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A. Calculation of radiative heating/cooling rate profiles: One-dimensional radiative heating/cooling rate profiles are a function of pressure for each spectral interval. For circulation model calculations, the ultimate quantity of interest is total shortwave heating rate profile and the total longwave cooling rate profile which represent the integration of spectral heating/cooling rate profile information over the 3000-50000 cm-1 and 100-3000 cm-1 bands respectively. The value of the radiative heating/cooling rate for a given pressure layer is directly proportional to the radiative flux divergence for that layer: z dFnet z C p z dz 1 (A1) where z is the spectral heating/cooling rate of the layer, z is the density of the layer, C p is the heat capacity, and Fnet z is the net (upward-downward) flux for the layer over the spectral interval denoted . For the longwave, the heating rate profile is generally negative, so the convention is to reverse the sign and use the term ‘cooling rate profile’ instead. The calculation of heating/cooling rate profiles is ubiquitous so a large amount of research has been devoted towards addressing the accuracy and computational efficiency of these values. For the clear-sky longwave conditions in local thermodynamic equilibrium, the derivation of the net flux divergence follows from a solution to the Fundamental Equation of Radiative Transfer because the source function is the Planck function. For upwelling radiance, the solution is: I , z B z surf T , z surf , z z zsurf B z ' T , z' , z dz ' z ' (A2) and for downwelling radiance, the solution is: I , z B z ' z T , z, z ' dz ' z ' (A3) where I , z is the radiance over a spectral interval in a layer and viewing angle cos , is the surface emissivity, B is the Planck function, z surf is the surface temperature, and T is the spectral transmittance between two layers. For the calculation of heating/cooling rates, radiance calculations must be converted into flux: F z I , z d 1 (A4) 0 where the superscript refers to separate upwelling and downwelling components. As an analog to spectral transmittance, the concept of flux transmittance allows the 1 representation of flux in similar terms as the solution to the radiative transfer equation in terms of radiance without having constantly to declare the angular integration: T f z ' , z T , z' , z d 1 (A5) 0 F z B zsurf T f zsurf ,z F z B z ' z z zsurf B z ' T f z, z ' dz ' z ' T f z',z dz ' z ' (A6) (A7) The definition of flux transmittance is such that T f z ' , z1 z2 T f z ' , z1 * T f z1 , z2 (A8) Consequently, the net flux divergence is given by the derivative of the net flux (upwelling-downwelling) and is given by: T f z surf , z B z surf z 2 f z T z ' , z dz ' 2 z zsurf B z ' C p z z ' z 2T f z, z ' dz ' z B z ' z ' z (A9) In practice cooling rate profile calculation is performed with an emphasis on computational efficiency. With a given atmospheric state (temperature, H2O, CO2, O3, CH4, N2O, and cloud optical depth profiles), band models programs are utilized to estimate interlayer transmittance. This value is scaled empirically to yield flux transmittance from which layer fluxes are derived. Radiance-to-flux conversion is achieved formally and exactly through exponential integrals (Goody and Yung, 1988). In practice, the computational expense of exponential integrals motivates the usage of limited-point quadrature. Gauss-Jacobi quadrature is an optimal means for the calculation of flux transmittance, and the utilization of three-point quadrature produces little discrepancy as compared to complete angular integration. Many fast radiative transfer models even use the diffusivity approximation (1-point quadrature) to calculate flux transmittance. Quadrature methods tend to produce some error in the layer exchange terms only with low optical depth bands. The discretized calculation of upwelling and downwelling fluxes at layer boundaries (levels) is given by: N 1 F zi B z surf T f z surf , zi B zk 1 / 2 * T f z i , zk 1 T f z i , zk (A10) k i N 1 F zi B zk 1 / 2 * T f z i , zk 1 T f z i , zk k i 2 (A11) Finite-difference derivatives of net flux produce flux divergence which is scaled to produce the cooling rate profile. Evaluation of analytic derivatives with respect to altitude for cooling rate profile calculation is generally avoided due to the inconsistency between the vertical coordinate scheme needed for accurate radiative transfer calculations and the Lipschitz condition [Jeffreys, 1988] which is necessary for derivative stability. The band models are typically evaluated over the fewest bands while minimizing the variation of the Planck function across the band and minimizing overlap between absorptions from different species. For the longwave, 10-15 bands are generally sufficient for reasonable accuracy for tropospheric and lower-stratospheric fluxes and cooling rates 3 B. Linear Bayesian Retrieval: There is a vast amount of literature devoted to appropriately balancing the information derived from a measurement with prior understanding of the retrieval target. For detailed discussions, see Twomey (1977), Hansen (1998), and Rodgers (2000). If we limit the treatment of the retrieval to a first-order analysis which is the linear Bayesian retrieval, the following analysis, summarized from Rodgers [2000], is sufficient: The conditional probability distribution function (pdf) of the retrieval target x (i.e. the profile of O3 or, for this study, the cooling rate profile) given the measurement y is described by Bayes’ Theorem: Px | y P(y | x) P(x) P( y ) (B1) where P (x ) is the prior pdf of the state x such that P (x)dx is the probability that x lies within x, x dx , P (y ) is the prior pdf of the measurement with similar meaning as P (x ) , P(y | x) is the conditional pdf of y given x such that P(y | x)dy is the probability that y lies in y, y dy when x has a certain value. A linear retrieval problem starts with the linearization of the forward model Fx : y Fx ε Kx ε (B2) where K is the Jacobian (sensitivity matrix) of the forward model with respect to the retrieval target and ε is a description of the uncertainty. If measurement error presents Gaussian statistics as it usually does: 2 ln P(y | x) y Kx Sε1 y Kx constant T (B3) where the T superscript denotes matrix transpose, the -1 superscript denotes matrix inverse, and S ε is the measurement covariance matrix which describes the estimated uncertainty in the measurement. Assuming that the retrieval target also presents Gaussian statistics: 2 ln P(x) x xa Sa1 x xa constant T (B4) x a is the a priori description of the retrieval target and S a is the covariance matrix of xa . Substituting Eq. (B4) and (B3) into Eq. (B1) yields: 4 2 ln P(x | y) y Kx Sε1 y Kx x x a S a1 x x a constant T T (B5) which is a quadratic form in x so we find that the retrieval statistics can be represented by: T 2 ln P(x | y ) x xˆ Sˆ 1 x xˆ constant (B6) where x̂ is the retrieved quantity and Ŝ is the covariance matrix of that quantity. By equating terms that are quadratic in x , we find that Ŝ is given by: Sˆ 1 KT Sε1K Sa1 (B7) and by equating terms that are linear in x , we find that xˆ K T S ε1K S a1 K S 1 T 1 ε y S a1x a (B8) This result allows for the incorporation of both a priori knowledge and the measurement and its uncertainty in order to derive an update to the retrieval target that is consistent with what is known. It also produces an estimate of the a posteriori uncertainty in the retrieval state which can be utilized in subsequent analysis using the retrieval results. The result in Eq. (B7) and (B8) lend readily to information content analysis. The information content of a measurement describes unidimensionally the amount of understanding derived about a multidimensional quantity as a result of an imperfect measurement. According to Shannon [1948], the information content can also be described by the entropy of the probability distribution functions associated with the a priori and a posteriori states. Given an assumption of Gaussian statistics for the quantity of interest, the entropy, and thus the information content can be directly related to the covariance matrix of the retrieval target: S Pa 1 log S a 2 log 2 H S Pf S Pa ˆ 1 H - 1 log S * S a 2 (B9) (B10) (B11) where S is the entropy of a state associated with Pa and Pf , the probability distributions of the retrieval target of the a priori and a posteriori states respectively. H is the information content in bits and the vertical bars denote the calculation of the matrix 5 determinant. Ultimately, this approach allows for the formal design of a retrieval system that optimizes with respect to the retrieval target information content. For the retrieval of profile quantities, it is useful to designate a method for determining the vertical resolution of the retrieval. That is, it is expected that the retrieval will be marginally sensitive to a perturbation of an infinitesimally thin layer associated with profile being retrieved. The averaging kernel matrix is conventionally utilized to understand this sensitivity and the entries in this matrix represent the sensitivity of the retrieved profile to a perturbation in the true profile. A xˆ x (B12) In order to associate the averaging kernel with a gross metric of resolution, the concept of the degrees of freedom of the signal is introduced as the number of statisticallyindependent quantities that can be retrieved for a profile retrieval. dof traceA (B13) Together, the degrees of freedom of the signal and the information content are useful for characterizing and optimizing a retrieval system. 6 C. Cooling Rate Retrieval Methods: Several papers have detailed methods for direct cooling rate retrievals using top-ofatmosphere measurements. Liou and Xue [1988] describe a relationship between radiance measurements across a spectral band and the cooling rate profile in that band. The original formulation for this cooling rate retrieval found that: 0 z K , z dz I I (C1) where K , z is a cooling rate weighting function that is K , z C p z T , z , (C2) by ansatz where refers to a wavenumber interval spanning an entire band (~ 100 cm-1), refers to higher spectral resolution measurements (~ 1 cm-1), and T , z, refers to the transmittance function between height z and outer space at viewing angle . From Eq. (C1) the term I refers to spectrally band-averaged radiance measured at a viewing angle of which is very similar to the angle used for the diffusivity approximation. The coefficients and are variables that depend on the ratio of band-averaged transmittance to spectral transmittance. This paper determined that the cooling rate retrieval is indeed feasible and numerically stable for cooling arising from the rotational bands of water vapor (far infrared), but many of the practical details associated with instrumentation viewing geometry requirements, spectral coverage, and a comparison between standard methods and direct retrieval methods were left to future research. Feldman et al [2006] utilized some of the methods described in Liou and Xue [1988] to retrieve the CO2 v2 band cooling rate from AIRS radiance data. This work found that, with a variety of assumptions based on cross-track scene correlation and empiricallyderived covariance matrices (see Mlynczak and Mertens, 1998), an optimal estimation theory approach to cooling rate retrievals using the AIRS instrument finds that the lower stratospheric cooling arising from the CO2 v2 band. 7 D. Conversion from spectral radiance to spectral flux Satellite-borne remote sensing observations necessarily measure radiance in order to achieve a reasonable spatial resolution. Wide field-of-view measurements that would actually measure top-of-atmosphere flux smear out the spatial heterogeneity while providing little information relevant to energy balance questions. However, circulation models calculate and utilize fluxes (and heating/cooling rates) extensively and calculate them with spatial resolution of several kilometers. Numerous efforts have been undertaken to address the practical conversion of top-of-atmosphere radiance measurements to high spatial-resolution top-of-atmosphere fluxes in order to address radiation balance issues. The Earth Radiation Budget Experiment and its successor the Clouds and Earth Radiant Energy System have been estimating broadband (1 shortwave, 2 longwave radiometers) top-of-atmosphere flux measurements for over two decades utilizing an advanced viewing geometry that observes the same footprint at several viewing angles. The central problem with the conversion from radiance measurements to flux is at odds with practical issues related to viewing geometry. The formal integration of radiance to produce flux is given by: F 2 0 /2 0 I , sin cos d d (D1) Since longwave radiance tends to vary minimally in the azimuthal direction, the conversion from radiance to flux is simplified as: F I d 1 (D2) 0 where cos . Formal numerical quadrature generally takes place through the use of interpolating functions. Newton-Cotes formulae are utilized where values of the integrand are measured at regularly-spaced integrals whereas Gaussian quadrature are 8 typically more accurate and can be utilized where the integrand can be evaluated at specifiable points throughout the interval of integration. Unfortunately, both methods of quadrature generally require evaluation of the integrand at points throughout most of the interval of integration and this requires extreme viewing angles from a satellite-borne platform. Therefore, a variety of methods have been developed for this brand of quadrature that essentially requires extrapolation at one integration end-point. Work by (SOURCES) have developed angular distribution models using empirically-derived, scene-specific anisotropic factors which are multiplied by the broadband radiance measurements to yield fluxes. The anisotropic factors are given by: * I , Fˆ R , (D3) where F̂ is the broadband (5-50 μm) IR flux estimated from broadband radiance radiance measurements at zenith and azimuth angles and respectively and R is the scene-specific angular distribution model which is derived empirically and the different scenes are classified according to surface type and cloud cover. These methods generally introduce only small errors into the calculation of fluxes and have allowed for large-scale atmospheric energetics studies. Estimated error introduction is less than 4 W/m2 for total OLR given proper scene type separation. Deriving spectral fluxes from TOA measurements, as is required by this research, has received much less attention, though it is arguably of great importance in the determination of whether models, which are correctly calculating the outgoing longwaveand shortwave-radiation (OLR and OSR respectively), are correctly describing the atmospheric state necessary to achieve OLR and OSR fluxes (SOURCE). In this case, a statistical approach to the estimation of TOA spectral fluxes is warranted. According to Huang et al (2006), estimation of tropical atmospheric fluxes from radiance measurements using the IRIS-D instrument can be performed according to the following: Fˆ s1, I s2, (D4) where s1, and s2, are regression coefficients. Total OLR error introduction using this approach is estimated at 2 W/m2. 9