Volume Extinction Coefficient Research Articles

Retrieving 3D distributions of atmospheric particles using Atmospheric Tomography with 3D Radiative Transfer – Part 2: Local optimization

Abstract. Our global understanding of clouds and aerosols relies on the remote sensing of their optical, microphysical, and macrophysical properties using, in part, scattered solar radiation. Current retrievals assume clouds and aerosols form plane-parallel, homogeneous layers and utilize 1D radiative transfer (RT) models. These assumptions limit the detail that can be retrieved about the 3D variability in the cloud and aerosol fields and induce biases in the retrieved properties for highly heterogeneous structures such as cumulus clouds and smoke plumes. In Part 1 of this two-part study, we validated a tomographic method that utilizes multi-angle passive imagery to retrieve 3D distributions of species using 3D RT to overcome these issues. That validation characterized the uncertainty in the approximate Jacobian used in the tomographic retrieval over a wide range of atmospheric and surface conditions for several horizontal boundary conditions. Here, in Part 2, we test the algorithm's effectiveness on synthetic data to test whether the retrieval accuracy is limited by the use of the approximate Jacobian. We retrieve 3D distributions of a volume extinction coefficient (σ3D) at 40 m resolution from synthetic multi-angle, mono-spectral imagery at 35 m resolution derived from stochastically generated cumuliform-type clouds in (1 km)3 domains. The retrievals are idealized in that we neglect forward-modelling and instrumental errors, with the exception of radiometric noise; thus, reported retrieval errors are the lower bounds. σ3D is retrieved with, on average, a relative root mean square error (RRMSE) < 20 % and bias < 0.1 % for clouds with maximum optical depth (MOD) < 17, and the RRMSE of the radiances is < 0.5 %, indicating very high accuracy in shallow cumulus conditions. As the MOD of the clouds increases to 80, the RRMSE and biases in σ3D worsen to 60 % and −35 %, respectively, and the RRMSE of the radiances reaches 16 %, indicating incomplete convergence. This is expected from the increasing ill-conditioning of the inverse problem with the decreasing mean free path predicted by RT theory and discussed in detail in Part 1. We tested retrievals that use a forward model that is not only less ill-conditioned (in terms of condition number) but also less accurate, due to more aggressive delta-M scaling. This reduces the radiance RRMSE to 9 % and the bias in σ3D to −8 % in clouds with MOD ∼ 80, with no improvement in the RRMSE of σ3D. This illustrates a significant sensitivity of the retrieval to the numerical configuration of the RT model which, at least in our circumstances, improves the retrieval accuracy. All of these ensemble-averaged results are robust in response to the inclusion of radiometric noise during the retrieval. However, individual realizations can have large deviations of up to 18 % in the mean extinction in clouds with MOD ∼ 80, which indicates large uncertainties in the retrievals in the optically thick limit. Using less ill-conditioned forward model tomography can also accurately infer optical depths (ODs) in conditions spanning the majority of oceanic cumulus fields (MOD < 80), as the retrieval provides ODs with bias and RRMSE values better than −8 % and 36 %, respectively. This is a significant improvement over retrievals using 1D RT, which have OD biases between −30 % and −23 % and RRMSE between 29 % and 80 % for the clouds used here. Prior information or other sources of information will be required to improve the RRMSE of σ3D in the optically thick limit, where the RRMSE is shown to have a strong spatial structure that varies with the solar and viewing geometry.

Retrieving 3D distributions of atmospheric particles using Atmospheric Tomography with 3D Radiative Transfer – Part 1: Model description and Jacobian calculation

Abstract. Our global understanding of clouds and aerosols relies on the remote sensing of their optical, microphysical, and macrophysical properties using, in part, scattered solar radiation. These retrievals assume that clouds and aerosols form plane-parallel, homogeneous layers and utilize 1D radiative transfer (RT) models, limiting the detail that can be retrieved about the 3D variability in cloud and aerosol fields and inducing biases in the retrieved properties for highly heterogeneous structures such as cumulus clouds and smoke plumes. To overcome these limitations, we introduce and validate an algorithm for retrieving the 3D optical or microphysical properties of atmospheric particles using multi-angle, multi-pixel radiances and a 3D RT model. The retrieval software, which we have made publicly available, is called Atmospheric Tomography with 3D Radiative Transfer (AT3D). It uses an iterative, local optimization technique to solve a generalized least squares problem and thereby find a best-fitting atmospheric state. The iterative retrieval uses a fast, approximate Jacobian calculation, which we have extended from Levis et al. (2020) to accommodate open and periodic horizontal boundary conditions (BCs) and an improved treatment of non-black surfaces. We validated the accuracy of the approximate Jacobian calculation for derivatives with respect to both the 3D volume extinction coefficient and the parameters controlling the open horizontal boundary conditions across media with a range of optical depths and single-scattering properties and find that it is highly accurate for a majority of cloud and aerosol fields over oceanic surfaces. Relative root mean square errors in the approximate Jacobian for a 3D volume extinction coefficient in media with cloud-like single-scattering properties increase from 2 % to 12 % as the maximum optical depths (MODs) of the medium increase from 0.2 to 100.0 over surfaces with Lambertian albedos <0.2. Over surfaces with albedos of 0.7, these errors increase to 20 %. Errors in the approximate Jacobian for the optimization of open horizontal boundary conditions exceed 50 %, unless the plane-parallel media providing the boundary conditions are optically very thin (∼0.1). We use the theory of linear inverse RT to provide insight into the physical processes that control the cloud tomography problem and identify its limitations, supported by numerical experiments. We show that the Jacobian matrix becomes increasing ill-posed as the optical size of the medium increases and the forward-scattering peak of the phase function decreases. This suggests that tomographic retrievals of clouds will become increasingly difficult as clouds become optically thicker. Retrievals of asymptotically thick clouds will likely require other sources of information to be successful. In Loveridge et al. (2023a; hereafter Part 2), we examine how the accuracy of the retrieved 3D volume extinction coefficient varies as the optical size of the target medium increases using synthetic data. We do this to explore how the increasing error in the approximate Jacobian and the increasingly ill-posed nature of the inversion in the optically thick limit affect the retrieval. We also assess the accuracy of retrieved optical depths and compare them to retrievals using 1D radiative transfer.

Assessment of Influence of Urban Aerosol Vertical Profile on Clear-Sky Diffuse Radiance Pattern

Abstract Aerosol particles spread in the atmosphere play an important role in solar light scattering and thus co-determine the sky radiance/luminance pattern as well as diffuse irradiances/illuminances at the ground. The particular influence is given by their optical properties and by their distribution in the atmosphere. The dependence of the aerosol extinction coefficient on altitude is usually described by the exponential law, which results from the averaging of a large number of aerosol realizations. This is also frequently the case of simulating of the solar diffuse radiance/luminance distribution over the sky, when it is based on solving the radiative transfer problem. However, the aerosol vertical profile can sometimes be significantly different from the exponential one. Mainly in the urban environment, the aerosol is often well-mixed within the atmospheric boundary layer, so its volume extinction coefficient is almost constant there. Under specific conditions also the so-called elevated aerosol layer may occur. This work investigates how such different profiles affect the clear sky radiance pattern and consequently also the ground-based horizontal diffuse irradiance. The numerical simulations revealed that the discrepancies are negligible in practice. So, it appears that the aerosol vertical distribution does not play any important role in sky radiance calculations, and the standard exponential law is general enough to cover also various specific aerosol conditions.

Simulation of false-alarm area of laser guidance based on Mie scattering model

In order to study the influence of backscattering of indicating laser in laser guidance process and laser guidance countermeasure test, the scattering function and volume extinction coefficient of typical aerosol distribution are calculated, and the backscattering detection model of 1.06 µm horizontally transmitted laser is established, based on Mie scattering theory and scattering function optimization algorithm; the model is used to study the change of backscattering energy detected by the detector at different positions and different detection angles, and the false-alarm area of laser guidance along the indicating laser path under different detection thresholds is obtained. The results can help to deepen the understanding of the influence of atmospheric scattering on the laser guidance process, and provide theoretical reference for the scheme design of the laser guidance countermeasure test.

Apparent dust size discrepancy in aerosol reanalysis in north African dust after long-range transport

Abstract. North African dust reaches the southeastern United States every summer. Size-resolved dust mass measurements taken in Miami, Florida, indicate that more than one-half of the surface dust mass concentrations reside in particles with geometric diameters less than 2.1 µm, while vertical profiles of micropulse lidar depolarization ratios show dust reaching above 4 km during pronounced events. These observations are compared to the representation of dust in the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) aerosol reanalysis and closely related Goddard Earth Observing System model version 5 (GEOS-5) Forward Processing (FP) aerosol product, both of which assimilate satellite-derived aerosol optical depths using a similar protocol and inputs. These capture the day-to-day variability in aerosol optical depth well, in a comparison to an independent sun-photometer-derived aerosol optical depth dataset. Most of the modeled dust mass resides in diameters between 2 and 6 µm, in contrast to the measurements. Model-specified mass extinction efficiencies equate light extinction with approximately 3 times as much aerosol mass, in this size range, compared to the measured dust sizes. GEOS-5 FP surface-layer sea salt mass concentrations greatly exceed observed values, despite realistic winds and relative humidities. In combination, these observations help explain why, despite realistic total aerosol optical depths, (1) free-tropospheric model volume extinction coefficients are lower than those retrieved from the micro-pulse lidar, suggesting too-low model dust loadings in the free troposphere, and (2) model dust mass concentrations near the surface can be higher than those measured. The modeled vertical distribution of dust, when captured, is reasonable. Large, aspherical particles exceeding the modeled dust sizes are also occasionally present, but dust particles with diameters exceeding 10 µm contribute little to the measured total dust mass concentrations after such long-range transport. Remaining uncertainties warrant a further integrated assessment to confirm this study's interpretations.

Micro-Pulse Lidar Cruising Measurements in Northern South China Sea

A shipborne micro-pulse lidar (Sigma Space Mini-MPL) was used to measure aerosol extinction coefficient over the northern region of the South China Sea from 9 August to 7 September 2016, the first time a mini-MPL was used for aerosol observation over the cruise region. The goal of the experiment was to investigate if the compact and affordable mini-MPL was usable for aerosol observation over this region. The measurements were used to calculate vertical profiles of volume extinction coefficient, depolarization ratio, and atmospheric boundary layer height. Aerosol optical depth (AOD) was lower over the southwest side of the cruise region, compared to the northeast side. Most attenuation occurred below 3.5 km, and maximum extinction values over coastal areas were generally about double of values offshore. The extinction coefficients at 532 nm (aerosol and molecular combined) over coastal and offshore areas were on average 0.04 km−1 and 0.02 km−1, respectively. Maximum values reached 0.2 km−1 and 0.14 km−1, respectively. Vertical profiles and back-trajectory calculations indicated vertical and horizontal layering of aerosols from different terrestrial sources. The mean volume depolarization ratio of the aerosols along the cruise was 0.04. The mean atmospheric boundary layer height along the cruise was 653 m, with a diurnal cycle reaching its mean maximum of 1041 m at 12:00 local time, and its mean minimum of 450 m at 20:00 local time. Unfortunately, only 11% of the measurements were usable. This was due to ship instability in rough cruise conditions, lack of stabilization rig, water condensation attached to the eye lens, and high humidity attenuating the echo signal. We recommend against the use of the mini-MPL in this cruise region unless substantial improvements are made to the default setup, e.g., instrument stabilization, instrument protection cover, and more theoretical work taking into account atmospheric gas scattering or absorption.

Reduction of Bias from Parameter Variance in Geophysical Data Estimation: Method and Application to Ice Water Content and Sedimentation Flux Estimated from Lidar

Abstract This paper addresses issues of statistical misrepresentation of the a priori parameters (henceforth called ancillary parameters) used in geophysical data estimation. Parameterizations using ancillary data are frequently needed to derive geophysical data of interest from remote measurements. Empirical fits to the ancillary data that do not preserve the distribution of such data may induce substantial bias. A semianalytical averaging approach based on Taylor expansion is presented to improve estimated cirrus ice water content and sedimentation flux for a range of volume extinction coefficients retrieved from spaceborne lidar observations by CALIOP combined with the estimated distribution of ancillary data from in situ aircraft measurements of ice particle microphysical parameters and temperature. It is shown that, given an idealized distribution of input parameters, the approach performs well against Monte Carlo benchmark predictions. Using examples with idealized distributions at the mean temperature for the tropics at 15 km, it is estimated that the commonly neglected variance observed in in situ measurements of effective diameters may produce a worst-case estimation bias spanning up to a factor of 2. For ice sedimentation flux, a similar variance in particle size distributions and extinctions produces a worst-case estimation bias of a factor of 9. The value of the bias is found to be mostly set by the correlation coefficient between extinction and ice effective diameter, which in this test ranged between all possible values. Systematic reporting of variances and covariances in the ancillary data and between data and observed quantities would allow for more accurate observational estimates.

Establishment of high-resolution aerosol parameterization and its influence on radiation calculations

To accurately simulate the effects of aerosols on the atmospheric radiation budget, we here establish an aerosol optical parameterization scheme with high spectral resolution (974-band) for radiative transfer model(BCC_RAD); this scheme includes sulfate (SF), black carbon (BC), organic carbon (OC), dust (SD), and sea salt (SS) aerosols. The results of the 974-band scheme are compared with those obtained using a low-resolution 17-band scheme. Our results show the 974-band scheme more accurate in its representation of the aerosols’ optical properties. The largest relative differences in the volume extinction coefficient(Kex) between the 974-band and 17-band schemes range from 5.87% to 54.64%, with BC (41.13%) and SF (54.64%) showing the largest values at 1.91 and 2.7 μm, respectively. The single scattering albedo of hygroscopic aerosols (SF, SS, and OC) show minimal values at 2.84 and 6.01 μm, respectively, in the 974-band scheme due to light absorption; however, the low spectral resolution of the 17-band scheme prevents these features from being resolved. Specifically, the relative difference between the two schemes approaches 72.72% at 2.84 μm for SF. Thus, improved spectral resolution may be required for some aerosols.We also compare the effects of aerosols on the radiation budget in East Asia simulated by 974-band and 17-band BCC_RAD models. Under clear-sky conditions, the simulation results indicate a relative difference in the radiation flux of 0.28–5.93% for the two schemes. The 974-band and 17-band schemes show daily mean direct radiative forcings (DRFs) due to all aerosols of −16.97 and −17.13 W/m2 at the surface and −7.12 and −6.93 W/m2 at the top of the atmosphere, respectively. Additionally, the 974-band model generally simulates a larger DRF for BC and smaller DRFs for scattering aerosols such as SF; these differences become greater for smaller zenith angles.

Engineering equations for the filamentation collapse distance in lossy, turbulent, nonlinear media.

The propagation of high peak-power laser beams in real atmospheres has been an active research area for a couple of decades. Atmospheric turbulence and loss will induce decreases in the filamentation self-focusing collapse distance as the refractive index structure parameter and volume extinction coefficient, respectively, increase. This paper provides a validated analytical method for predicting the filamentation onset distance in lossy, turbulent, nonlinear media. It is based on a modification of Petrishchev's and Marburger theories. It postulates that the ratio of the peak power to critical power at range in turbulence is modified by a multiplicative, rather than additive, gain factor. Specifically, this new approach modifies the Petrishchev's turbulence equation to create the required multiplicative factor. This is necessary to create the shortened filamentation onset distance that occurs when a laser beam propagates through the cited nonlinear medium. This equation then is used with the Marburger distance and the Karr et al loss equations to yield the filamentation onset distance estimate in lossy, turbulent, nonlinear environment. Theory validation is done against two independent sets of computer simulation results. One comes from the NRL's HELCAP software and the other from MZA's Wave Train modeling software package. This paper also shows that once the zero-turbulence onset distance is set based on link loss, the addition of turbulence creates essentially the same PDFs at similar median distances for each loss case. This result had not been previously reported. This is the first quantitative comparison between closed form equations and computer simulation results characterizing filament generation in a lossy, turbulent, nonlinear medium.

Ground-Level PM2.5 Concentration Estimation from Satellite Data in the Beijing Area Using a Specific Particle Swarm Extinction Mass Conversion Algorithm

Particulate matter (PM) has a substantial influence on the environment, climate change and public health. Due to the limited spatial coverage of a ground-level PM2.5 monitoring system, the ground-based PM2.5 concentration measurement is insufficient in many circumstances. In this paper, a Specific Particle Swarm Extinction Mass Conversion Algorithm (SPSEMCA) using remotely sensed data is introduced. Ground-level observed PM2.5, planetary boundary layer height (PBLH) and relative humidity (RH) reanalyzed by the European Centre for Medium-Range Weather Forecasts (ECMWF) and aerosol optical depth (AOD), fine-mode fraction (FMF), particle size distribution, and refractive indices from AERONET (Aerosol Robotic Network) of the Beijing area in 2015 were used to establish this algorithm, and the same datasets for 2016 were used to test the performance of the SPSEMCA. The SPSEMCA involves four steps to obtain PM2.5 values from AOD datasets, and every step has certain advantages: (I) In the particle correction, we use η2.5 (the extinction fraction caused by particles with a diameter less than 2.5 μm) to make an accurate assimilation of AOD2.5, which is contributed to by the specific particle swarm PM2.5. (II) In the vertical correction, we compare the performance of PBLHc retrieved by satellite Lidar CALIPSO data and PBLHe reanalysis by ECMWF. Then, PBLHc is used to make a systematic correction for PBLHe. (III) For extinction to volume conversion, the relative humidity and the FMF are used together to assimilate the AVEC (averaged volume extinction coefficient, μm2/μm3). (IV) PM2.5 measured by ground-based air quality stations are used as the dry mass concentration when calculating the AMV (averaged mass volume, cm3/g) in humidity correction, that will avoid the uncertainties derived from the estimation of the particulate matter density ρ. (V) Multi-Angle Implementation of Atmospheric Correction (MAIAC) 1 km × 1 km AOD was used to retrieve high resolution PM2.5, and a LookUP Table-based Spectral Deconvolution Algorithm (LUT-SDA) FMF was used to avoid the large uncertainties caused by the MODIS FMF product. The validation of PM2.5 from the SPSEMCA algorithm to the AERONET observation data and MODIS monitoring data achieved acceptable results, R = 0.70, RMSE (root mean square error) = 58.75 μg/m3 for AERONET data, R = 0.75, RMSE = 43.38 μg/m3 for MODIS data, respectively. Furthermore, the trend of the temporal and spatial distribution of Beijing was revealed.

Evaluation of the operational Aerosol Layer Height retrieval algorithm for Sentinel-5 Precursor: application to O<sub>2</sub> A band observations from GOME-2A

Abstract. An algorithm setup for the operational Aerosol Layer Height product for TROPOMI on the Sentinel-5 Precursor mission is described and discussed, applied to GOME-2A data, and evaluated with lidar measurements. The algorithm makes a spectral fit of reflectance at the O2 A band in the near-infrared and the fit window runs from 758 to 770 nm. The aerosol profile is parameterised by a scattering layer with constant aerosol volume extinction coefficient and aerosol single scattering albedo and with a fixed pressure thickness. The algorithm's target parameter is the height of this layer. In this paper, we apply the algorithm to observations from GOME-2A in a number of systematic and extensive case studies, and we compare retrieved aerosol layer heights with lidar measurements. Aerosol scenes cover various aerosol types, both elevated and boundary layer aerosols, and land and sea surfaces. The aerosol optical thicknesses for these scenes are relatively moderate. Retrieval experiments with GOME-2A spectra are used to investigate various sensitivities, in which particular attention is given to the role of the surface albedo. From retrieval simulations with the single-layer model, we learn that the surface albedo should be a fit parameter when retrieving aerosol layer height from the O2 A band. Current uncertainties in surface albedo climatologies cause biases and non-convergences when the surface albedo is fixed in the retrieval. Biases disappear and convergence improves when the surface albedo is fitted, while precision of retrieved aerosol layer pressure is still largely within requirement levels. Moreover, we show that fitting the surface albedo helps to ameliorate biases in retrieved aerosol layer height when the assumed aerosol model is inaccurate. Subsequent retrievals with GOME-2A spectra confirm that convergence is better when the surface albedo is retrieved simultaneously with aerosol parameters. However, retrieved aerosol layer pressures are systematically low (i.e., layer high in the atmosphere) to the extent that retrieved values no longer realistically represent actual extinction profiles. When the surface albedo is fixed in retrievals with GOME-2A spectra, convergence deteriorates as expected, but retrieved aerosol layer pressures become much higher (i.e., layer lower in atmosphere). The comparison with lidar measurements indicates that retrieved aerosol layer heights are indeed representative of the underlying profile in that case. Finally, subsequent retrieval simulations with two-layer aerosol profiles show that a model error in the assumed profile (two layers in the simulation but only one in the retrieval) is partly absorbed by the surface albedo when this parameter is fitted. This is expected in view of the correlations between errors in fit parameters and the effect is relatively small for elevated layers (less than 100 hPa). If one of the scattering layers is near the surface (boundary layer aerosols), the effect becomes surprisingly large, in such a way that the retrieved height of the single layer is above the two-layer profile. Furthermore, we find that the retrieval solution, once retrieval converges, hardly depends on the starting values for the fit. Sensitivity experiments with GOME-2A spectra also show that aerosol layer height is indeed relatively robust against inaccuracies in the assumed aerosol model, even when the surface albedo is not fitted. We show spectral fit residuals, which can be used for further investigations. Fit residuals may be partly explained by spectroscopic uncertainties, which is suggested by an experiment showing the improvement of convergence when the absorption cross section is scaled in agreement with Butz et al. (2013) and Crisp et al. (2012), and a temperature offset to the a priori ECMWF temperature profile is fitted. Retrieved temperature offsets are always negative and quite large (ranging between −4 and −8 K), which is not expected if temperature offsets absorb remaining inaccuracies in meteorological data. Other sensitivity experiments investigate fitting of stray light and fluorescence emissions. We find negative radiance offsets and negative fluorescence emissions, also for non-vegetated areas, but from the results it is not clear whether fitting these parameters improves the retrieval. Based on the present results, the operational baseline for the Aerosol Layer Height product currently will not fit the surface albedo. The product will be particularly suited for elevated, optically thick aerosol layers. In addition to its scientific value in climate research, anticipated applications of the product for TROPOMI are providing aerosol height information for aviation safety and improving interpretation of the Absorbing Aerosol Index.

Vertical structure and optical properties of Titan’s aerosols from radiance measurements made inside and outside the atmosphere

Prompted by the detection of stratospheric cloud layers by Cassini’s Composite Infrared Spectrometer (CIRS; see Anderson, C.M., Samuelson, R.E. [2011]. Icarus 212, 762–778), we have re-examined the observations made by the Descent Imager/Spectral Radiometer (DISR) in the atmosphere of Titan together with two constraints from measurements made outside the atmosphere. No evidence of thin layers (<1km) in the DISR image data sets is seen beyond the three previously reported layers at 21km, 11km, and 7km by Karkoschka and Tomasko (Karkoschka, E., Tomasko, M.G. [2009]. Icarus 199, 442–448). On the other hand, there is evidence of a thicker layer centered at about 55km. A rise in radiance gradients in the Downward-Looking Visible Spectrometer (DLVS) data below 55km indicates an increase in the volume extinction coefficient near this altitude. To fit the geometric albedo measured from outside the atmosphere the decrease in the single scattering albedo of Titan’s aerosols at high altitudes, noted in earlier studies of DISR data, must continue to much higher altitudes. The altitude of Titan’s limb as a function of wavelength requires that the scale height of the aerosols decrease with altitude from the 65km value seen in the DISR observations below 140km to the 45km value at higher altitudes. We compared the variation of radiance with nadir angle observed in the DISR images to improve our aerosol model. Our new aerosol model fits the altitude and wavelength variations of the observations at small and intermediate nadir angles but not for large nadir angles, indicating an effect that is not reproduced by our radiative transfer model. The volume extinction profiles are modeled by continuous functions except near the enhancement level near 55km altitude. The wavelength dependence of the extinction optical depth is similar to earlier results at wavelengths from 500 to 700nm, but is smaller at shorter wavelengths and larger toward longer wavelengths. A Hapke-like model is used for the ground reflectivity, and the variation of the Hapke single scattering albedo with wavelength is given. Fits to the visible spectrometers looking upward and downward are achieved except in the methane bands longward of 720nm. This is possibly due to uncertainties in extrapolation of laboratory measurements from 1km-am paths to much longer paths at lower pressures. It could also be due to changes in the single scattering phase functions at low altitudes, which strongly affect the path length through methane that the photons travel. We demonstrate the effects on the model fits by varying each model parameter individually in order to illustrate the sensitivity of our determination of each model parameter.

A new ice cloud parameterization for infrared radiative transfer simulation of cloudy radiances: Evaluation and optimization with IIR observations and ice cloud profile retrieval products

AbstractA new ice cloud optical property database in the thermal infrared has been parameterized for the RTTOV radiative transfer model. The Self‐Consistent Scattering Model (SCSM) database is based on an ensemble model of ice crystals and a parameterization of the particle size distribution. This convolution can predict the radiative properties of cirrus without the need of a priori information on the ice particle shape and an estimate of the ice crystal effective dimension. The ice cloud optical properties are estimated through linear parameterizations of ambient temperature and ice water content. We evaluate the new parameterization against existing parameterizations used in RTTOV. We compare infrared observations from Imaging Infrared Radiometer, on board CALIPSO, against RTTOV simulations of the observations. The simulations are performed using two different products of ice cloud profiles, retrieved from the synergy between space‐based radar and lidar observations. These are the 2C‐ICE and DARDAR products. We optimized the parameterization by testing different SCSM databases, derived from different shapes of the particle size distribution, and weighting the volume extinction coefficient of the ensemble model. By selecting a large global data set of ice cloud profiles of visible optical depths between 0.03 and 4, we found that the simulations, based on the optimized SCSM database parameterization, reproduces the observations with a mean bias of only 0.43 K and a standard deviation of 6.85 K. The optimized SCSM database parameterization can also be applied to any other radiative transfer model.

A new parameterization for ice cloud optical properties used in BCC-RAD and its radiative impact

A new parameterization of the solar and infrared optical properties of ice clouds that considers the multiple habits of ice particles was developed on the basis of a prescribed dataset. First, the fitting formulae of the bulk extinction coefficient, single-scatter albedo, asymmetry factor, and δ-function forward-peak factor at the given 65 wavelengths as a function of effective radius were created for common scenarios, which consider a greater number of wavelengths and are more accurate than those used previously. Then, the band-averaged volume extinction and absorption coefficients, asymmetry factor and forward-peak factor of ice cloud were derived for the BCC-RAD (Beijing Climate Center radiative transfer model) using a parameter reference table. Finally, the newly developed and the original schemes in the BCC-RAD and the commonly used Fu Scheme of ice cloud were all applied to the BCC-RAD. Their influences on radiation calculations were compared using the mid-latitude summer atmospheric profile with ice clouds under no-aerosol conditions, and produced a maximum difference of approximately 30.0W/m2 for the radiative flux, and 4.0K/d for the heating rate. Additionally, a sensitivity test was performed to investigate the impact of the ice crystal density on radiation calculations using the three schemes. The results showed that the maximum difference was 68.1W/m2 for the shortwave downward radiative flux (for the case of perpendicular solar insolation), and 4.2K/d for the longwave heating rate, indicating that the ice crystal density exerts a significant effect on radiation calculations for a cloudy atmosphere.

Calculations of relative optical air masses for various aerosol types and minor gases in Arctic and Antarctic atmospheres

AbstractThe dependence functions of relative optical air mass on apparent solar zenith angle θ have been calculated over the θ &lt; 87° range for the vertical profiles of wet‐air molecular number density in the Arctic and Antarctic atmospheres, extinction coefficients of different aerosol types, and molecular number density of water vapor, ozone, nitrogen dioxide, and oxygen dimer. The calculations were made using as weight functions the seasonal average vertical profiles of (i) pressure and temperature derived from multiyear sets of radiosounding measurements performed at Ny‐Ålesund, Alert, Mario Zucchelli, and Neumayer stations; (ii) volume extinction coefficients of background summer aerosol, Arctic haze, and Kasatochi and Pinatubo volcanic aerosol measured with lidars or balloon‐borne samplings; and (iii) molecular number concentrations of the above minor gases, derived from radiosonde, ozonesonde, and satellite‐based observations. The air mass values were determined using a formula based on a realistic atmospheric air‐refraction model. They were systematically checked by comparing their mutual differences with the uncertainties arising from the seasonal and daily variations in pressure and temperature conditions within the various ranges, where aerosol and gases attenuate the solar radiation most efficiently. The results provide evidence that secant‐approximated and midlatitude air mass values are inappropriate for analyzing the Sun photometer measurements performed at polar sites. They indicate that the present evaluations can be reliably used to estimate the aerosol optical depth from the Arctic and Antarctic measurements of total optical depth, after appropriate corrections for the Rayleigh scattering and gaseous absorption optical depths.

Relationships between Ice Water Content and Volume Extinction Coefficient from In Situ Observations for Temperatures from 0° to −86°C: Implications for Spaceborne Lidar Retrievals

AbstractAn examination of 2 yr of Cloud–Aerosol Lidar Infrared Pathfinder Satellite Observations (CALIPSO) lidar observations and CloudSat cloud radar observations shows that ice clouds at temperatures below about −45°C frequently fall below the CloudSat radar’s detection threshold yet are readily detectable by the lidar. The CALIPSO ice water content (IWC) detection threshold is about 0.1 versus 5 mg m−3 for CloudSat. This comparison emphasizes the need for developing a lidar-only IWC retrieval method that is reliable for high-altitude ice clouds at these temperatures in this climatically important zone of the upper troposphere. Microphysical measurements from 10 aircraft field programs, spanning latitudes from the Arctic to the tropics and temperatures from −86° to 0°C, are used to develop relationships between the IWC and volume extinction coefficient σ in visible wavelengths. Relationships used to derive a radiatively important ice cloud property, the ice effective diameter De, from σ are also developed. Particle size distributions (PSDs) and direct IWC measurements, together with evaluations of the ice particle shapes and comparisons with semidirect extinction measurements, are used in this analysis. Temperature-dependent De(σ) and IWC–σ relationships developed empirically facilitate the retrieval of IWC from lidar-derived σ and De values and for comparison with other IWC observations. This suite of empirically derived relationships can be expressed analytically. These relationships can be used to derive IWC and De from σ and are developed for use in climate models to derive σ from prognosed values of IWC and specified PSD properties.

A self‐consistent scattering model for cirrus. II: The high and low frequencies

AbstractThe predictive quality of an ensemble model of cirrus ice crystals to model passive and active measurements of ice cloud, from the ultraviolet (UV) to the microwave, is tested. The ensemble model predicts m ∝ D2, where D is the maximum dimension of the ice crystal, and m is its mass. This predicted m‐D relationship is applied to a moment estimation parametrization of the particle size distribution (PSD), to estimate the PSD shape, given ice water content (IWC) and in‐cloud temperature. The same microphysics is applied across the electromagnetic spectrum to model UV, infrared, microwave and radar observations. The short‐wave measurements consist of airborne UV backscatter lidar (light detection and ranging) estimates of the volume extinction coefficient, total solar optical depth, and space‐based multi‐directional spherical albedo retrievals, at 0.865 µm, between the scattering angles 85° and 125°. The airborne long‐wave measurements consist of high‐resolution interferometer upwelling brightness temperatures, obtained between the wavelengths of about 3.45 µm and 4.1 µm, and 8.0 µm to 12.0 µm. The low‐frequency measurements consist of ground‐based Chilbolton 35 GHz radar reflectivity measurements and space‐based upwelling 190 GHz brightness temperature measurements. The predictive quality of the ensemble model is demonstrated to be generally within the experimental uncertainty of the lidar backscatter estimates of the volume extinction coefficient and total solar optical depth. The ensemble model prediction of the high‐resolution brightness temperature measurements is generally within ±2 K and ±1 K at solar and infrared wavelengths, respectively. The 35 GHz radar reflectivity and 190 GHz brightness temperatures are generally simulated to within ±2 dBZe, and ±2 K, respectively. The directional spherical albedo observations suggest that the scattering phase function of the most randomized ensemble model gives the best fit to the measurements (generally within ±3%). This article demonstrates that the ensemble model, assuming the same microphysics, is physically consistent across the electromagnetic spectrum.

Cloud ice water content retrieved from the CALIOP space‐based lidar

Ice water content (IWC) profiles are derived from retrievals of optical extinction from the Cloud‐Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite lidar, using a parameterization derived from particle probe measurements acquired during several aircraft field campaigns. With more than five years of data now available, CALIOP IWC is well suited for characterization of the climate‐sensitive upper troposphere/lower stratosphere where reliable global IWC measurements are needed to reduce climate model uncertainty. We describe CALIOP IWC and compare it with global satellite‐based and regional airborne IWC measurements made during August 2007. IWC distributions in a convective cloud sampled during the Tropical Clouds, Chemistry, Composition and Climate experiment show temperature‐dependent differences betweenin situmeasured IWC, IWC retrieved from CloudSat and CALIOP, and IWC parameterized from the airborne Cloud Physics Lidar (CPL) 532 nm volume extinction coefficients. At temperatures above −50°C the CALIOP IWC retrieval indicates less cloud ice than the other instruments, due to signal attenuation and screening for horizontally‐oriented ice crystals. Above 12 km where temperatures drop below −50°C CALIOP compares well within situ IWC measurements. In situmeasurements are limited above 12 km, and more cold‐temperature comparisons are needed. Global zonal in‐cloud IWC averages at altitudes above 9 km show that CloudSat IWC is roughly an order of magnitude higher than CALIOP IWC, consistent with a higher detection threshold. When averaged to the vertical resolution characteristic of Microwave Limb Sounder (MLS), global zonal averages of CALIOP and MLS IWC were found to agree to about +/−50%.

Infrared Extinction Properties of Nanostructured and Conventional Particles

Brass flakes and carbon-based particulates are effective obscurants in the infrared (IR) region of the electromagnetic spectrum; however, they are toxic and can cause respiratory problems and environmental concerns. There is a need to develop or identify nontoxic IR obscurants. This research was conducted to determine the potential of nanostructured particles as IR obscurants. Three commercial nanostructured particles were compared with two conventional particles and common obscurants. Experiments involved dispersing a known mass of particles into a particle chamber and measuring the IR transmission through the chamber with a Fourier transform infrared analyzer and the mass concentration with filter samplers. The size distribution of the aerosolized particles was also measured with an aerodynamic particle sizer spectrometer. From the measured data, the mean values of the mass extinction coefficient, σm, and volume extinction coefficient, σv, for the spectral bands of interest (i.e., 3–5 μm and 8–12 μm) were calculated. Results showed that ISO fine test dust, NaHCO3 and NanoActive TiO2 (for 3–5 μm) appeared to be the most promising alternatives to brass or graphite flakes. By manipulating the size and/or morphology of these particles, it might be possible to enhance their IR extinction performance.

Titan’s aerosol and stratospheric ice opacities between 18 and 500 μm: Vertical and spectral characteristics from Cassini CIRS

Vertical distributions and spectral characteristics of Titan’s photochemical aerosol and stratospheric ices are determined between 20 and 560 cm −1 (500–18 μm) from the Cassini Composite Infrared Spectrometer (CIRS). Results are obtained for latitudes of 15°N, 15°S, and 58°S, where accurate temperature profiles can be independently determined. In addition, estimates of aerosol and ice abundances at 62°N relative to those at 15°S are derived. Aerosol abundances are comparable at the two latitudes, but stratospheric ices are ∼3 times more abundant at 62°N than at 15°S. Generally, nitrile ice clouds (probably HCN and HC 3N), as inferred from a composite emission feature at ∼160 cm −1, appear to be located over a narrow altitude range in the stratosphere centered at ∼90 km. Although most abundant at high northern latitudes, these nitrile ice clouds extend down through low latitudes and into mid southern latitudes, at least as far as 58°S. There is some evidence of a second ice cloud layer at ∼60 km altitude at 58°S associated with an emission feature at ∼80 cm −1. We speculate that the identify of this cloud may be due to C 2H 6 ice, which in the vapor phase is the most abundant hydrocarbon (next to CH 4) in the stratosphere of Titan. Unlike the highly restricted range of altitudes (50–100 km) associated with organic condensate clouds, Titan’s photochemical aerosol appears to be well-mixed from the surface to the top of the stratosphere near an altitude of 300 km, and the spectral shape does not appear to change between 15°N and 58°S latitude. The ratio of aerosol-to-gas scale heights range from 1.3–2.4 at about 160 km to 1.1–1.4 at 300 km, although there is considerable variability with latitude. The aerosol exhibits a very broad emission feature peaking at ∼140 cm −1. Due to its extreme breadth and low wavenumber, we speculate that this feature may be caused by low-energy vibrations of two-dimensional lattice structures of large molecules. Examples of such molecules include polycyclic aromatic hydrocarbons (PAHs) and nitrogenated aromatics. Finally, volume extinction coefficients N χ E derived from 15°S CIRS data at a wavelength of λ = 62.5 μm are compared with those derived from the 10°S Huygens Descent Imager/Spectral Radiometer (DISR) data at 1.583 μm. This comparison yields volume extinction coefficient ratios N χ E (1.583 μm)/N χ E (62.5 μm) of roughly 70 and 20, respectively, for Titan’s aerosol and stratospheric ices. The inferred particle cross-section ratios χ E (1.583 μm)/ χ E (62.5 μm) appear to be consistent with sub-micron size aerosol particles, and effective radii of only a few microns for stratospheric ice cloud particles.