shorter periods with optimum conditions for denitrification. However, we find that NAT particles could have grown to large sizes in all of these winters and could have caused significant denitrification. We define the quantity "closed flow area'' (the fraction of the cold pool in which air parcel trajectories can form closed loops) and show that it is a very useful indicator of possible denitrification. We find that even with a constant NAT nucleation rate throughout the cold pool, the average NAT number concentration and size can vary by up to a factor of 10 in response to this meteorological quantity. These changes in particle properties account for a high degree of variability in denitrification between the different winters. This large meteorologically induced variability in denitrification rate needs to be compared with that which could arise from a variable nucleation rate of NAT particles, which remains an uncertain quantity in models

Constraining uncertainty in aerosol direct forcing

The uncertainty in present-day anthropogenic forcing is dominated by uncertainty in the strength of the contribution from aerosol. Much of the uncertainty in the direct aerosol forcing can be attributed to uncertainty in the anthropogenic fraction of aerosol in the present-day atmosphere, due to a lack of historical observations. Here we present a robust relationship between total present-day aerosol optical depth and the anthropogenic contribution across three multi-model ensembles and a large single-model perturbed parameter ensemble. Using observations of aerosol optical depth, we determine a reduced likely range of the anthropogenic component and hence a reduced uncertainty in the direct forcing of aerosol

Polymer-mediated entropic forces between scale-free objects

The number of configurations of a polymer is reduced in the presence of a barrier or an obstacle. The resulting loss of entropy adds a repulsive component to other forces generated by interaction potentials. When the obstructions are scale invariant shapes (such as cones, wedges, lines or planes) the only relevant length scales are the polymer size R_0 and characteristic separations, severely constraining the functional form of entropic forces. Specifically, we consider a polymer (single strand or star) attached to the tip of a cone, at a separation h from a surface (or another cone). At close proximity, such that h<<R_0, separation is the only remaining relevant scale and the entropic force must take the form F=AkT/h. The amplitude A is universal, and can be related to exponents \eta governing the anomalous scaling of polymer correlations in the presence of obstacles. We use analytical, numerical and epsilon-expansion techniques to compute the exponent \eta for a polymer attached to the tip of the cone (with or without an additional plate or cone) for ideal and self-avoiding polymers. The entropic force is of the order of 0.1 pN at 0.1 micron for a single polymer, and can be increased for a star polymer.Comment: LaTeX, 15 pages, 4 eps figure