Development of a nonlocal convective mixing scheme with varying upward mixing rates for use in air quality and chemical transport models

BACKGROUND, AIM, AND SCOPE: Asymmetrical convective non-local scheme (CON) with varying upward mixing rates is developed for simulation of vertical turbulent mixing in the convective boundary layer in air quality and chemical transport models. MATERIALS AND METHODS: The upward mixing rate form the surface layer is parameterized using the sensible heat flux and the friction and convective velocities. Upward mixing rates varying with height are scaled with an amount of turbulent kinetic energy in layer, while the downward mixing rates are derived from mass conservation. RESULTS: This scheme provides a less rapid mass transport out of surface layer into other layers than other asymmetrical convective mixing schemes. DISCUSSION: In this paper, we studied the performance of a nonlocal convective mixing scheme with varying upward mixing in the atmospheric boundary layer and its impact on the concentration of pollutants calculated with chemical and air-quality models. This scheme was additionally compared versus a local eddy-diffusivity scheme (KSC). Simulated concentrations of NO(2) and the nitrate wet deposition by the CON scheme are closer to the observations when compared to those obtained from using the KSC scheme. CONCLUSIONS: Concentrations calculated with the CON scheme are in general higher and closer to the observations than those obtained by the KSC scheme (of the order of 15-20%). Nitrate wet deposition calculated with the CON scheme are in general higher and closer to the observations than those obtained by the KSC scheme. RECOMMENDATIONS AND PERSPECTIVES: To examine the performance of the scheme, simulated and measured concentrations of a pollutant (NO(2)) and nitrate wet deposition was compared for the year 2002. The comparison was made for the whole domain used in simulations performed by the chemical European Monitoring and Evaluation Programme Unified model (version UNI-ACID, rv2.0) where schemes were incorporated.     

Impacts of boundary layer mixing on pollutant vertical profiles in the lower troposphere: Implications to satellite remote sensing

Mixing in the planetary boundary layer (PBL) affects vertical distributions of air tracers in the lower troposphere. An accurate representation of PBL mixing is critical for chemical-transport models (CTMs) for applications sensitive to simulations of the vertical profiles of tracers. The full mixing assumption in the widely used global CTM GEOS-Chem has recently been supplemented with a non-local PBL scheme. This study analyzes the impact of the non-local scheme on model representation of PBL mixing, consequences for simulations of vertical profiles of air tracers and surface air pollution, and implications for model applications to the interpretation of data retrieved from satellite remote sensing. The non-local scheme significantly improves simulations of the vertical distributions for NO₂ and O₃, as evaluated using aircraft measurements in summer 2004. It also reduces model biases over the U.S. by more than 10 ppb for surface ozone concentrations at night and by 2–5 ppb for peak ozone in the afternoon, as evaluated using ground observations. The application to inverse modeling of anthropogenic NO_x emissions for East China using satellite retrievals of NO₂ from OMI and GOME-2 suggests that the full mixing assumption results in 3–14% differences in top–down emission budgets as compared to the non-local scheme. The top–down estimate combining the non-local scheme and the Lin et al. inverse modeling approach suggests a magnitude of 6.6 TgN yr^?1 for emissions of NO_x over East China in July 2008 and 8.0 TgN yr^?1 for January 2009, with the magnitude and seasonality in good agreement with bottom–up estimates.     

Vertical distribution of hydrocarbons in the low troposphere below and above the mixing height: tethered balloon measurements in Milan, Italy

A novel approach for measuring vertical profiles of HCs and particle number concentrations was described and applied in the low troposphere over Milan (Italy) during typical spring and summer days. Particle profiles yielded nearly homogeneous concentrations below the mixing height, with level-to-ground concentration ratios of 92-97%, while HCs showed a more pronounced decrease (74-95%). Vertical mixing and photochemical loss of HCs were demonstrated to cause these gradients. Much lower concentrations were observed for the profiles above the mixing height, where the HC mixtures showed also a different composition, which was partially explained by the horizontal advection of air with HC sources different to those prevailing at the site. The application of pseudo-first order kinetics for reactions between HCs and the hydroxyl radical allowed for the estimation of the vertical mixing time scale in the order of 100 ± 20 min.     

Employing Heisenberg's turbulent spectral transfer theory to parameterize sub-filter scales in LES models

A turbulent subfilter viscosity for large eddy simulation (LES) models is proposed, based on Heisenberg's mechanism of energy transfer. Such viscosity is described in terms of a cutoff wave number, leading to relationships for the grid mesh spacing, for a convective boundary layer (CBL). The limiting wave number represents a sharp filter separating large and small scales of a turbulent flow and, henceforth, Heisenberg's model agrees with the physical foundation of LES models. The comparison between Heisenberg's turbulent viscosity and the classical ones, based on Smagorinsky's parameterization, shows that both procedures lead to similar subgrid exchange coefficients. With this result, the turbulence resolution length scale and the vertical mesh spacing are expressed only in terms of the longitudinal mesh spacing. Through the employment of spectral observational data in the CBL, the mesh spacings, the filter width and the subfilter eddy viscosity are described in terms of the CBL height. The present development shows that Heisenberg's theory naturally establishes a physical criterium that connects the subgrid terms to the large-scale dimensions of the system. The proposed constrain is tested employing a LES code and the results show that it leads to a good representation of the boundary layer variables, without an excessive refinement of the grid mesh.     

Vertical transport of ozone and CO during super cyclones in the Bay of Bengal as detected by Tropospheric Emission Spectrometer

Vertical profiles of carbon monoxide (CO) and ozone retrieved from Tropospheric Emission Spectrometer have been analyzed during two super cyclone systems Mala and Sidr. Super cyclones Mala and Sidr traversed the Bay of Bengal (BOB) region on April 24–29, 2006 and November 12–16, 2007 respectively. The CO and ozone plume is observed as a strong enhancement of these pollutants in the upper troposphere over the BOB, indicating deep convective transport. Longitude–height cross-section of these pollutants shows vertical transport to the upper troposphere. CO mixing ratio ~90 ppb is observed near the 146-mb level during the cyclone Mala and near 316 mb during the cyclone Sidr. Ozone mixing ratio ~60–100 ppb is observed near the 316-mb level during both the cyclones. Analysis of National Centers for Environmental Prediction (NCEP) reanalysis vertical winds (omega) confirms vertical transport in the BOB.     

Evaluating the ability of a numerical weather prediction model to forecast tracer concentrations during ETEX 2

In this paper the meteorological processes responsible for transporting tracer during the second ETEX (European Tracer EXperiment) release are determined using the UK Met Office Unified Model (UM). The UM predicted distribution of tracer is also compared with observations from the ETEX campaign. The dominant meteorological process is a warm conveyor belt which transports large amounts of tracer away from the surface up to a height of 4 km over a 36 h period. Convection is also an important process, transporting tracer to heights of up to 8 km. Potential sources of error when using an operational numerical weather prediction model to forecast air quality are also investigated. These potential sources of error include model dynamics, model resolution and model physics. In the UM a semi-Lagrangian monotonic advection scheme is used with cubic polynomial interpolation. This can predict unrealistic negative values of tracer which are subsequently set to zero, and hence results in an overprediction of tracer concentrations. In order to conserve mass in the UM tracer simulations it was necessary to include a flux corrected transport method. Model resolution can also affect the accuracy of predicted tracer distributions. Low resolution simulations (50 km grid length) were unable to resolve a change in wind direction observed during ETEX 2, this led to an error in the transport direction and hence an error in tracer distribution. High resolution simulations (12 km grid length) captured the change in wind direction and hence produced a tracer distribution that compared better with the observations. The representation of convective mixing was found to have a large effect on the vertical transport of tracer. Turning off the convective mixing parameterisation in the UM significantly reduced the vertical transport of tracer. Finally, air quality forecasts were found to be sensitive to the timing of synoptic scale features. Errors in the position of the cold front relative to the tracer release location of only 1 h resulted in changes in the predicted tracer concentrations that were of the same order of magnitude as the absolute tracer concentrations.     

On plume meandering in unstable stratification

Vertical plume meandering of gaseous pollutant is commonly experienced in the daytime atmospheric boundary layer (also know as convective boundary layer, CBL) that arose from the complicated interaction between buoyancy-generated turbulence and gravitational force. It leads to rapid pollutant mixing that cannot be accurately modeled by conventional Gaussian plume model. In the light of explaining the mechanism of plume rises and descents in CBLs, this study employs a direct numerical simulation (DNS) technique to compute the plume behaviors for pollutant emitted from line sources placed parallel to the spanwise direction in an unstably stratified turbulent open channel flow. The DNS results show that the plume meandering is due to the domination of uni-directional mean vertical pollutant fluxes above and below the mean plume height.     

PLATIN (plant-atmosphere interaction) I: A model of plant-atmosphere interaction for estimating absorbed doses of gaseous air pollutants

A PLant-ATmosphere INteraction model (PLATIN) was developed for estimating air pollutant absorbed doses under ambient conditions. PLATIN is based on the canopy energy balance combined with a gas transport submodel. The model has three major resistance components: (1) a turbulent atmospheric resistance Rah(zm) that describes the atmospheric transport properties between a measurement height above the canopy and the conceptual height z=d+z0m which represents the sink for momentum according to the big-leaf concept; (2) a quasilaminar layer resistance R(b,A) that quantifies the way in which the transfer of sensible heat and matter (e.g. latent heat, ozone) differs from momentum transfer; (3) a canopy or surface resistance R(c,A) that describes the influences of the plant/soil system on the exchange processes. Soil water content is simulated by a Force-Restore model. By a simple interception submodel precipitation and dew are partitioned into intercepted water and water reaching the soil surface. PLATIN can be run in a prognostic or a diagnostic mode. It is also intended for on-line use in air quality monitoring networks.     

Comparison between the atmospheric boundary layer in Paris and its rural suburbs during the ECLAP experiment

The ECLAP experiment has been performed during the winter of 1995 in order to study the influence of the urban area of Paris on the vertical structure and diurnal evolution of the atmospheric boundary layer, in situations favourable to intense urban heat island and pollution increase. One urban site and one rural site have been instrumented with sodars, lidars and surface measurements. Additional radiosondes, 100 m masts and Eiffel Tower data were also collected. This paper gives a general overview of this experiment, and presents results of the analysis of four selected days, characterized by various wind directions and temperature inversion strengths. This analysis, which consists in a comparison between data obtained in the two sites, has been focused on three parameters of importance to the ABL dynamics: the standard deviation of vertical velocity, the surface sensible heat flux, and the boundary layer height. The vertical component of turbulence is shown to be enhanced by the urban area, the amplitude of this effect strongly depending on the meteorological situation. The sensible heat flux in Paris is generally found larger than in the rural suburbs. The most frequent differences range from 25–65 W m^-2, corresponding to relative differences of 20–60%. The difference of unstable boundary layer height between both sites are most of the time less than 100 m. However, sodar and temperature data show that the urban influence is enhanced during night-time and transitions between stable and unstable regimes.     

Chemical segregation by heterogeneous emissions

Ozone pollution in the boundary layer results from photoactivated chemistry of primary pollutants released at the ground. As emissions are highly inhomogeneous in space and time and some chemical time-scales are of the order or larger than dynamical time-scales, it is admitted that turbulent transport and mixing is a key factor in ozone production. We study the interaction between chemistry and convective boundary layer turbulent with a large eddy simulation model coupled to CHIMERE, a detailed chemical model, over a $10\times 10\mathrm{km}$ domain. Our results show that when emissions are concentrated over a limited area, strong values of segregation between chemical species are obtained over the first two active hours during the morning, leading to significant impact in terms of pollutants concentration. After 3 h, for each heterogeneous emission case considered, segregation drops to a few percents for most compounds pairs, due to the strong convective mixing of the boundary layer.     

Ozone and meteorological boundary-layer conditions at Summit,Greenland, during 3–21 June 2000

The temporal and spatial distributions of boundary-layer ozone were studied during June 2000 at Summit, Greenland, using surface-level measurements and vertical profiling from a tethered balloon platform. Three weeks of continuous ozone surface data, 133 meteorological vertical profile data and 82 ozone vertical profile data sets were collected from the surface to a maximum altitude of 1400 m above ground.The lower atmosphere at Summit was characterized by the prevalence of strong stable conditions with strong surface temperature inversions. These inversions reversed to neutral to slightly unstable conditions between ∼9.00 and 18.00 h local time with the formation of shallow mixing heights of ∼70–250 m above the surface.The surface ozone mixing ratio ranged from 39 to 68 ppbv and occasionally had rapid changes of up to 20 ppb in 12 h. The diurnal mean ozone mixing ratio showed diurnal trends indicating meteorological and photochemical controls of surface ozone. Vertical profiles were within the range of 37–76 ppb and showed strong stratification in the lower troposphere. A high correlation of high ozone/low water vapor air masses indicated the transport of high tropospheric/low stratospheric air into the lower boundary layer. A ∼0.1–3 ppb decline of the ozone mixing ratio towards the surface was frequently observed within the neutrally stable mixed layer during midday hours. These data suggest that the boundary-layer ozone mixing ratio and ozone depletion and deposition to the snowpack are influenced by photochemical processes and/or transport phenomena that follow diurnal dependencies. With 37 ppb of ozone being the lowest mixing ratio measured in all data no evidence was seen for the occurrence of ozone depletion episodes similar to those that have been reported within the boundary layer at coastal Arctic sites during springtime.     

A fluctuating plume model for concentration fluctuations in a plant canopy

A one-particle Lagrangian model for continuous releases in the non-Gaussian inhomogeneous turbulence of a canopy layer is derived based on the fluctuating plume model of Franzese [2003. Lagrangian stochastic modeling of a fluctuating plume in the convective boundary layer. Atmos. Environ. 37, 1691–1701.]. The model equations are filtered by a time-dependent low-pass filter applied to the turbulent kinetic energy in order to obtain a fluctuating plume model able to simulate the vertical meandering of the cloud centroid through non-stationary Lagrangian equations. The model satisfies the well-mixed condition. The relative dispersion of particles and the concentration fluctuation statistics of a passive tracer inside a modeled vegetal canopy are studied. The probability density function of the concentration relative to the plume centroid is parameterized and the mean and variance fields of concentration are simulated and compared with wind-tunnel data and numerical simulations. A skewed, reflected probability density function for the vertical position of the plume centroid is considered.     

Spatio-temporal covariation of urban particle number concentration and ambient noise

Mobile measurements of ambient noise and particle number concentrations were carried out within an urban residential area in Essen, Germany, during summer 2008. A busy major road with a traffic intensity of about 44,000 vehicles per day was situated within the study area. The spatio-temporal distribution of noise and particles was closely coupled to road traffic on the major road. Total particle number concentrations in proximity to the main road were on average between 25,000 cm^?3 and 35,000 cm^?3 while sound levels reached 70–78 dB(A). These estimates were more than double-fold (factor 2.4) in comparison to the urban residential background. At a 50 m distance off the road particle number concentrations were decaying to about 50% of the initial value. The measurements were characterised by close spatial correlation between total particle number concentration and ambient noise with correlation coefficients of up to r = 0.74. However, during one measurement day coupling between both quantities was weak due to higher turbulent mixing within the canopy layer and a change in ambient wind directions. Enhanced dilution of particle emission from road traffic by turbulent mixing and ‘decoupling’ from the influence of road traffic are believed to be responsible.     

Boundary-layer dynamics and its influence on atmospheric chemistry at Summit,Greenland

Sonic anemometer turbulence measurements were made at Summit, Greenland during summer 2004 and spring 2005. These measurements allow for the characterization of the variability of the atmospheric boundary layer at this site by describing seasonal and diurnal changes in sensible heat flux and boundary layer stability as well as providing estimates of mixing layer height. Diurnal sensible heat fluxes at Summit ranged from −18 to −2 W m⁻² in the spring and from −7 to +10 W m⁻² in the summer. Sustained stable surface layer conditions and low wind speeds occured during the spring but not during the summer months. Unstable conditions were not observed at Summit until late April. Diurnal cycles of convective conditions during the daytime (0700–1700 h local time) were observed throughout July and August. Boundary layer heights, which were estimated for neutral to stable conditions, averaged 156 m for the spring 2005 observations. Comparisons of the boundary layer characteristics of Summit with those from South Pole, Antarctica, provide possible explanations for the significant differences in snowpack and surface-layer chemistry between the two sites.     

Simulation of boundary layer trajectory dispersion sensitivity to soil moisture conditions: MM5 and Noah-based investigation

In this study, the sensitivity of trajectory paths to anomalous soil moisture was analyzed during three different synoptic episodes in June 2006. The MM5 and Noah land surface models were used to simulate the response of the planetary boundary layer. The HYSPLIT model was used for trajectory analysis. It was found that the response in horizontal lower-level wind field was larger at regions where vertical wind velocity changes were also large. In addition, the sensitivity to soil moisture changes was significant and localized where convective activity was well developed and synoptic effects did not dominate. A non-local effect was felt over the rest of the domain where convection was not present since the model atmosphere reacted as a whole to compensate for induced changes in vertical velocity. This finding was supported by the fact that domain averaged vertical velocities changes were of the order of 0.2 cm s^?1 or less at about 650 hPa and about 200 times smaller than modeled local vertical velocity changes. The largest change in horizontal wind field near the surface was found for weak synoptic events on June 11–12 and June 22–23 while the stronger synoptic event of June 17–18 showed smaller differences. These changes in wind field conditions impacted the transport and dispersion of pollutants. To quantify the sensitivity of air quality estimates to soil moisture uncertainty, we have used three well known measures of trajectory differences: the absolute horizontal transport deviation (AHTD), the relative horizontal transport deviation (RHTD) and the absolute vertical transport deviation (AVTD) for an ensemble of 98 trajectories departing from a region well within the computational domain. For the June 11–12 event it was found that for wet and dry soil moisture experiments, AHTD, RHTD, and AVGTD can reach values in the range 60–100 km, 10–20% and 500–900 m at 24 h run time, respectively. For the June 17–18 and June 22–23 events these values of trajectory differences were reduced more than half. These differences in behavior between time periods are largely attributed to the combined effects of synoptic forcing and the sensitivity of planetary boundary layer to soil moisture changes during well developed convection. The implication for air quality studies is that the soil moisture anomaly and related uncertainty in planetary boundary layer response needs to be incorporated in order to construct an ensemble of the most probable scenarios in which pollutants are released and transported throughout a given target region.     

The energy balance of central Mexico City during the dry season

The first measurements of the energy balance fluxes of a dry, densely built-up, central city site are presented. Direct observation of the net radiation, sensible and latent heat flux densities above roof-top in the old city district of Mexico City allow the heat storage flux density to be found by residual. The most important finding is that during daytime, when evaporation is very small (<4% of net radiation), and therefore sensible heat uses dominate (Bowen ratio >8), the uptake of heat by the buildings and substrate is so large (58%) that convective heating of the atmosphere is reduced to a smaller role than expected (38%). The nocturnal release of heat from storage is equal to or larger than the net radiation and sufficient to maintain an upward convective heat flux throughout most nights. It is important to see if this pattern is repeated at other central city, or dry urban sites, or whether it is only found in districts dominated by massive stone structures. These findings have implications for the height of the urban mixing layer and the magnitude of the urban heat island.     

A study of the variation of urban mixed layer heights

The AERMET model is used to estimate hourly mixing heights during the Joint URBAN (2003) experiment in Oklahoma City, Oklahoma. AERMET is a simple 2-D model that requires only routine meteorological observations and an early morning atmospheric sounding to estimate convective boundary layer (CBL) growth. Estimated mixing heights are compared with observed mixing heights measured during Joint URBAN 2003. Observed CBL heights are derived from profiler data using a peak signal-to-noise ratio method. The method of deriving mixing heights from profiler data is validated using daily atmospheric sounding data. Estimated mixing heights using AERMET show good agreement with observations on days of varying temperature and cloud cover. AERMET was able to estimate the rapid boundary layer growth observed in the late morning and early afternoon hours during highly convective conditions. CBL heights of over 3000 m are observed in sounding data during the late afternoon. Estimated CBL heights of over 3000 m during the late afternoon agreed well with observations from the sounding and profiler data.     

Simulation of the evolution of particle size distributions containing coarse particulate in the atmospheric surface layer with a simple convection-diffusion-sedimentation model

The Fugitive Dust Model (FDM) and Industrial Source Complex (ISC), widely used coarse particulate dispersion models, have been shown inaccurate due to the neglect of vertical variations in atmospheric wind speed and turbulent diffusivity (Vesovic et al., 2001), omission of the gravitational advection velocity, and an underestimation of the ground deposition velocity (Kim and Larson, 2001). A simple, transient two-dimensional convection-diffusion-sedimentation model is proposed to simulate the evolution in particle size distribution of an aerosol ‘puff’ containing coarse particulate in the atmospheric surface layer. Monin-Okhubov similarity theory, accompanied by empirical observations made by Businger et al. (1971), is adopted to characterize the surface layer wind speed and turbulent diffusivity profiles over a wide range of atmospheric conditions. A first order analysis of the crossing trajectories effect suggests simulation data presented here are not significantly affected by particle inertia. The model is validated against Suffield experimental data in which coarse particulate deposition was measured out to a distance of 800 m from the source (Walker, 1965). Good agreement is found for the decay in ground deposits with distance from the source for stable atmospheres. Deposition data was also simulated for unstable atmospheric stratification and the current model was determined to modestly underestimate the peak concentration with increasing accuracy further downwind of the release. The current model's effective deposition velocity was compared to that suggested by Kim et al. (2000) and shows improvement with respect to FDM. Lastly, the model was used to simulate the dispersion of nine lognormal aerosol puffs in the lowest 50 m of the atmospheric surface layer for four classes of atmospheric stability. The simulated mass median aerodynamic diameters (MMAD) at multiple downwind sampling locations were calculated and plotted with distance from the source. The first 50 m from the source was found to have a substantial impact on the evolution of MMAD for stable atmospheric conditions. Away from the source, it was observed that particle size distributions were truncated by removal of all particles larger than about 60 μm. A particle Peclet number was also defined to quantify the relative importance of turbulent dispersion and sedimentation on particle motion in the vertical direction.     

Ground-based remote sensing measurements of aerosol and ozone in an urban area: A case study of mixing height evolution and its effect on ground-level ozone concentrations

We have estimated the mixing height (MH) and investigated the relationship between vertical mixing and ground-level ozone concentrations in Seoul, Korea, by using three ground-based active remote sensing instruments operating side by side: micro-pulse lidar (MPL), differential absorption lidar (DIAL), and differential optical absorption spectroscopy (DOAS). The MH is estimated from MPL measurements of aerosol extinction profiles by the gradient method under convective conditions. Comparisons of the MHs estimated from MPL and radiosonde measurements show a good agreement (r²=0.99). Continuous MPL measurements with high temporal and vertical resolution reveal the diurnal variations of the MH under convective conditions and the presence of a residual layer during the nighttime. Comprehensive measurements of ozone and aerosol by MPL, DIAL and DOAS during an high ozone episode (24–26 May 2000) in Seoul, Korea, reveal that (1) photochemical ozone production and advection from upwind regions (the western part of Seoul) contribute two peaks of ozone concentrations at the ground around 14:00 and 18:00 local time on 25 May 2000, respectively, and (2) the entrainment and the fumigation processes of ozone aloft in the nighttime residual layer into the ground is a major contributor of high concentrations of ground-level ozone observed on the following day (26 May 2000).     

New particle formation in the Midwestern USA: Event characteristics,meteorological context and vertical profiles

Two years of continuous particle size distribution measurements at three heights over and in a deciduous forest in southern Indiana exhibit evidence of particle nucleation on 46% of classifiable days, and clear nucleation with consistent subsequent growth on 14% of days. Events characterized by high ultra-fine particle production and clear growth are most frequent in spring. These events most frequently follow cold front passages and exhibit a higher frequency of northerly back-trajectories. Local meteorological conditions, as described using the Nucleation Parameter (NP) of Boy and Kulmala (2002) and stability indices, indicate a significant association with ultra-fine particle concentrations, and specifically that nucleation was frequently preceded by destabilization of the atmosphere consistent with entrainment of elevated pollution layers. There appears to be little or no dependence of nucleation frequency or intensity on the in situ condensational sink particularly during spring, which is consistent with very high regional emissions of the precursors of ternary nucleation. Vertical gradients of particle size distributions exhibit evidence for nucleation being focused above canopy and accordingly mean ratios of above and below canopy concentrations of ultra-fine particles (6–30 nm) just subsequent to nucleation are 1.8 and 1.7 respectively during leaf-on and leaf-off periods. The difference in vertical concentration ratios during leaf-on and leaf-off are used to infer that of the order of 25% of ultra-fine particles are captured by foliar elements in the canopy during turbulent mixing through the canopy.