Diffuse radiation,twilight, and photochemistry — I

A photochemical scheme which includes a detailed treatment of multiple scattering up to solar zenith angles of 96° (developed for use in a GCM) has been used to study partitioning within chemical families. Attention is drawn to the different zenith angle dependence of diffuse radiation for the two spectral regions <310 nm and >310 nm. The effect that this has on the so-called 40 km ozone problem is discussed. The importance of correctly including multiple scattering for polar ozone studies is emphasised.     

Theoretical Simulation of Solar Ultraviolet Fluxes Measured on the 8 July 1974 Stratoprobe I flights

Solar ultraviolet fluxes in the wavelength region 1900 to 2300Å were measured during the first balloon flight of Project stratoprobe on July 8, 1974, over a range of solar zenith angles at a float altitude of 28.6 km. High‐resolution computer simulations of the measured spectra were made for a range of solar zenith angles of 40° to 80° over the wavelength region 2050 to 2150A, and comparisons made with the observed spectra at 40° and 47 °. Qualitative agreements were obtained but there were significant discrepancies between the simulated and experimentally obtained fluxes. Sources of the discrepancies are discussed.     

Modelling radiation quantities and photolysis frequencies in the troposphere

STAR (System for Transfer of Atmospheric Radiation) was developed to calculate accurately and efficiently the irradiance, the actinic flux, and the radiance in the troposphere. Additionally a very efficient calculation scheme to computer photolysis frequencies for 21 different gases was evolved. STAR includes representative data bases for atmospheric constituents, especially aerosol particles. With this model package a sensitivity study of the influence of different parameter on photolysis frequencies in particular of O₃ to Singlet D oxygen atoms, of NO₂, and of HCHO was performed. The results show the quantitative effects of the influence of the solar zenith angle, the ozone concentration and vertical profile, the aerosol particles, the surface albedo, the temperature, the pressure, the concentration of NO₂, and different types of clouds on the photolysis frequencies.Notation I _A(, ) actinic flux - I _H(, ) irradiance - L(, , , ) radiance - wavelength - azimuth angle - cosine of zenith angle - _s cosine of solar zenith angle - optical depth - _s scattering coefficient - _c extinction coefficient - _o single scattering albedo - p _mix mixed phase function - g _mix mixed asymmetry factor - J _gas photolysis frequency     

On the angular correction of satellite radiation measurements: The performance of ERBE angular dependence model in the Arctic

Summary An angular dependence model (ADM) is needed to convert radiance measurements into fluxes. This paper provides an overview on the progress and issues related to the angular correction of radiation data at the top-of-the-atmosphere (TOA), followed by an investigation on the performance of the Earth Radiation Budget Experiment (ERBE) ADMs in the Arctic during summer. The variation of inferred albedo with viewing geometry indicates the merit of an ADM. The ERBE ADM for land does well as it leads to near constant albedos for given solar zenith angles. The ADM for snow/ice is least satisfactory when applied to the Arctic in summer. The performance of the ocean ADM is acceptable except at large solar zenith angles for which albedo increases with viewing zenith angle. Significant and systematic variation of albedo with viewing angle and relative azimuth angle are manifest when the overcast ERBE ADM is applied to over-cast-over-snow/ice scenes. A methodology for correcting ERBE ADMs was proposed by normalizing the anisotropic factor over bins containing sufficient measurements.With 6 Figures     

A modified profile method for determining the vertical fluxes of NO,NO2, ozone,and HNO3 in the atmospheric surface layer

A modified profile method for determining the vertical deposition (or/and exhalation) fluxes of NO, NO₂, ozone, and HNO₃ in the atmospheric surface layer is presented. This method is based on the generally accepted micrometeorological ideas of the transfer of momentum, sensible heat and matter near the Earth's surface and the chemical reactions among these trace gases. The analysis (aerodynamic profile method) includes a detailed determination of the micrometeorological quantities (such as the friction velocity, the fluxes of sensible and latent heat, the roughness length and the zero plane displacement), and of the height-invariant fluxes of the composed chemically conservative trace gases with group concentrations c ₁=[NO]+[NO₂]+[HNO₃], c ₂=[NO₂]+[O₃]+3/2·[HNO₃], and c ₃=[NO]–[O₃]–1/2·[HNO₃]. The fluxes of the individual species are finally determined by the numerical solution of a system of coupled nonlinear ordinary differential equations for the concentrations of ozone and HNO₃ (decoding method). The parameterization of the fluxes is based on the flux-gradient relationships in the turbulent region of the atmospheric surface layer. The model requires only the vertical profile data of wind velocity, temperature and humidity and concentrations of NO, NO₂, ozone, and HNO₃.The method has been applied to vertical profile data obtained at Jülich (September 1984) and collected in the BIATEX joint field experiment LOVENOX (Halvergate, U.K., September 1989).     

Comparison between measured and modelled cloudless‐sky solar irradiances at the surface and at the top of the atmosphere

Abstract

Cloudless‐sky solar fluxes calculated by the radiative transfer algorithm used in the Canadian Climate Centre's general circulation climate model are compared with measurements of upwelling radiation at the top of the atmosphere (TOA) and downwelling radiation at the surface. The 12‐layer model partitions the solar spectrum into two broad wavebands (0.25–0.68 and 0.68–4.00 μm). The comparison utilized TOA fluxes estimated from Nimbus‐ 7 measurements and measured downwelling fluxes at the surface for Kalgoorlie, West Australia, and downwelling fluxes at the surface for Woodbridge, Ontario. Model estimates and measurements agreed to within experimental error for most solar zenith angles. Estimates improved, especially at Woodbridge, when aerosol effects were included. The mean bias error was less than 4% for surface irradiance and less than 6% for upwelling TOA irradiance, which produces a TOA albedo error of about 0.01.     

Numerical integration errors in calculated tropospheric photodissociation rate coefficients

Tropospheric photodissociation rate coefficients (J values) were calculated for NO₂, O₃, HNO₂, CH₂O, and CH₃CHO using high spectral resolution (0.1 mm wavelength increments), and compared to the J values obtained with numerically degraded resolution (=1, 2, 4, 6, 8, and 10 nm, and several commonly used nonuniform grids). Depending on the molecule, substantial errors can be introduced by the larger increments. Thus for =10 nm, errors are less than 1% for NO₂, less than 2% for HNO₂, +6.5% to -16% for CH₂O, -6.9% to +24% for CH₃CHO, and -24% to +110% for O₃. The errors for CH₂O arise from the fine structure of its absorption spectrum, and are prevalently negative (underestimate of J). The errors for O₃, and to a lesser extent for CH₃CHO, arise mainly from under-resolving the overlap of the molecular action spectrum and the tropospheric actinic flux in the wavelength region of stratospheric ozone attenuation. The sign of those errors depends on whether the actinic flux is averaged onto the grid before or after the radiative transfer calculation. In all cases studied, grids with 2 nm produced errors no larger than 5%.     

Effects of tropospheric aerosols on the solar radiative heating in a clear atmosphere

Summary The broadband solar absorptivity concept is employed to parameterize the aerosol absorption effect. The solar radiation model developed by Liou and his associates was modified to incorporate the parameterization of solar radiative transfer in an aerosol layer. Comparison of the results from this method with other schemes exhibits close agreement. A Sahara dust storm case was also chosen to test the performance of the present model, and the computed heating rate profiles agree well with calculations based on optical properties derived from observations for both clear and dust cases. In general, enhanced heating due to aerosol absorption of solar flux occurs particularly in the lower troposphere (below 5 km). The heating rate is independent of the scattering partition factor (), but the planetary albedo increases with . Further study shows that the aerosol heating is sensitive to the surface albedo (r _s ) and to the cosine of the solar zenith angle (µ ₀). The decrease inr _s and/or increase inµ ₀ lower the solar heating rate, the planetary albedo and the atmospheric absorptivity, but raise the surface absorptivity due to reduced multiple reflection between the atmosphere and surface.With 9 Figures     

Modelling of the vertical fluxes of nitric acid,ammonia, and ammonium nitrate

Results from numerical investigations regarding the exchange of HNO₃, NH₃, and NH₄NO₃ between the atmosphere and the biosphere are presented. The investigations were performed with a modified inferential method which is based on the generally accepted micrometeorological ideas of the transfer of momentum, sensible heat and matter near the Earth's surface and the chemical reactions among these nitrogen compounds. This modified inferential method calculates the micrometeorological quantities (such as the friction velocity and the fluxes of sensible and latent heat), the height-invariant fluxes of the composed chemically conservative trace species with group concentrationsc ₁=[HNO₃]+[NH₄NO₃] (total nitrate),c ₂=[NH₃]+[NH₄NO₃] (total ammonia), andc ₃=[HNO₃]-[NH₃] as well as the fluxes of the individual nitrogen compounds. The parameterization of the fluxes is based on the flux-gradient relationships in the turbulent region of the atmospheric surface layer. The modified inferential method requires only the data of wind velocity, temperature, humidity and concentrations (HNO₃, NH₃, and NH₄NO₃) measured at a reference height by stations of a monitoring network.     

Calculations of the temperature dependence of the NO2 photodissociation coefficient in the atmosphere

The photodissociation coefficient, J _NO2 of NO₂ in the atmosphere was calculated at 235 and 298 K using the measured temperature dependences of the absorption cross-sections and quantum yields. These calculations gave a ratio J _NO2(298 K)/J _NO2(235 K)=1.155±0.010 which is only weakly dependent on altitude, surface albedo and solar zenith angle.     

A Wind Tunnel Model for Quantifying Fluxes in the Urban Boundary Layer

Transport of pollution and heatout of streets into the boundary layer above is not currently understood and so fluxes cannot be quantified. Scalar concentration within the street is determined by the flux out of it and so quantifying fluxes for turbulent flow over a rough urban surface is essential. We have developed a naphthalene sublimation technique to measure transfer from a two-dimensional street canyon in a wind tunnel for the case of flow perpendicular to the street. The street was coated with naphthalene, which sublimes at room temperature, so that the vapour represented the scalar source. The transfer velocity w_T relates the flux out of the canyon to the concentration within it and is shown to be linearly related to windspeed above the street. The dimensionless transfer coefficient w_T/U represents the ventilation efficiency of the canyon (here, w_T is a transfer velocity,U is the wind speed at the boundary-layer top). Observed values are between 1.5 and 2.7 ×10^-3 and, for the case where H/W0 (ratio of buildingheight to street width), values are in the same range as estimates of transfer from a flat plate, giving confidence that the technique yields accurate values for street canyon scalar transfer. w_T/U varies with aspect ratio (H/W), reaching a maximum in the wake interference regime (0.3 < H/W < 0.65). However, when upstream roughness is increased, the maximum in w_T/U reduces, suggesting that street ventilation is less sensitive to H/W when the flow is in equilibrium with the urban surface. The results suggest that using naphthalene sublimation with wind-tunnel models of urban surfaces can provide a direct measure of area-averaged scalar fluxes.     

A coupled ocean-atmosphere climate model: temperature versus salinity effects on the thermohaline circulation

A simple nonlinear three-box ocean model of the North Atlantic Ocean including the rudiments of eddy mixing, vertical stratification and thermohaline circulation is first presented. It is subject to uniform latitudinal differential heating, q, and net evaporation m _e , and includes a linear equation of state. Two quite different limiting steady-state solutions exist. The first has a warm saline surface water and a cold, low-salinity deep ocean; deep water is primarily formed in higher latitudes by the prevalence of differential heating. A second limiting solution consists of a warm saline deep ocean underlying a cool, low-salinity surface ocean; deep water is formed primarily in lower latitudes as a consequence of large differential evaporation. A coupled ocean-atmosphere model, in which the oceanic surface heat fluxes are determined internally but with differential evaporation at the ocean surface m _e remaining an external parameter, is next presented. The atmosphere component is a simple energy balance model that emphasizes the vertical fluxes of radiative, sensible and latent heat fluxes but does not include temperature-albedo feedback. Model response depends on the external parameters m _e and , controlling the magnitude of the thermohaline-driven circulation, and on the magnitudes of the eddy mixing coefficients and the solar constant. For small m _e , a steady-state solution corresponding to a cold fresh deep ocean is found, qualitatively similar to the modern ocean. For large m _e , a steady-state solution with a warm saline deep ocean occurs; this solution resembles conceptual models that have been proposed for the warm saline Cretaceous ocean. There exists an intermediate region of values of m _e for which the solutions are more complex. On the lower end of this region, both the cold fresh deep-ocean and warm saline deep-ocean circulations coexist as stable equilibria. On the upper end, the cold-deep ocean becomes unstable, manifesting oscillations with growing amplitude, and ultimately reaches the warm saline deep-ocean solution. In the neighborhood of a cusp on the , m _e plane, that is, for relatively small , more complex behaviour occurs, which has not yet been fully analyzed. The model response in the region of complexity is not sensitive to changes in the solar constant but is sensitive to the eddy mixing coefficients.     

A numerical model study of the structure and similarity scaling of the nocturnal boundary layer (NBL)

A one-dimensional numerical model based on the equations of mean motion and turbulent kinetic energy (TKE), with Delage's (1974) mixing-length parameterization has been used to simulate the mean and turbulent structure of the evolving stably stratified nocturnal boundary layer (NBL). The model also includes a predictive equation for the surface temperature and longwave radiational cooling effects.In the absence of advective and gravity wave effects, it is found that the model-simulated structure, after a few hours of evolution, could be ordered fairly well by a similarity scaling (u _*0, _*0, L ₀, and h) based on surface fluxes and the NBL height. Simple expressions are suggested to describe the normalized profiles of momentum and heat fluxes, TKE, eddy-viscosity and energy dissipation. A good ordering of the same variables is also achieved by a local scaling (u _*0, _* and L) based on the height-dependent local fluxes. The normalized TKE, eddy viscosity and energy dissipation are unique functions of z/L and approach constant values as z/L , where L is the local Monin-Obukhov length. These constants are close to the values predicted for the surface layer as z/L , thus suggesting that the Monin-Obukhov similarity theory can be extended to the whole NBL, by using the local (height-dependent) scales in place of surface-layer scales. The observed NBL structure has been shown to follow local similarity (Nieuwstadt, 1984).     

Comparison of areally averaged turbulent fluxes over non-homogeneous terrain: Results from the EFEDA-field experiment

In June 1991 the EFEDA-field experiment (ECHIVAL Field Experiment in a Desertification-Threatened Area) was carried out in the Spanish province Castilla-La Mancha, to improve the understanding of the interactions between the soil, the vegetation and the atmosphere.Here results of energy balance studies at the Barrax site are given, one of the three intensively studied experimental sites within Castilla-La Mancha. This area is characterized by a large fraction of irrigated fields (40%) while the remaining 60% was fallow land at the end of June 1991. The energy balances over these two characteristic land-use classes totally differ. While for the irrigated fields the evapotranspiration is dominant, for the non-irrigated fields the sensible and the soil heat fluxes dominate and the latent heat flux is nearly negligible.In order to achieve areally averaged turbulent fluxes, surface, SODAR and aircraft data have been used. Comparing the surface fluxes from all three facilities, it can be found that:The sensible heat flux estimation from SODAR (_w-method) gives reliable results when a calibration of _w is done with another independent system (e.g. aircraft).Aircraft measurements in conjunction with energy budget methods yield surface fluxes of sensible heat, which are about 20% lower than the areally averaged values calculated by the surface measurements. The areally averaged latent heat fluxes from aircraft and surface measurements agree better than the sensible heat fluxes.     

In the Core of the Night-Effects of Intermittent Mixing on a Horizontally Heterogeneous Surface

Intermittent breakdowns that accompany wind gusts at the surface are responsible for a large fraction of the turbulent exchange between the surface and the upper boundary layer in the core of clear nights. Vertical and horizontal structure of the breakdowns are investigated using data from a network of 26 stations in an area of 30 km × 30 km. Surface heterogeneity in the area includes complex terrain with different types of land cover. We treat the fine-scale landscape structure near sensors (sheltering) as a separate component of heterogeneity. These features have important consequences on the spatial distribution of mean variables and surface fluxes. We found that breakdowns connect the surface layer to a higher level (level H_C). Weak wind gusts below a threshold (approximately 1.5 m s^-1) mix the air down to the colder ground, cooling the surface layer. On the other hand, wind gusts above this threshold promote mixing with upper levels, warming the surface layer. The spatial maximum of surface temperature over the network can be used as an estimate of the temperature at H_C, allowing vertical gradients and stability to be approximated. Minimum temperature is a function of topography and sheltering. Appreciable surface fluxes at night occur primarily at high, open locations, and can be large enough there to influencearea-averaged values. Surface-fluxparameterizations currently used in mesoscale models were tested first by estimating fluxes at each station and aggregating, and then by formingarea-averages before estimating fluxes. Results show that these formulations underestimate the average surface fluxes over a region for most of the nights.     

Interaction between the atmospheric and oceanic boundary layers

The two-layer system of an atmosphere over water bodies is reduced to a single-layer problem. Values of the interfacial quantities, such as the friction velocity, the surface velocity, the angles, and , between the surface shear stress and the geostrophic wind velocity and the surface wind velocity, respectively, and the surface roughness, all of which depend upon external parameters, such as the geostrophic wind and stratifications, are obtained. The geostrophic drag coefficient C _d, the geostrophic wind coefficient C _f, and the angles , and , of the turbulent flow at the sea-air interface are functions of a dimensionless number, mfG/kg, with S ₁ and S ₂ as two free stratification parameters. The surface roughness is uniquely determined from the geostrophic wind rather than from the wind profile in the boundary layer.Formerly Visiting Research Associate, Applied Physics Branch, Earth Observations Division, NASA-Manned Spacecraft Center, Houston, Texas.     

Effects of heat and water vapor transport on eddy covariance measurement of CO2 fluxes

Flux densities of carbon dioxide were measured over an arid, vegetation-free surface by eddy covariance techniques and by a heat budget-profile method, in which CO₂ concentration gradients were specified in terms of mixing ratios. This method showed negligible fluxes of CO₂, consistent with the bareness of the experimental site, whereas the eddy covariance measurements indicated large downward fluxes of CO₂. These apparently conflicting observations are in quantitative agreement with the results of a recent theory which predicts that whenever there are vertical fluxes of sensible or latent heat, a mean vertical velocity is developed. This velocity causes a mean vertical convective mass flux (= _cw for CO₂, in standard notation). The eddy covariance technique neglects this mean convective flux and measures only the turbulent flux _c w. Thus, when the net flux of CO₂ is zero, the eddy covariance method indicates an apparent flux which is equal and opposite to the mean convective flux, i.e., _c w = – _c w. Corrections for the mean convective flux are particularly significant for CO₂ because _cw and _c w are often of similar magnitude. The correct measurement of the net CO₂ flux by eddy covariance techniques requires that the fluxes of sensible and latent heat be measured as well.     

Photochemical aspects of tropospheric iodine behaviour

The I-atom sensitised decomposition of ozone in air at 1 atm pressure and ambient temperature has been investigated. Iodine atoms were produced by photolysis of I₂ using visible light or of CH₃I using ultraviolet light. In both cases, the quantum yield for O₃ decomposition was 1.25 (±0.11) per I atom. An important role is proposed for the self-reaction of IO radicals leading to higher oxides of iodine, IO+IO(+M)I₂O₂(+M)higher oxides, which predominated over the bimolecular reaction leading to regeneration of I atoms, IO+IO2I+O₂, with k _2a/k _2b4. Simple computer modelling calculations indicate that reaction (2a) may be important in determining the fate of photolabile iodine species in the atmosphere. The consequences for the behaviour of radioiodine releases are also discussed.     

Similarity scaling applied to sodar observations of the convective boundary layer above an irregular hill

Nine profiles of the temperature structure parameter C _T ² and the standard deviation of vertical velocity fluctuations ( _w) in the convective boundary layer (CBL) were obtained with a monostatic Doppler sodar during the second intensive field campaign of the First ISLSCP Field Experiment in 1987. The results were analyzed by using local similarity theory. Local similarity curves depend on four parameters: the height of the mixed layer (z _i ), the depth of the interfacial layer (), and the temperature fluxes at the top of the mixed layer (Q _i ) and the surface (Q _o). Values of these parameters were inferred from sodar data by using the similarity curve for C _T ² and observations at three points in its profile. The effects of entrainment processes on the profiles of C _T ² and _wnear the top of the CBL appeared to be described well by local similarity theory. Inferred estimates of surface temperature flux, however, were underestimated in comparison to fluxes measured by eddy correlation. The measured values of _wappeared to be slightly smaller than estimates based on available parmeterizations. These discrepancies might have been caused by experimental error or, more likely, by the distortion of turbulence structure above the site by flow over the nonuniform terrain at the observation site.     

Variability of surface roughness and turbulence intensities at a coastal site in India

Surface-layer features with different prevailing wind directions for two distinct seasons (Southwest Monsoon and Northeast Monsoon) on the west coast of India are studied using data obtained from tower-based sensors at a site located about 500 m from the coast. Only daytime runs have been used for the present analysis. The surface boundary-layer fluxes have been estimated using the eddy correlation method. The surface roughnessz ₀ obtained using the stability-corrected wind profiles (Paulson, 1970) has been found to be low for the Southwest monsson season. For the other season,z ₀ is relatively high. The drag coefficientC _D varies with height in the NE monsoon season but not in the season with lowz ₀. This aspect is reflected in the wind profiles for the two seasons and is discussed in detail. The scaling behaviour of friction velocityu _* and the turbulence intensity of longitudinal, lateral and vertical winds _u, _v and _w, respectively) are further examined to study their dependence on fetch. Our study shows that for the non-dimensional case, _u/u_* and _v/u_* do not show any surface roughness dependence in either season. On the other hand, for _w/u_* for the season with lowz ₀, the values are seen to agree well with that of Panofskyet al. (1977) for homogeneous terrain whereas for the other season with highz ₀, the results seem to conform more to the values observed by Smedman and Högström (1983) for coastal terrain. The results are discussed in the light of observations by other investigators.