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We present a newly developed global ocean mercury (Hg) transport and biogeochemistry model and use preanthropogenic equilibrium simulations to highlight physical and chemical processes which reveal significant knowledge gaps that need to be addressed. As with previous 3-D ocean Hg model work we use a bulk chemistry scheme based on particulate organic carbon remineralization. We also include an explicit methylation cycle based on available reaction rates. The methylation to demethylation rate ratio based on various field studies is found to be inconsistent with the concentration ratios measured in the Southern Ocean around Antarctica and in the Arctic. There is also model-measurement disagreement in the old waters of the tropical and North Pacific Ocean. The model produces an intermediate water maximum in total Hg in this region reflecting the higher age of water which is absent in observations. The model also underestimates total Hg concentrations in the deepest waters in this region. These disagreements in depth profile shape point to an inadequate representation of scavenging and sedimentation and possibly seabed emission or remobilization of Hg. In addition, the total Hg distribution differences compared to previous model work reflect sensitivity to ocean model transport characteristics and in particular the tracer diffusion. The residence time of Hg in the global ocean and the surface evasion flux of elemental Hg is sensitive to such model aspects. We find a global ocean Hg turnover time against sediment burial to be about 1100 years which is within the range of previous studies. [ABSTRACT FROM AUTHOR]

A new model for greenhouse gas transport has been developed based on Environment and Climate Change Canada's operational weather and environmental prediction models. When provided with realistic posterior fluxes for CO2, the CO2 simulations compare well to NOAA's CarbonTracker fields and to near-surface continuous measurements, columns from the Total Carbon Column Observing Network (TCCON) and NOAA aircraft profiles. This coupled meteorological and tracer transport model is used to study the predictability of CO2. Predictability concerns the quantification of model forecast errors and thus of transport model errors. CO2 predictions are used to compute model- data mismatches when solving flux inversion problems and the quality of such predictions is a major concern. Here, the loss of meteorological predictability due to uncertain meteorological initial conditions is shown to impact CO2 predictability. The predictability of CO2 is shorter than that of the temperature field and increases near the surface and in the lower stratosphere. When broken down into spatial scales, CO2 predictability at the very largest scales is mainly due to surface fluxes but there is also some sensitivity to the land and ocean surface forcing of meteorological fields. The predictability due to the land and ocean surface is most evident in boreal summer when biospheric uptake produces large spatial gradients in the CO2 field. This is a newly identified source of uncertainty in CO2 predictions but it is expected to be much less significant than uncertainties in fluxes. However, it serves as an upper limit for the more important source of transport error and loss of predictability, which is due to uncertain meteorological analyses. By isolating this component of transport error, it is demonstrated that CO2 can only be defined on large spatial scales due to the presence of meteorological uncertainty. Thus, for a given model, there is a spatial scale below which fluxes cannot be inferred simply due to the fact that meteorological analyses are imperfect. These unresolved spatial scales correspond to small scales near the surface but increase with altitude. By isolating other components of transport error, the largest or limiting error can be identified. For example, a model error due to the lack of convective tracer transport was found to impact transport error on the very largest (wavenumbers less than 5) spatial scales. Thus for wavenumbers greater than 5, transport model error due to meteorological analysis uncertainty is more important for our model than the lack of convective tracer transport. [ABSTRACT FROM AUTHOR]

A new model for greenhouse gas transport has been developed based on Environment and Climate Change Canada's operational weather and environmental prediction models. When provided with realistic posterior fluxes for CO2, the CO2 simulations compare well to NOAA's CarbonTracker fields, and to near surface continuous measurements, columns from the Total Carbon Column Observing Network (TCCON), and NOAA aircraft profiles. This coupled meteorological and tracer transport model is used to study the atmospheric modulation of CO2 transport. The predictability of CO2 due to initial state sensitivity is shorter than that for the temperature field but is consistent with the predictability of the wind fields. However, when broken down into spatial scales, CO2 has predictability at the very largest scales due to long time scale memory in surface CO2 fluxes as well as in land and ocean surface forcing of meteorological fields. The predictability due to the land and ocean surface is most evident in boreal summer when biospheric uptake produces large spatial gradients in the CO2 field. Predictability errors provide an upper limit for errors arising solely from the use of uncertain meteorological analyses. When considering meteorological analysis errors, CO2 can be defined only on large scales. Thus, there is a spatial scale below which information cannot be obtained simply due to the fact that meteorological analyses are imperfect. Compared to the spatial scales resolvable in the context of imperfect atmospheric analyses, the differences between two sets of posterior fluxes are resolvable only for very large scales. Similarly, the impact of convective tracer transport exceeds that due to atmospheric analysis errors for only the largest spatial scales. [ABSTRACT FROM AUTHOR]

In the tropical middle atmosphere the climatological radiative equilibrium temperature is inconsistent with gradient-wind balance and the available angular momentum, especially during solstice seasons. Adjustment toward a balanced state results in a type of Hadley circulation that lies outside the 'downward control' view of zonally averaged dynamics. This middle-atmosphere Hadley circulation is reexamined here using a zonally symmetric balance model driven through an annual cycle. It is found that the inclusion of a realistic radiation scheme leads to a concentration of the circulation near the stratopause and to its closing off in the mesosphere, with no need for relaxational damping or a rigid lid. The evolving zonal flow is inertially unstable, leading to a rapid process of inertial adjustment, which becomes significant in the mesosphere. This short-circuits the slower process of angular momentum homogenization by the Hadley circulation itself, thereby weakening the latter. The effect of the meridional circulation associated with extratropical wave drag on the Hadley circulation is considered. It is shown that the two circulations are independent for linear (quasigeostrophic) zonal-mean dynamics, and interact primarily through the advection of temperature and angular momentum. There appears to be no significant coupling in the deep Tropics via temperature advection since the wave-driven circulation is unable to alter meridional temperature gradients in this region. However, the wave-driven circulation can affect the Hadley circulation by advecting angular momentum out of the Tropics. The validity of the zonally symmetric balance model with parameterized inertial adjustment is tested by comparison with a three-dimensional primitive equations model. Fields from a middle-atmosphere GCM are also examined for evidence of these processes. While many aspects of the GCM circulation are indicative of the middle-atmosphere Hadley circulation, particularly in the upper stratosphere, it appears that the circulation is obscured in the mesosphere and lower stratosphere by other processes.

The dynamics of the tropical upwelling branch of the stratospheric Brewer-Dobson circulation are examined, with a particular focus on the role of the middle-atmosphere Hadley circulation. Upwelling is examined in terms of both the diabatic circulation and Lagrangian trajectories using a zonally symmetric balance model. The behavior of the wave-driven circulation in the presence of angular momentum redistribution by the Hadley circulation is also considered. The results of the zonally symmetric model are compared with fields from a middle-atmosphere GCM. It is found that the Hadley circulation makes a significant contribution to annual mean tropical upwelling at the upwelling maximum in the vicinity of the stratopause, and can account for most of the annual mean upwelling seen in the GCM. In the mid- to lower stratosphere, the role of the Hadley circulation is much weaker and wave drag appears to be required to explain the observed upwelling, although the Hadley circulation makes a nonnegligible contribution to the annual cycle of the upwelling. Subtropical wave drag can produce annual mean upwelling through a nonlinear mechanism; viscosity is not required. However, the magnitude of the observed upwelling suggests that wave drag must penetrate quite close to the equator.

A useful aerosol model must be able to adequately resolve the chemical complexity and phase state of the wide particle size range arising from the many different secondary aerosol growth processes to assess their environmental and health impacts. Over the past two decades, significant advances in understanding of gas-aerosol partitioning have occurred, particularly with respect to the role of organic compounds, yet aerosol representations have changed little in air quality and climate models since the late 1990s and early 2000s. The gas-aerosol partitioning models which are still commonly used in air quality models are separate inorganics-only thermodynamics and secondary organic aerosol (SOA) formation based on absorptive partitioning theory with an assumption of well-mixed liquid-like particles that continuously maintain equilibrium with the gas phase. These widely used approaches in air quality models for secondary aerosol composition and growth based on separated inorganic and organic processes are inadequate. This review summarizes some of the important developments during the past two decades in understanding of gas aerosol mass transfer processes. Substantial increases in computer performance in the last decade justify increasing the process detail in aerosol models. Organics play a central role during post-nucleation growth into the accumulation mode and change the hygroscopic properties of sulfate aerosol. At present, combined inorganic-organic aerosol thermodynamics models are too computationally expensive to be used online in 3-D simulations without high levels of aggregation of organics into a small number of functional surrogates. However, there has been progress in simplified modeling of liquid-liquid phase separation (LLPS) and distinct chemical regimes within organic-rich and inorganic-rich phases. Additional limitations of commonly used thermodynamics models are related to lack of surface tension data for various aerosol compositions in the small size limit, and lack of a comprehensive representation of surface interaction terms such as disjoining pressure in the Gibbs free energy which become significant in the small size limit and which affect both chemical composition and particle growth. As a result, there are significant errors in modeling of hygroscopic growth and phase transitions for particles in the nucleation and Aitken modes. There is also increasing evidence of reduced bulk diffusivity in viscous organic particles and, therefore, traditional secondary organic aerosol models, which are typically based on the assumption of instantaneous equilibrium gas-particle partitioning and neglect the kinetic effects, are no longer tenable. [ABSTRACT FROM AUTHOR]