Statistical inference of OH concentrations and air mass dilution rates from successive observations of non-methane hydrocarbons in single air masses

Bayesian inference has been used to determine rigorous estimates of hydroxyl radical concentrations () and air mass dilution rates (K) averaged following air masses between linked observations of nonmethane hydrocarbons (NMHCs) spanning the North Atlantic during the Intercontinental Transport and Chemical Transformation (ITCT)-Lagrangian-2K4 experiment. The Bayesian technique obtains a refined (posterior) distribution of a parameter given data related to the parameter through a model and prior beliefs about the parameter distribution. Here, the model describes hydrocarbon loss through OH reaction and mixing with a background concentration at rate K. The Lagrangian experiment provides direct observations of hydrocarbons at two time points, removing assumptions regarding composition or sources upstream of a single observation. The estimates are sharpened by using many hydrocarbons with different reactivities and accounting for their variability and measurement uncertainty. A novel technique is used to construct prior background distributions of many species, described by variation of a single parameter . This exploits the high correlation of species, related by the first principal component of many NMHC samples. The Bayesian method obtains posterior estimates of , K and following each air mass. Median values are typically between 0.5 and 2.0 �� 106 molecules cm���3, but are elevated to between 2.5 and 3.5 �� 106 molecules cm���3, in low-level pollution. A comparison of estimates from absolute NMHC concentrations and NMHC ratios assuming zero background (the ���photochemical clock��� method) shows similar distributions but reveals systematic high bias in the estimates from ratios. Estimates of K are ���0.1 day���1 but show more sensitivity to the prior distribution assumed.

Origins of dry air in the Tropics and Subtropics

The humidity in the dry regions of the tropical and subtropical troposphere has a major impact on the ability of the atmosphere to radiate heat to space. The water vapour content in these regions is determined by their ``origins'', here defined as the last condensation event following air masses. Trajectory simulations are used to investigate such origins using ERA40 data for January 1993. It is shown that 96% of air parcels experience condensation within 24 days and most of the remaining 4% originate in the stratosphere. Dry air masses are shown to experience a net pressure increase since last condensation which is uniform with latitude, while the median time taken for descent is 5 days into the subtropics but exceeds 16 days into the equatorial lower troposphere. The associated rate of decrease in potential temperature is consistent with radiative cooling. The relationship between the drier regions in the tropics and subtropics and the geographical localization of their origin is investigated. Four transport processes are identified to explain these relationships.

Precipitating convection in cold air: virtual potential temperature structure

Simulations of precipitating convection are used to illustrate the importance of the turbulent kinetic energy (TKE) budget in determining the virtual potential-temperature structure of the convecting atmosphere. Two sets of simulations are presented: in one the surface temperature was increased to simulate cold air flowing over a warmer surface and in the second a cooling profile, representing cold-air advection, was imposed. It is shown that the terms in the TKE budgets for both sets of simulations scale in the same way, but that the non-dimensional profiles are different. It is suggested that this is associated with the effects of sublimation of ice. It is shown that the magnitudes of the transport and precipitation terms in the virtual potential temperature budget are determined by the scaling of the TKE budget. Some implications of these results for parametrizations of moist convection are discussed. Copyright �� 2007 Royal Meteorological Society

Lagrangian analysis of low level anthropogenic plume processing across the North Atlantic

The photochemical evolution of an anthropogenic plume from the New-York/Boston region during its transport at low altitudes over the North Atlantic to the European west coast has been studied using a Lagrangian framework. This plume, originally strongly polluted, was sampled by research aircraft just off the North American east coast on 3 successive days, and 3 days downwind off the west coast of Ireland where another aircraft re-sampled a weakly polluted plume. Changes in trace gas concentrations during transport were reproduced using a photochemical trajectory model including deposition and mixing effects. Chemical and wet deposition processing dominated the evolution of all pollutants in the plume. The mean net O3 production was evaluated to be -5 ppbv/day leading to low values of O3 by the time the plume reached Europe. Wet deposition of nitric acid was responsible for an 80% reduction in this O3 production. If the plume had not encountered precipitation, it would have reached the Europe with O3 levels up to 80-90 ppbv, and CO levels between 120 and 140 ppbv. Photochemical destruction also played a more important role than mixing in the evolution of plume CO due to high levels of both O3 and water vapour showing that CO cannot always be used as a tracer for polluted air masses, especially for plumes transported at low altitudes. The results also show that, in this case, an important increase in the O3/CO slope can be attributed to chemical destruction of CO and not to photochemical O3 production as is often assumed.

Boundary-layer ventilation by baroclinic lifecycles

Ventilation of the boundary layer has an important effect on local and regional air quality and is a prerequisite for long-range pollution transport. Once in the free troposphere, pollutants can alter the chemical composition of the troposphere and impact on the Earth's radiative forcing. Idealised baroclinic life cycles, LC1 and LC2, have been simulated in a three-dimensional dry hemispheric model in the presence of boundary-layer turbulent fluxes. A passive tracer is added to the simulations to represent pollution emitted at, or near, the surface. A simple conveyor-belt diagnostic is developed to objectively identify regions of the boundary layer that can be ventilated by either warm or cold conveyor belts. Transport of pollutants within and above the boundary layer is examined on synoptic scales. Three different physical mechanisms are found to interact with each other to ventilate pollutants out of the boundary layer. These mechanisms are turbulent mixing within the boundary layer, horizontal advection due to Ekman convergence and divergence within the boundary layer, and advection by the warm conveyor belt. The mass of tracer ventilated by the two life cycles is remarkably similar given the differences in frontal structure, suggesting that the large-scale baroclinicity is an effective constraint on ventilation.

A double-Gerdien instrument for simultaneous bipolar air conductivity measurements on balloon platforms

A bipolar air conductivity instrument is described for use with a standard disposable meteorological radiosonde package. It is intended to provide electrical measurements at cloud boundaries, where the ratio of the bipolar air conductivities is affected by the presence of charged particles. The sensors are two identical Gerdien-type electrodes, which, through a voltage decay method, measure positive and negative air conductivities simultaneously. Voltage decay provides a thermally stable approach and a novel low current leakage electrometer switch is described which initiates the decay sequence. The radiosonde supplies power and telemetry, as well as measuring simultaneous meteorological data. A test flight using a tethered balloon determined positive (��+) and negative (�����) conductivities of ��+ = 2.77��0.2���fS���m���1 and ����� = 2.82��0.2���fS���m���1, respectively, at 400���m aloft, with ��+/����� = 0.98��0.04.

Air-earth current density measurements at Lerwick; implications for seasonality in the global electric circuit

Atmospheric electricity measurements were made at Lerwick Observatory in the Shetland Isles (60��09���N, 1��08���W) during most of the 20th century. The Potential Gradient (PG) was measured from 1926 to 84 and the air-earth conduction current (Jc) was measured during the final decade of the PG measurements. Daily Jc values (1978���1984) observed at 15 UT are presented here for the first time, with independently-obtained PG measurements used to select valid data. The 15 UT Jc (1978���1984) spans 0.5���9.5 pA/m2, with median 2.5 pA/m2; the columnar resistance at Lerwick is estimated as 70 P��m2. Smoke measurements confirm the low pollution properties of the site. Analysis of the monthly variation of Lerwick Jc data shows that winter (DJF) Jc is significantly greater than the summer (JJA) Jc by 20%. The Lerwick atmospheric electricity seasonality differs from the global lightning seasonality, but Jc has a similar seasonal phasing to that observed in Nimbostratus clouds globally, suggesting a role for non-thunderstorm rain clouds in the seasonality of the global circuit.

Application of the Lighthill-Ford theory of spontaneous imbalance to clear-air turbulence forecasting

A new method of clear-air turbulence (CAT) forecasting based on the Lighthill���Ford theory of spontaneous imbalance and emission of inertia���gravity waves has been derived and applied on episodic and seasonal time scales. A scale analysis of this shallow-water theory for midlatitude synoptic-scale flows identifies advection of relative vorticity as the leading-order source term. Examination of leading- and second-order terms elucidates previous, more empirically inspired CAT forecast diagnostics. Application of the Lighthill���Ford theory to the Upper Mississippi and Ohio Valleys CAT outbreak of 9 March 2006 results in good agreement with pilot reports of turbulence. Application of Lighthill���Ford theory to CAT forecasting for the 3 November 2005���26 March 2006 period using 1-h forecasts of the Rapid Update Cycle (RUC) 2 1500 UTC model run leads to superior forecasts compared to the current operational version of the Graphical Turbulence Guidance (GTG1) algorithm, the most skillful operational CAT forecasting method in existence. The results suggest that major improvements in CAT forecasting could result if the methods presented herein become operational.