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PACE Technical Report Series, Volume 4: Cloud Retrievals in the PACE Mission: PACE Science Team Consensus Document

Earth is a complex dynamical system exhibiting continuous change in its atmosphere, ocean,and surface elements. Nearly all (99.97%) of the energy driving these systems is linked to the Sun. Measurements of reflected sunlight contain a unique signature of wavelength-specific scattering and absorption interactions occurring between incoming solar energy and atmospheric (molecules, aerosols,clouds) and surface features Clouds can affect significantly both shortwave and long wave radiation, depending on altitude/vertical structure, thermodynamic phase, and optical properties. Low, warm, and optically thick clouds predominantly have a cooling effect, while high, cold, optically thin clouds can cause warming by absorbing warmer radiation emitted from the surface and lower atmosphere.When the net difference between outgoing and incoming solar radiation is matched by the net infrared radiation emitted to space, the Earth's climate is in radiative balance. While radiative forcing components (GHGs, aerosols - direct and indirect) contribute to a net radiative imbalance, climate sensitivity is ultimately determined by the contribution of various system feed backs. The role of cloud feedback in a warming climate is currently the largest inter-model uncertainty in climate sensitivity and therefore in climate prediction [Bony and Dufresne 2005]. A comprehensive understanding of current cloud propertiesand dynamic/microphysical processes requires a global perspective from satellites.

Plankton, Aerosol, Cloud, ocean Ecosystem (PACE)↗

The 2175-A feature from irradiated graphitic particles

In diffuse clouds, a subpopulation of the carbon grains is graphitized by UV starlight during cloud lifetimes of roughly 100 Myr. Graphitic dust created in this way will behave like monosize Rayleigh particles and produce a 2175-A absorption band showing a Lorentzian profile. A physical model is outlined in which the strength and width of the band correlate with the dust grain environment, but the central wavelength is fixed by the Froehlich frequency for surface plasmons in a homogeneous sphere. On this model, the band appears strong and narrow only in dust clouds where the flux of UV starlight is high and the H atom gas density is low. The width of the band increases from diffuse to dense clouds mainly as a result of gas-phase H atoms accreted on to the grain surface. It is shown that hydrogenation weakens the band in dense clouds, and thus explains the anticorrelation between band strength and high carbon depletion. The model as a whole uses only 30 percent of the cosmic carbon and gives good agreement with observations of the 2175-A feature and the average interstellar extinction law.

Sorrell, Wilfred H.↗

The O{sub 2} A-Band in the Fluxes and Polarization of Starlight Reflected by Earth-Like Exoplanets

Earth-like, potentially habitable exoplanets are prime targets in the search for extraterrestrial life. Information about their atmospheres and surfaces can be derived by analyzing the light of the parent star reflected by the planet. We investigate the influence of the surface albedo A {sub s}, the optical thickness b {sub cloud}, the altitude of water clouds, and the mixing ratio of biosignature O{sub 2} on the strength of the O{sub 2} A-band (around 760 nm) in the flux and polarization spectra of starlight reflected by Earth-like exoplanets. Our computations for horizontally homogeneous planets show that small mixing ratios ( η < 0.4) will yield moderately deep bands in flux and moderate-to-small band strengths in polarization, and that clouds will usually decrease the band depth in flux and the band strength in polarization. However, cloud influence will be strongly dependent on properties such as optical thickness, top altitude, particle phase, coverage fraction, and horizontal distribution. Depending on the surface albedo and cloud properties, different O{sub 2} mixing ratios η can give similar absorption-band depths in flux and band strengths in polarization, especially if the clouds have moderate-to-high optical thicknesses. Measuring both the flux and the polarization is essential to reduce the degeneracies, although it will not solve them, especially not for horizontally inhomogeneous planets. Observations at a wide range of phase angles and with a high temporal resolution could help to derive cloud properties and, once those are known, the mixing ratio of O{sub 2} or any other absorbing gas.

79 ASTRONOMY AND ASTROPHYSICS↗

First astronomical detection of the cumulene carbon chain molecule H2C6 in TMC-1

The cumulene carbenes are important components of hydrocarbon chemistry in low-mass star-forming cores. Here we report the first astronomical detection of the long-chain cumulene carbene H2C6 in the interstellar cloud TMC-1, from observations of two of its rotational transitions: J(K,K') = 7(1,7) --> 6(1,6) at 18.8 GHz and 8(1,8) --> 7(1,7) at 21.5 GHz, using NASA's Deep Space Network 70 m antenna at Goldstone, California. In addition we also observed the shorter cumulene carbene H2C4 at the same position. The fractional abundance of H2C6 relative to H2 is about 4.7 x 10(-11) and that of H2C4 is about 4.1 x 10(-9). The abundance of H2C6 is in fairly good agreement with gas-phase chemical models for young molecular cloud cores, but the abundance of H2C4 is significantly larger than predicted.

NASA Discipline Exobiology↗

Windowed and Wavelet Analysis of Marine Stratocumulus Cloud Inhomogeneity

To improve radiative transfer calculations for inhomogeneous clouds, a consistent means of modeling inhomogeneity is needed. One current method of modeling cloud inhomogeneity is through the use of fractal parameters. This method is based on the supposition that cloud inhomogeneity over a large range of scales is related. An analysis technique named wavelet analysis provides a means of studying the multiscale nature of cloud inhomogeneity. In this paper, the authors discuss the analysis and modeling of cloud inhomogeneity through the use of wavelet analysis. Wavelet analysis as well as other windowed analysis techniques are used to study liquid water path (LWP) measurements obtained during the marine stratocumulus phase of the First ISCCP (International Satellite Cloud Climatology Project) Regional Experiment. Statistics obtained using analysis windows, which are translated to span the LWP dataset, are used to study the local (small scale) properties of the cloud field as well as their time dependence. The LWP data are transformed onto an orthogonal wavelet basis that represents the data as a number of times series. Each of these time series lies within a frequency band and has a mean frequency that is half the frequency of the previous band. Wavelet analysis combined with translated analysis windows reveals that the local standard deviation of each frequency band is correlated with the local standard deviation of the other frequency bands. The ratio between the standard deviation of adjacent frequency bands is 0.9 and remains constant with respect to time. This ratio defined as the variance coupling parameter is applicable to all of the frequency bands studied and appears to be related to the slope of the data's power spectrum. Similar analyses are performed on two cloud inhomogeneity models, which use fractal-based concepts to introduce inhomogeneity into a uniform cloud field. The bounded cascade model does this by iteratively redistributing LWP at each scale using the value of the local mean. This model is reformulated into a wavelet multiresolution framework, thereby presenting a number of variants of the bounded cascade model. One variant introduced in this paper is the 'variance coupled model,' which redistributes LWP using the local standard deviation and the variance coupling parameter. While the bounded cascade model provides an elegant two- parameter model for generating cloud inhomogeneity, the multiresolution framework provides more flexibility at the expense of model complexity. Comparisons are made with the results from the LWP data analysis to demonstrate both the strengths and weaknesses of these models.

Gollmer, Steven M.↗

Photoreduction of gaseous oxidized mercury changes global atmospheric mercury speciation, transport and deposition

Anthropogenic mercury (Hg(0)) emissions oxidize to gaseous Hg(II) compounds, before deposition to Earth surface ecosystems. Atmospheric reduction of Hg(II) competes with deposition, thereby modifying the magnitude and pattern of Hg deposition. Global Hg models have postulated that Hg(II) reduction in the atmosphere occurs through aqueous-phase photoreduction that may take place in clouds. Here we report that experimental rainfall Hg(II) photoreduction rates are much slower than modelled rates. We compute absorption cross sections of Hg(II) compounds and show that fast gas-phase Hg(II) photolysis can dominate atmospheric mercury reduction and lead to a substantial increase in the modelled, global atmospheric Hg lifetime by a factor two. Models with Hg(II) photolysis show enhanced Hg (0) deposition to land, which may prolong recovery of aquatic ecosystems long after Hg emissions are lowered, due to the longer residence time of Hg in soils compared with the ocean. Fast Hg(II) photolysis substantially changes atmospheric Hg dynamics and requires further assessment at regional and local scales.

54 ENVIRONMENTAL SCIENCES↗

Long chain carbon molecules and diffuse interstellar lines

An estimate of the abundances of chain hydrocarbon molecules expected in dense interstellar clouds as a result of gas-phase chemistry alone supports the hypothesis that the long chain molecules are responsible for the diffuse interstellar lines seen in the optical spectra of stars lying behind fairly low-density interstellar clouds. In particular, it is shown that the equilibrium abundances of the long chain carbon molecules may remain quite high even for molecules with as many as 11 carbon atoms.

Mitchell, G. F.↗

Cloud-property retrieval using merged HIRS and AVHRR data

A technique is developed that uses a multispectral, multiresolution method to improve the overall retrieval of mid- to high-level cloud properties by combining HIRS sounding channel data with higher spatial resolution AVHRR radiometric data collocated with the HIRS footprint. Cirrus cloud radiative and physical properties are determined using satellite data, surface-based measurements provided by rawinsondes and lidar, and aircraft-based lidar data collected during the First International Satellite Cloud Climatology Program Regional Experiment in Wisconsin during the months of October and November 1986. HIRS cloud-height retrievals are compared to ground-based lidar and aircraft lidar when possible. Retrieved cloud heights are found to have close agreement with lidar for thin cloud, but are higher than lidar for optically thick cloud. The results of the reflectance-emittance relationships derived are compared to theoretical scattering model results for both water-droplet spheres and randomly oriented hexagonal ice crystals. It is found that the assumption of 10-micron water droplets is inadequate to describe the reflectance-emittance relationship for the ice clouds seen here. Use of this assumption would lead to lower cloud heights using the ISCCP approach. The theoretical results show that use of hexagonal ice crystal phase functions could lead to much improved results for cloud retrieval algorithms using a bispectral approach.

Baum, Bryan A.↗

Two-phase models of quasar emission line regions

It is demonstrated that the emitting gas in clouds of quasar emission line regions must be confined by a hot intercloud medium, provided only that the heating mechanisms are strong enough to drive the low-density intercloud gas above a few tens of millions degrees K. The study of the thermal properties of the gas presented includes heating by photoionization, Compton scattering, suprathermal particles, absorption of radio frequency radiation, cloud friction, thermal conduction, and shocks. Cooling curves for photoionized gases are presented, and phase diagrams analogous to the pressure-temperature diagrams used in studying the interstellar medium are constructed for various conditions. It is shown that two-phase equilibria occur over a wide range of mean density, but over a much narrower range of pressure. The implications of these results for the emission line region are discussed, and it is shown that the emission clouds may be short-lived.

Krolik, J. H.↗

Spectrally-Invariant Approximation Within Atmospheric Radiative Transfer

Certain algebraic combinations of single scattering albedo and solar radiation reflected from, or transmitted through, vegetation canopies do not vary with wavelength. These "spectrally invariant relationships" are the consequence of wavelength independence of the extinction coefficient and scattering phase function in vegetation. In general, this wavelength independence does not hold in the atmosphere, but in cloud~dominated atmospheres the total extinction and total scattering phase function vary only weakly with wavelength. This paper identifies the atmospheric conditions under which the spectrally invariant approximation can accurately describe the extinction. and scattering properties of cloudy atmospheres. The validity of the assumptions and the accuracy of the approximation are tested with ID radiative transfer calculations using publicly available radiative transfer models: Discrete Ordinate Radiative Transfer (DISORT) and Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART). It is shown for cloudy atmospheres with cloud optical depth above 3, and for spectral intervals that exclude strong water vapor absorption, that the spectrally invariant relationships found in vegetation canopy radiative transfer are valid to better than 5%. The physics behind this phenomenon, its mathematical basis, and possible applications to remote sensing and climate are discussed.

Marshak, A.↗

Venus' spectroscopic phase variation - Implications of the Mariner 10 photographs

The recent ultraviolet photographs of Venus by Mariner 10 have shown an irregular cloud structure. There is an apparent tendency for clearing along a wide equatorial band more or less centered on the subsolar point. This synoptic picture is in marked contrast to the uniform cloud cover conventionally used in model calculations of the variation with phase of CO2 absorption bands. To illustrate the consequences of subsolar weakening of CO2 absorption, a mathematically simple (but realistically naive) model is used. Two conclusions are reached: (1) efforts to distinguish between single- and double-layer models for the clouds from spectroscopic data alone are not merely ambiguous (as argued earlier by Chamberlain and Smith); with present data they are hopeless; (2) the decrease in the CO2 absorption close to full phase, as reported by Young et al., could result entirely from an equatorial darkening that is relatively inconsequential at the crescent phase and increasingly predominant for fuller phases.

Chamberlain, J. W.↗

High-resolution spectra of Io's sodium emission

The shape of Io's sodium D2 emission profile varies markedly with Io's orbital phase, and its width suggests that the sodium cloud may be expanding with velocities up to 18 km/sec. This offers an explanation for at least part of the orbital phase asymmetry observed for the D-line emission.

Trafton, L.↗

Circumpolar hoods and clouds and their relation to the Martian H2O cycle

Water exists in both vapor and solid phases in the Martian atmosphere. The polar hoods are shrouds of condensate clouds which obscure both polar regions at times during their respective fall and winter seasons. The hemispheric asymmetries in the polar hood clouds are reviewed and their significance to the seasonal water cycle is discussed. Comparisons of images acquired using short wavelength filters, which provide maximum cloud contrast, and long wavelength filters, which are sensitive to surface features including the surface cap, provide correlations between cloud formation and large scale planetary dynamics.

James, Philip B.↗

Field Validation of Cloud Properties Sensor (SAIL Field Campaign Report)

The purpose of the Field Validation of Cloud Properties Sensor – SAIL campaign was to deploy Aerodyne’s extended-wavelength TWST cloud optical properties sensor (TWST-CPS) in an operationally relevant environment with co-located, externally validated sensors. Colocation with The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s deployment of its second Mobile Facility (AMF2) on the Surface Atmosphere Integrated Field Laboratory (SAIL) campaign at Crested Butte, Colorado was ideal because of the variety of operational sensors that can measure some of the same cloud properties using different modalities. While cloud property sensors have long existed, they tend to be costly to produce and maintain. Our sensor measures absolute spectral radiance over 440-1700 nm and retrieves cloud optical depth (COD), droplet effective radius (Reff), and thermodynamic phase (Phase). Our prototype is built predominantly from off-the-shelf components and uses uncooled spectrometers. A low-cost, easy-to-use sensor such as this could allow deployment at many more sites for greater spatial coverage. Instrument deployment to test robust operations and a new stray-light baffle design, and the continued development of analysis and retrieval algorithms using the data from this deployment, are central technical objectives of Aerodyne Research’s U.S. Department of Energy Small Business Innovative Research Phase 2 contract (DE-SC0020473, Low-cost shortwave spectroradiometer for retrieval of cloud properties).

54 ENVIRONMENTAL SCIENCES↗

Field Validation of Cloud Properties Sensor – SAIL Field Campaign Report

The purpose of the Field Validation of Cloud Properties Sensor – SAIL campaign was to deploy Aerodyne’s extended-wavelength TWST cloud optical properties sensor (TWST-CPS) in an operationally relevant environment with co-located, externally validated sensors. Colocation with The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s deployment of its second Mobile Facility (AMF2) on the Surface Atmosphere Integrated Field Laboratory (SAIL) campaign at Crested Butte, Colorado was ideal because of the variety of operational sensors that can measure some of the same cloud properties using different modalities. While cloud property sensors have long existed, they tend to be costly to produce and maintain. Our sensor measures absolute spectral radiance over 440-1700 nm and retrieves cloud optical depth (COD), droplet effective radius (Reff), and thermodynamic phase (Phase). Our prototype is built predominantly from off-the-shelf components and uses uncooled spectrometers. A low-cost, easy-to-use sensor such as this could allow deployment at many more sites for greater spatial coverage. Instrument deployment to test robust operations and a new stray-light baffle design, and the continued development of analysis and retrieval algorithms using the data from this deployment, are central technical objectives of Aerodyne Research’s U.S. Department of Energy Small Business Innovative Research Phase 2 contract (DE-SC0020473, Low-cost shortwave spectroradiometer for retrieval of cloud properties).

54 ENVIRONMENTAL SCIENCES↗

Simulating the Transport and Rupture of Pollen in the Atmosphere

Pollen, one type of primary biological aerosol particle (PBAP), is emitted from the terrestrial biosphere and can undergo physical changes in the atmosphere via particle rupture. To examine the fate of pollen and its atmospheric processing, a pollen emission and transport scheme is coupled to the Weather Research and Forecasting Model with Chemistry (WRF-Chem). We simulate the emission of pollen and its impacts on the cloud properties and precipitation in the Southern Great Plains from 12 to 19 April 2013, a period with both high pollen emissions and convective activity. We conduct a suite of ensemble runs that simulate primary pollen and three different pollen rupture mechanisms that generate subpollen particles, including (a) high humidity-induced surface rupture, (b) high humidity-induced in-atmosphere plus surface rupture, and (c) lightning-induced rupture, where in-cloud and cloud-to-ground lightning strikes trigger pollen rupture events. When relative humidity is high (>80%), coarse primary pollen (~1 μg m –3 ) is converted into fine subpollen particles (~1.2e –4 μg m –3 ), which produces 80% more subpollen particles than lightning-induced rupture. The in-atmosphere humidity-driven rupture predominantly produces subpollen particles, which is further enhanced during a frontal thunderstorm. During strong convection, vertical updrafts lift primary pollen and subpollen particles (~0.5e –4 μg m –3 ) to the upper troposphere (~12 km) and laterally transports the ruptured pollen in the anvil top outflow. In regions of high pollen and strong convection, ruptured pollen can influence warm cloud formation by decreasing low cloud (<4 km) cloud water mixing ratios and increasing ice phase hydrometeors aloft (>10 km)

54 ENVIRONMENTAL SCIENCES↗

Scattering in the atmosphere of Venus. III - Line profiles and phase curves for Rayleigh scattering

Spectral line profiles, curves of growth, and curves for the equivalent width of a line as a function of Venus phase angle have been computed for a Rayleigh scattering cloud and compared with those for a cloud of isotropic scatterers. The results are very similar for the two kinds of scattering, with the exception of the curves of equivalent width as a function of Venus phase angle. These latter curves exhibit the 'inverse phase effect' and rule out a scale height of the clouds much less than half the scale height of the gas. The optical depth of the clouds is approximately 100.

Young, L. D. G.↗

A Fourier approach to cloud motion estimation

A Fourier technique is described for estimating cloud motion from pairs of pictures using the phase of the cross spectral density. The method allows motion estimates to be made for individual spatial frequencies, which are related to cloud pattern dimensions. Results obtained are presented and compared with the results of a Fourier domain cross correlation scheme. Using both artificial and real cloud data show that the technique is relatively sensitive to the presence of mixtures of motions, changes in cloud shape, and edge effects.

Arking, A.↗