Abstract
The role of clouds in photodissociation is examined by both modeling and observations. It is emphasized that the photodissociation rate is proportional to the actinic flux rather than to the irradiance. (The actinic flux concerns the energy that is incident on a molecule, irrespective of the direction of incidence. The irradiance concerns the energy that is incident on a plane.) A 3-layer model is used to calculate the actinic flux above and below a cloud, relative to the incident flux, in terms of cloud albedo, zenith angle and the albedo of the underlying and overlying atmosphere. Cloud albedo is mainly determined by cloud optical thickness. An expression for the in-cloud actinic flux is given as a function of in-cloud optical thickness. The 3-layer model seems to be an useful model for estimation of photodissociation rates in dispersion models. Further, a multi-layer delta-Eddington model is used to calculate irradiances, actinic fluxes and photodissociation rates of nitrogen dioxide J(NO2) as a function of height in inhomogeneous atmospheres. For the considered wavelength interval [290–420 nm], Rayleigh scattering, ozone absorption and Mie scattering and absorption by cloud drops and aerosols should be taken into account. It is stressed that both models are one-dimensional and as such are unable to deal with partial cloudiness. It is shown that if no clouds are present, the actinic flux depends primarily on the solar zenith angle. The actinic flux usually increases with height. For cloudy atmospheres, another important parameter with respect to the actinic flux is added: cloud optical thickness, which determines cloud albedo. It can be shown that in-cloud characteristics and cloud height are less important in describing the effect of a cloud on the actinic flux (outside the cloud). The in-cloud values of the actinic flux can exceed the values outside the cloud. Finally, using the photostationary state relationship, good agreement is found between model results and aircraft measurements.
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Duynkerke, P.G., Van Weele, M. Actinic fluxes: The role of clouds in photodissociation. Boundary-Layer Meteorol 62, 417–432 (1993). https://doi.org/10.1007/BF00705570
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DOI: https://doi.org/10.1007/BF00705570