Optical properties of transition ions in crystals under bombardment by energetic particles, x and gamma rays and light final report
Effects of radiationless processes on radiating states of excited crystals containing rare earth ions
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Effects of radiationless processes on radiating states of excited crystals containing rare earth ions
Degradation of Earth’s inland water resources due to anthropogenic perturbations and climate anomalies at both local and global scales continues to place human health at substantial risk. There is now a growing necessity to develop pragmatic approaches that allow timely and effective extrapolation of local processes, to spatially resolved global products, and to promote operational and sustainable resource policy management. This presentation will be discussing the progress made developing SWIPE: Spectral Water Inversion Processor and Emulator. SWIPE is a platform for advanced modeling of coastal and inland aquatic habitats. The goal is create a comprehensive and cohesive system to leverage recent advancements in computation and machine learning to develop a synthetic training ground for sensitivity studies and algorithm development. The four principal facets of SWIPE include: 1. Advanced two-layer coated sphere bio-optical modeling and GPU radiative transfer modeling, 2. Big Data involving massive synthetic spectral libraries of optical properties of various global aquatic particles, surface reflectance, and top-of-atmosphere reflectance, all at hyperspectral resolution leveraging high-end computing systems at NASA Ames Research Center, 3. Deep Learning for algorithm development for water quality inversion of concentrations of common biogeophysical variables as well as optics, full uncertainty characterization by water type, and forward emulation, and lastly, 4. Image Processing for application of developed retrieval algorithms for both hyperspectral and multispectral sensors with experimental corrections for global adjacency, noise, sunglint, and benthic reflectance. This presentation will demonstrate the Equivalent Algal Populations (EAP) two-layer coated sphere scattering model which has been used develop spectral libraries of hyperspectral inherent optical properties of roughly 80 species of phytoplankton, covering 15 different classes and nine taxonomic functional types. The EAP model was also used to derive spectral properties of 10 different non-algal particle functional types. Examples of how the SMART-G (Speed-up Monte-carlo Advanced Radiative Transfer using GPU) radiative transfer code is used to model optically complex aquatic signals will be presented and discussed in the context of creating a massive synthetic database which can leverage the full power of next generation machine learning techniques and high end computing for water quality inversion. We will discuss our active investigation in things like appropriate model architectures, dimensionality reduction techniques such as PCA and autoencoders, uncertainty quantification and abstaining, and which variables actually benefit most from hyperspectral information versus multispectral resolution. We are also curious about questions relating to cost/benefit analysis in terms of computation resources, neural network complexity, and data volumes. Answers to these questions will hopefully elaborate on cost efficiency for potential future sensor design considerations.
Shapes of ice crystals can significantly affect the radiative transfer in ice clouds. The angular distribution of the polarized reflectance over ice clouds strongly depends on ice crystal shapes. Although the angular-distribution features of the total or polarized reflectance over ice clouds implies a possibility of retrieving ice cloud particle shapes by use of remote sensing data, the accuracy of the retrieval must be evaluated. In this study, a technique, which applies single ice crystal habit and multidirectional polarized radiance to retrieve ice cloud particle shapes, is assessed. Our sensitivity studies show that the retrieved particle shapes &om this algorithm can be considered good approximations to those in actual clouds in calculation of the phase matrix elements. Although a fractal poly-crystal shape or an inhomogeneous hexagonal column may also produce this type of phase functions, more representative single-scattering properties from combinations of natural particle shapes and size distributions may still be necessary in accurate retrieval of other cloud properties such as optical thickness and particle size.
The effect of thin cirrus clouds in retrieving the dust optical depth from MODIS observations is investigated by using a simplified aerosol retrieval algorithm based on the principles of the Deep Blue aerosol property retrieval method. Specifically, the errors of the retrieved dust optical depth due to thin cirrus contamination are quantified through the comparison of two retrievals by assuming dust-only atmospheres and the counterparts with overlapping mineral dust and thin cirrus clouds. To account for the effect of the polarization state of radiation field on radiance simulation, a vector radiative transfer model is used to generate the lookup tables. In the forward radiative transfer simulations involved in generating the lookup tables, the Rayleigh scattering by atmospheric gaseous molecules and the reflection of the surface assumed to be Lambertian are fully taken into account. Additionally, the spheroid model is utilized to account for the nonsphericity of dust particles In computing their optical properties. For simplicity, the single-scattering albedo, scattering phase matrix, and optical depth are specified a priori for thin cirrus clouds assumed to consist of droxtal ice crystals. The present results indicate that the errors in the retrieved dust optical depths due to the contamination of thin cirrus clouds depend on the scattering angle, underlying surface reflectance, and dust optical depth. Under heavy dusty conditions, the absolute errors are comparable to the predescribed optical depths of thin cirrus clouds.
During the initial period of the work we concentrated on Saharan dust storms and published a sequence of papers (Colarco et a1 2002,2003a,b, Toon, 2004). The U.S. Air Force liked the dust model so well that they appropriated it for operational dust storm forecasting (Barnum et al., 2004). The Air Force has used it for about 5 yrs in the Middle East where dust storms cause significant operational problems. The student working on this project, Peter Colarco, has graduated and is now a civil servant at Goddard where he continues to interact with the TOMS team. This work helped constrain the optical properties of dust at TOMS wavelengths, which is useful for climate simulations and for TOMS retrievals of dust properties such as optical depth. We also used TOMS data to constrain the sources of dust in Africa and the Middle East, to determine the actual paths taken by Saharan dust storms, to learn more about the mechanics of variations in the optical depths, and to learn more about the mechanisms controlling the altitudes of the dust. During the last two years we have been working on smoke from fires. Black carbon aerosols are one of the leading factors in radiative forcing. The US Climate Change Science Program calls this area out for specific study. It has been suggested by Jim Hansen, and Mark Jacobsen among others, that by controlling emissions of black carbon we might reduce greenhouse radiative forcing in a relatively painless manner. However, we need a greatly improved understanding of the amount of black carbon in the atmosphere, where it is located, where it comes from, how it is mixed with other particles, what its actual optical properties are, and how it evolves. In order to learn about these issues we are using a numerical model of smoke. We have applied this model to the SAFARI field program data, and used the TOMS satellite observations in that period (Sept. 2000). Our goal is to constrain source function estimates for black carbon, and smoke optical properties.
The infrared absorption spectrum of solid ammonia is obtained from 2 to 125 microns as a composite of the published measurements. From this, the absorption coefficient and the complex refractive index are calculated as a function of frequency by integration of the Kramers-Kroenig dispersion relations. These data are used in a Mie theory analysis to obtain the basic parameters for scattering of long wavelength radiation by solid ammonia particles; this is believed to be an important process in radiative transfer within the atmospheres of the giant planets.
The optical properties of suspended dust particles from the eruption of Mt. St. Helens on July 23, 1980 are investigated using photoelectric observations of standard stars obtained on the 0.76-m telescope at the University of Washington 48 hours after the eruption. Measurements were made with five broad-band filters centered at 3910, 5085, 5480, 6330, and 8050 A on stars of varying color and over a wide range of air masses. Anomalous extinction effects due to the volcanic ash were detected, and a significant change in the wavelength-dependent extinction parameter during the course of the observations was established by statistical analysis. Mean particle size (a) and column density (N) are estimated using the Mie theory, assuming a log-normal particle-size distribution: a = 0.18 micron throughout; N = 1.02 x 10 to the 9th/sq cm before 7:00 UT and 2.33 x 10 to the 9th/sq cm after 8:30 UT on July 25, 1980. The extinction is attributed to low-level, slowly migrating ash, possibly combined with products of gas-to-particle conversion and coagulation.
The Smoke, Clouds, and Radiation-Brazil (SCAR-B) field project took place in the Brazilian Amazon and cerrado regions in August-September 1995 as a collaboration between Brazilian and American scientists. SCAR-B, a comprehensive experiment to study biomass burning, emphasized measurements of surface biomass, fires, smoke aerosol and trace gases, clouds, and radiation. their climatic effects, and remote sensing from aircraft and satellites. It included aircraft and ground-based in situ measurements of smoke emission factors and the compositions, sizes, and optical properties of the smoke particles; studies of the formation of ozone; the transport and evolution of smoke; and smoke interactions with water vapor and clouds. This overview paper introduces SCAR-B and summarizes some of the main results obtained so far. (1) Fires: measurements of the size distribution of fires, using the 50 m resolution MODIS Airborne Simulator, show that most of the fires are small (e.g. 0.005 square km), but the satellite sensors (e.g., AVHRR and MODIS with I km resolution) can detect fires in Brazil which are responsible for 60-85% of the burned biomass: (2) Aerosol: smoke particles emitted from fires increase their radius by as much as 60%, during their first three days in the atmosphere due to condensation and coagulation, reaching a mass median radius of 0.13-0.17 microns: (3) Radiative forcing: estimates of the globally averaged direct radiative forcing due to smoke worldwide, based on the properties of smoke measured in SCAR-B (-O.l to -0.3 W m(exp -2)), are smaller than previously modeled due to a lower single-scattering albedo (0.8 to 0.9), smaller scattering efficiency (3 square meters g(exp -2) at 550 nm), and low humidification factor; and (4) Effect on clouds: a good relationship was found between cloud condensation nuclei and smoke volume concentrations, thus an increase in the smoke emission is expected to affect cloud properties. In SCAR-B, new techniques were developed for deriving the absorption and refractive index of smoke from ground-based remote sensing. Future spaceborne radiometers (e.g., MODIS on the Earth Observing System), simulated on aircraft, proved to be very useful for monitoring smoke properties, surface properties, and the impacts of smoke on radiation and climate.
Though the emphasis of the Southern Africa Regional Science Initiative 2000 (SAFARI-2000) dry season campaign was largely on emission sources and transport, the assemblage of aircraft (including the high altitude NASA ER-2 remote sensing platform and the University of Washington CV-580, UK MRF C130, and South African Weather Bureau JRA in situ aircrafts) provided a unique opportunity for cloud studies. Therefore, as part of the SAFARI initiative, investigations were undertaken to assess regional aerosol-cloud interactions and cloud remote sensing algorithms. In particular, the latter part of the experiment concentrated on marine boundary layer stratocumulus clouds off the southwest coast of Africa. Associated with cold water upwelling along the Benguela current, the Namibian stratocumulus regime has received limited attention but appears to be unique for several reasons. During the dry season, outflow of continental fires and industrial pollution over this area can be extreme. From below, upwelling provides a rich nutrient source for phytoplankton (a source of atmospheric sulphur through DMS production as well as from decay processes). The impact of these natural and anthropogenic sources on the microphysical and optical properties of the stratocumulus is unknown. Continental and Indian Ocean cloud systems of opportunity were also studied during the campaign. Aircraft flights were coordinated with NASA Terra Satellite overpasses for synergy with the Moderate Resolution Imaging Spectroradiometer (MODIS) and other Terra instruments. An operational MODIS algorithm for the retrieval of cloud optical and physical properties (including optical thickness, effective particle radius, and water path) has been developed. Pixel-level MODIS retrievals (11 km spatial resolution at nadir) and gridded statistics of clouds in th SAFARI region will be presented. In addition, the MODIS Airborne Simulator flown on the ER-2 provided high spatial resolution retrievals (50 m at nadir). These retrievals will be discussed and compared with in situ observations.
The CERES Surface and Atmosphere Radiation Budget (SARB) product (Charlock et al, 2002) includes the vertical profile of broadband SW, broadband LW, and 8-12 micron window (WN) fluxes; upwelling and downwelling at TOA, 70 hPa, 200 hPa, 500 hPa, and the surface; and for all-sky and clear-sky conditions. We test the archived CERES TRMM record of SARB for January-August 1998 and focus on discrepancies with ground-based measurements at SGP. The CERES SARB is generated by a highly modified Fu-Liou radiative transfer code (Fu and Liou, 1993). The most critical inputs for this application are cloud optical properties (fractional area, optical depth, particle size and phase, height of top, and estimate of geometrical thickness Minnis et al., 2002) from the narrowband VIRS imager. Numerous VIRS pixels (approx. 2km resolution at nadir) are matched to each of the large (approx. 20km) CERES broadband footprints (Wielicki et al, 1996). Other inputs include temperature and humidity from ECMWF (Rabier et al, 1998) , NCEP ozone profiles from SBUV and TOVS (Yang et al, 2001), aerosol optical thickness (AOT) from the Model for Atmospheric Transport and Chemistry (MATCH) aerosol assimilation (Collins et al., 2001) or alternately from the VIRS imager (Ignatov and Stowe, 2000). VIRS AOT is available for clear and partly cloudy ocean footprints during daylight; and only when viewing geometry renders a contribution from sunglint as unlikely. For other footprints, AOT is taken from MATCH. AOT is apportioned into fractions of dust (Tegan and Lacis, 1996), sea salt, sulfate, dust, soluble organic, insoluble organic, and soot (Hess et al., 1996) using the 6-hourly MATCH output. Tuned fluxes are retrieved by adjusting inputs to nudge computed TOA fluxes toward CERES observations (Rose et al, 1997). In clear conditions, the fields of humidity, surface skin temperature, surface albedo and AOT are adjusted to produce a closer match of computed and observed fluxes at TOA. When CERES footprints have clouds, the cloud optical thickness, fractional area within the footprint, and temperature of cloud top are adjusted by the tuning algorithm. Both tuned and untuned fluxes are archived, as are the respective adjustments to any parameters at the surface or within the atmosphere.
The Cassini Ion and Neutral Mass Spectrometer (Waite, Jr., et al., 2007) and the Composite Infrared Spectrometer (Coustenis, A., et al., 2007) have detected benzene in the upper atmosphere and stratosphere of Titan. Photochemical reactions involving benzene in Titan's atmosphere may influence polycyclic aromatic hydrocarbon formation, aerosol formation, and the radiative balance of Titan's atmosphere. We measure the effect of benzene on the optical properties of Titan analog particles in the laboratory. Using cavity ring-down aerosol extinction spectroscopy, we determine the real and imaginary refractive index at 532 nm of particles formed by benzene photolysis and Titan analog particles formed with ppm-levels of benzene. These studies are compared to the previous study by Hasenkopf, et a1. (2010) of Titan analog particles formed by methane photolysis.
A new dust detection algorithm is developed by combining the results of multiple dust detectionmethods using IR channels onboard the MODerate resolution Imaging Spectroradiometer (MODIS). Brightness Temperature Difference (BTD) between two wavelength channels has been used widely in previous dust detection methods. However, BTDmethods have limitations in identifying the offset values of the BTDto discriminate clear-sky areas. The current algorithm overcomes the disadvantages of previous dust detection methods by considering the Brightness Temperature Ratio (BTR) values of the dual wavelength channels with 30-day composite, the optical properties of the dust particles, the variability of surface properties, and the cloud contamination. Therefore, the current algorithm shows improvements in detecting the dust loaded region over land during daytime. Finally, the confidence index of the current dust algorithm is shown in 10 × 10 pixels of the MODIS observations. From January to June, 2006, the results of the current algorithm are within 64 to 81% of those found using the fine mode fraction (FMF) and aerosol index (AI) from the MODIS and Ozone Monitoring Instrument (OMI). The agreement between the results of the current algorithm and the OMI AI over the non-polluted land also ranges from 60 to 67% to avoid errors due to the anthropogenic aerosol. In addition, the developed algorithm shows statistically significant results at four AErosol RObotic NETwork (AERONET) sites in East Asia.
Aerosol forcing uncertainty represents the largest climate forcing uncertainty overall. Its magnitude has remained virtually undiminished over the past 20 years despite considerable advances in understanding most of the key contributing elements. Recent work has produced modest increases only in the confidence of the uncertainty estimate itself. This review summarizes the contributions toward reducing the uncertainty in the aerosol forcing of climate made by satellite observations, measurements taken within the atmosphere, as well as modeling and data assimilation. We adopt a more measurement-oriented perspective than most reviews of the subject in assessing the strengths and limitations of each; gaps and possible ways to fill them are considered. Currently planned programs supporting advanced, global-scale satellite and surface-based aerosol, cloud, and precursor gas observations, climate modeling, and intensive field campaigns aimed at characterizing the underlying physical and chemical processes involved, are all essential. But in addition, new efforts are needed: (a) to obtain systematic aircraft in situ measurements capturing the multi-variate probability distribution functions of particle optical, microphysical, and chemical properties (and associated uncertainty estimates), as well as co-variability with meteorology, for the major aerosol airmass types; (b) to conceive, develop, and implement a suborbital (aircraft plus surface-based) program aimed at systematically quantifying the cloud-scale microphysics, cloud optical properties, and cloud-related vertical velocities associated with aerosol-cloud interactions; and (c) to focus much more research on integrating the unique contributions of satellite observations, suborbital measurements, and modeling, to reduce the persistent uncertainty in aerosol climate forcing.
Photons at wavelengths between 0.3 and 4.5 microns penetrate the atmospheres of Uranus and Neptune to pressures between about 0.01 bar and 10 bars. This pressure range brackets the radiative convective boundary in both atmospheres and is therefore designated upper troposphere. Physical processes which govern the transfer of radiation in Uranus's and Neptune's atmospheres at these wavelengths include Rayleigh/Raman scattering by hydrogen, scattering and broadband absorption by suspended aerosol particles and absorption in discrete bands and lines by methane and hydrogen. Consequently, tropospheric properties constrained by observations at these wavelengths include optical properties and distribution of aerosol particles, methane/hydrogen ratio, and ortho/para hydrogen ratio. Recent observations of Uranus and Neptune in this spectral range, are reviewed and compared with predictions based on models of the atmospheric structures. Significant results for Uranus include the presence of an opaque lower boundary to the visible atmosphere very near the level corresponding to 2 bars pressure, and consequently a methane/hydrogen ratio no less than 3 percent.
The treatment of biomass burning (BB) carbonaceous particles in the Multiangle Imaging SpectroRadiometer (MISR) Standard Aerosol Retrieval Algorithm is assessed, and algorithm refinements are suggested, based on a theoretical sensitivity analysis and comparisons with near-coincident AERONET measurements at representative BB sites. Over the natural ranges of BB aerosol microphysical and optical properties observed in past field campaigns, patterns of retrieved Aerosol Optical Depth (AOD), particle size, and single scattering albedo (SSA) are evaluated. On the basis of the theoretical analysis, assuming total column AOD of 0.2, over a dark, uniform surface, MISR can distinguish two to three groups in each of size and SSA, except when the assumed atmospheric particles are significantly absorbing (mid-visible SSA approx.0.84), or of medium sizes (mean radius approx.0.13 pin); sensitivity to absorbing, medium-large size particles increases considerably when the assumed column AOD is raised to 0.5. MISR Research Aerosol Retrievals confirm the theoretical results, based on coincident AERONET inversions under BB-dominated conditions. When BB is externally mixed with dust in the atmosphere, dust optical model and surface reflection uncertainties, along with spatial variability, contribute to differences between the Research Retrievals and AERONET. These results suggest specific refinements to the MISR Standard Aerosol Algorithm complement of component particles and mixtures. They also highlight the importance for satellite aerosol retrievals of surface reflectance characterization, with accuracies that can be difficult to achieve with coupled surface-aerosol algorithms in some higher AOD situations.
The theoretical basis is explored for inferring the microphysical properties of ice crystal from high-spectral resolution infrared observations. A radiative transfer model is employed to simulate spectral radiances to address relevant issues. The extinction and absorption efficiencies of individual ice crystals, assumed as hexagonal columns for large particles and droxtals for small particles, are computed from a combination of the finite- difference time-domain (FDTD) technique and a composite method. The corresponding phase functions are computed from a combination of FDTD and an improved geometric optics method (IGOM). Bulk scattering properties are derived by averaging the single- scattering properties of individual particles for 30 particle size distributions developed from in situ measurements and for additional four analytical Gamma size distributions for small particles. The non-sphericity of ice crystals is shown to have a significant impact on the radiative signatures in the infrared (IR) spectrum; the spherical particle approximation for inferring ice cloud properties may result in an overest&ation of the optical thickness and an inaccurate retrieval of effective particle size. Furthermore, we show that the error associated with the use of the Henyey-Greenstein phase function can be as larger as 1 K in terms of brightness temperature for larger particle effective size at some strong scattering wavenumbers. For small particles, the difference between the two phase functions is much less, with brightness temperatures generally differing by less than 0.4 K. The simulations undertaken in this study show that the slope of the IR brightness temperature spectrum between 790-960/cm is sensitive to the effective particle size. Furthermore, a strong sensitivity of IR brightness temperature to cloud optical thickness is noted within the l050-1250/cm region. Based on this spectral feature, a technique is presented for the simultaneous retrieval of the visible optical thickness and effective particle size from high spectral resolution infrared data under ice cloudy con&tion. The error analysis shows that the uncertainty of the retrieved optical thickness and effective particle size has a small range of variation. The error for retrieving particle size in conjunction with an uncertainty of 5 K in cloud'temperature, or a surface temperature uncertainty of 2.5 K, is less than 15%. The corresponding e m r in the uncertainty of optical thickness is within 5-2096, depending on the value of cloud optical thickness. The applicability of the technique is demonstrated using the aircraft-based High- resolution Interferometer Sounder (HIS) data from the Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) in 1996 and the First ISCCP Regional Experiment - Arctic Clouds Experiment (FIRE-ACE) in 1998.
New over-ocean aerosol models are developed by integrating the inversion data from the Aerosol Robotic Network (AERONET) sun/sky radiometers with a database for the optical properties of tri-axial ellipsoid particles. The new aerosol models allow more accurate retrieval of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) in the case of high AOD (AOD greater than 0.3). The aerosol models are categorized by using the fine-mode fraction (FMF) at 550 nm and the singlescattering albedo (SSA) at 440 nm from the AERONET inversion data to include a variety of aerosol types found around the globe. For each aerosol model, the changes in the aerosol optical properties (AOPs) as functions of AOD are considered to better represent aerosol characteristics. Comparisons of AODs between AERONET and MODIS for the period from 2003 to 2010 show that the use of the new aerosol models enhances the AOD accuracy with a Pearson coefficient of 0.93 and a regression slope of 0.99 compared to 0.92 and 0.85 calculated using the MODIS Collection 5 data. Moreover, the percentage of data within an expected error of +/-(0.03 + 0.05xAOD) is increased from 62 percent to 64 percent for overall data and from 39 percent to 51 percent for AOD greater than 0.3. Errors in the retrieved AOD are further characterized with respect to the Angstrom exponent (AE), scattering angle, SSA, and air mass factor (AMF). Due to more realistic AOPs assumptions, the new algorithm generally reduces systematic errors in the retrieved AODs compared with the current operational algorithm. In particular, the underestimation of fine-dominated AOD and the scattering angle dependence of dust-dominated AOD are significantly mitigated as results of the new algorithm's improved treatment of aerosol size distribution and dust particle nonsphericity.
The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) measured a variety of aerosol radiative effects (including flux changes) while simultaneously measuring the chemical, physical, and optical properties of the responsible aerosol particles. Here we use TARFOX-determined aerosol and surface properties to compute shortwave radiative flux changes for a variety of aerosol situations, with midvisible optical depths ranging from 0.06 to 0.55. We calculate flux changes by several techniques with varying degrees of sophistication, in part to investigate the sensitivity of results to computational approach. We then compare computed flux changes to those determined from aircraft measurements. Calculations using several approaches yield downward and upward flux changes that agree with measurements. The agreement demonstrates closure (i.e. consistency) among the TARFOX-derived aerosol properties, modeling techniques, and radiative flux measurements. Agreement between calculated and measured downward flux changes is best when the aerosols are modeled as moderately absorbing (midvisible single-scattering albedos between about 0.89 and 0.93), in accord with independent measurements of the TARPOX aerosol. The calculated values for instantaneous daytime upwelling flux changes are in the range +14 to +48 W/sq m for midvisible optical depths between 0.2 and 0.55. These values are about 30 to 100 times the global-average direct forcing expected for the global-average sulfate aerosol optical depth of 0.04. The reasons for the larger flux changes in TARFOX include the relatively large optical depths and the focus on cloud-free, daytime conditions over the dark ocean surface. These are the conditions that produce major aerosol radiative forcing events and contribute to any global-average climate effect.