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At least 739 records · Page 41

Improving the Capabilities and Computational Efficiency of the RTE+RRTMGP Radiation Code (Final Report)

This report details progress on the RTE+RRTMGP radiation codes made during the period of performance. RTE+RRTMGP is a set of codes for computing radiative fluxes in planetary atmospheres. RRTMGP uses a k-distribution to provide an optical description (absorption and possibly Rayleigh optical depth) of the gaseous atmosphere, along with the relevant source functions, on a pre-determined spectral grid given temperatures, pressures, and gas concentration. RTE computes fluxes given spectrally-resolved optical descriptions and source functions. Spectrally-resolved fluxes are summarized (“reduced”) via a user extensible class. The initial release of the code and the design choices are described in Pincus et al. 2019; the codes are available on Github. Although RRTMGP was based on current (at the time) empirical spectroscopic data, RTE and RRTMGP were developed in large part to modernize software practices. The design focused on flexibility broadly interpreted: by separating code from data and allowing data to drive computation; in coupling to the host model (e.g. the coupling of clouds to radiative fluxes is user-controlled); with respect to programming languages (computational tasks are accessed via widely-compatible C interfaces); and with respect to hardware (the codes run on a range of CPU and GPU architectures). The code also puts an emphasis on modularity and clarity. RTE+RRTMGP v1.0 was released in September 20219. This award supported the evolution of the RTE+RRTMGP code base to support greater flexibility, accuracy, and efficiency.

54 ENVIRONMENTAL SCIENCES↗

Answering the Call for Model-Relevant Observations of Aerosols and Clouds

We describe a technique for combining multiple A-Train aerosol data sets, namely MODIS spectral AOD (aerosol optical depth), OMI AAOD (absorption aerosol optical depth) and CALIOP aerosol backscatter retrievals (hereafter referred to as MOC retrievals) to estimate full spectral sets of aerosol radiative properties, and ultimately to calculate the 3-D distribution of direct aerosol radiative effects (DARE). We present MOC results using almost two years of data collected in 2007 and 2008, and show comparisons of the aerosol radiative property estimates to collocated AERONET retrievals. We compare the spatio-temporal distribution of the MOC retrievals and MOC-based calculations of seasonal clear-sky DARE to values derived from four models that participated in the Phase II AeroCom model intercomparison initiative. Comparisons of seasonal aerosol property to AeroCom Phase II results show generally good agreement best agreement with forcing results at TOA is found with GMI-MerraV3.We discuss the challenges in making observations that really address deficiencies in models, with some of the more relevant aspects being representativeness of the observations for climatological states, and whether a given model-measurement difference addresses a sampling or a model error.

Redemann, J.↗

Using Observations of Deep Convective Systems to Constrain Atmospheric Column Absorption of Solar Radiation in the Optically Thick Limit

Atmospheric column absorption of solar radiation A(sub col) is a fundamental part of the Earth's energy cycle but is an extremely difficult quantity to measure directly. To investigate A(sub col), we have collocated satellite-surface observations for the optically thick Deep Convective Systems (DCS) at the Department of Energy Atmosphere Radiation Measurement (ARM) Tropical Western Pacific (TWP) and Southern Great Plains (SGP) sites during the period of March 2000 December 2004. The surface data were averaged over a 2-h interval centered at the time of the satellite overpass, and the satellite data were averaged within a 1 deg X 1 deg area centered on the ARM sites. In the DCS, cloud particle size is important for top-of-atmosphere (TOA) albedo and A(sub col) although the surface absorption is independent of cloud particle size. In this study, we find that the A(sub col) in the tropics is approximately 0.011 more than that in the middle latitudes. This difference, however, disappears, i.e., the A(sub col) values at both regions converge to the same value (approximately 0.27 of the total incoming solar radiation) in the optically thick limit (tau greater than 80). Comparing the observations with the NASA Langley modified Fu_Liou 2-stream radiative transfer model for optically thick cases, the difference between observed and model-calculated surface absorption, on average, is less than 0.01, but the model-calculated TOA albedo and A(sub col) differ by 0.01 to 0.04, depending primarily on the cloud particle size observation used. The model versus observation discrepancies found are smaller than many previous studies and are just within the estimated error bounds. We did not find evidence for a large cloud absorption anomaly for the optically thick limit of extensive ice cloud layers. A more modest cloud absorption difference of 0.01 to 0.04 cannot yet be ruled out. The remaining uncertainty could be reduced with additional cases, and by reducing the current uncertainty in cloud particle size.

Dong, Xiquan↗

Optical path switching based differential absorption radiometry for substance detection

An optical path switch divides sample path radiation into a time series of alternating first polarized components and second polarized components. The first polarized components are transmitted along a first optical path and the second polarized components along a second optical path. A first gasless optical filter train filters the first polarized components to isolate at least a first wavelength band thereby generating first filtered radiation. A second gasless optical filter train filters the second polarized components to isolate at least a second wavelength band thereby generating second filtered radiation. A beam combiner combines the first and second filtered radiation to form a combined beam of radiation. A detector is disposed to monitor magnitude of at least a portion of the combined beam alternately at the first wavelength band and the second wavelength band as an indication of the concentration of the substance in the sample path.

Sachse, Glen W.↗

Optical path switching based differential absorption radiometry for substance detection

An optical path switch divides sample path radiation into a time series of alternating first polarized components and second polarized components. The first polarized components are transmitted along a first optical path and the second polarized components along a second optical path. A first gasless optical filter train filters the first polarized components to isolate at least a first wavelength band thereby generating first filtered radiation. A second gasless optical filter train filters the second polarized components to isolate at least a second wavelength band thereby generating second filtered radiation. A beam combiner combines the first and second filtered radiation to form a combined beam of radiation. A detector is disposed to monitor magnitude of at least a portion of the combined beam alternately at the first wavelength band and the second wavelength band as an indication of the concentration of the substance in the sample path.

Sachse, Glen W.↗

High-resolution optical and ultraviolet absorption-line studies of interstellar gas

Recent progress in the characterization of the interstellar medium (ISM) by means of optical and UV spectral data is summarized. The gas is studied by focusing on background stars whose spectra can be accurately modeled to provide the light source for the absorption-line scans. The capabilities of earth- and space-based instruments which have been and are used for the surveys are delineated. The distributions of diffuse gas densities and characteristics of the cold, warm and hot gas in the Galaxy are described in terms of the elemental abundances, kinetics and distributions of the gas. Particular note is taken of gas in the solar neighborhood and around SNR, and of absorption-line data of cosmological significance.

Cowie, Lennox L.↗

A comparison of interstellar Na I, Ca II, and K I absorption

The strongest and generally most useful optical interstellar absorption lines include the D lines of Na I, the H and K lines of Ca II, and the resonance doublet at 7600 A and 7664 A of K I. The interferometric data for these strongest atomic lines are examined in a comprehensive manner. The numerical results pertaining to the total column densities are collected in a table, which lists 82 stars. The correlations among some of the quantities listed in the table are displayed in a number of graphs.

Hobbs, L. M.↗

A-Train Aerosol Observations Preliminary Comparisons with AeroCom Models and Pathways to Observationally Based All-Sky Estimates

We have developed a technique for combining CALIOP aerosol backscatter, MODIS spectral AOD (aerosol optical depth), and OMI AAOD (absorption aerosol optical depth) retrievals for the purpose of estimating full spectral sets of aerosol radiative properties, and ultimately for calculating the 3-D distribution of direct aerosol radiative forcing. We present results using one year of data collected in 2007 and show comparisons of the aerosol radiative property estimates to collocated AERONET retrievals. Use of the recently released MODIS Collection 6 data for aerosol optical depths derived with the dark target and deep blue algorithms has extended the coverage of the multi-sensor estimates towards higher latitudes. We compare the spatio-temporal distribution of our multi-sensor aerosol retrievals and calculations of seasonal clear-sky aerosol radiative forcing based on the aerosol retrievals to values derived from four models that participated in the latest AeroCom model intercomparison initiative. We find significant inter-model differences, in particular for the aerosol single scattering albedo, which can be evaluated using the multi-sensor A-Train retrievals. We discuss the major challenges that exist in extending our clear-sky results to all-sky conditions. On the basis of comparisons to suborbital measurements, we present some of the limitations of the MODIS and CALIOP retrievals in the presence of adjacent or underlying clouds. Strategies for meeting these challenges are discussed.

Aerosol↗

Direct Aerosol Radiative Forcing Based on Combined A-Train Observations: Towards All-sky Estimates and Attribution to Aerosol Type

We describe a technique for combining CALIOP aerosol backscatter, MODIS spectral AOD (aerosol optical depth), and OMI AAOD (absorption aerosol optical depth) measurements for the purpose of estimating full spectral sets of aerosol radiative properties, and ultimately for calculating the 3-D distribution of direct aerosol radiative forcing. We present results using one year of data collected in 2007 and show comparisons of the aerosol radiative property estimates to collocated AERONET retrievals. Initial calculations of seasonal clear-sky aerosol radiative forcing based on our multi-sensor aerosol retrievals compare well with over-ocean and top of the atmosphere IPCC-2007 model-based results, and with more recent assessments in the "Climate Change Science Program Report: Atmospheric Aerosol Properties and Climate Impacts" (2009). We discuss some of the challenges that exist in extending our clear-sky results to all-sky conditions. On the basis of comparisons to suborbital measurements, we present some of the limitations of the MODIS and CALIOP retrievals in the presence of adjacent or underlying clouds. Strategies for meeting these challenges are discussed. We also discuss a methodology for using the multi-sensor aerosol retrievals for aerosol type classification based on advanced clustering techniques. The combination of research results permits conclusions regarding the attribution of aerosol radiative forcing to aerosol type.

AOD↗

Fiber-optic thermometer using temperature dependent absorption, broadband detection, and time domain referencing

A fiber-optic thermometer based on temperature dependent absorption in Nd(3+) doped glass is demonstrated over the 298-573 K range. A broadband detection technique allows the use of the complete spectrum of a pulse modulated light emitting diode. A fiber-optic recirculating loop is employed to construct a reference channel in the time domain by generating a train of pulses from one initial pulse. A theoretical model is developed, and experimental data are shown to compare well with the theory. Possible sources of error and instability are identified, and ways to enhance the performance of the system are proposed.

Adamovsky, Grigory↗

Absolute photoluminescence intensity in thin film solar cells

A calculation is presented for the direct conversion of a measured luminescence signal to the implied open circuit voltage. The effects of re-absorption, spectral dependence, and interference with front and back interfaces are all included, so long as the optical properties of the structure are known. The method is validated through a comparison of the terminal open-circuit voltage with the photoluminescence intensity of Cu(In,Ga)Se 2 solar cells, each as a function of illumination intensity.

14 SOLAR ENERGY↗

Interstellar absorption toward HD 14633

Observations are reported of optical interstellar absorption lines of Ti II, Ca II, and Na I in the spectrum of HD 14633, a probable runaway O star ejected from the Perseus spiral arm. Unusually high gas-phase abundances of the normally depleted elements Ca and Ti are found in three high-velocity interstellar line components; the light paths to only a few other stars are known to show a comparably strong Routly-Spitzer effect. The greatly reduced heavy-element depletions in these parcels of gas presumably reflect the disruption of interstellar grains in gas which may be located in the lower galactic halo at an absolute value of 2 of about 1 kpc.

Hobbs, L. M.↗

The early ultraviolet spectral evolution of Nova Cygni 1992

We report on the high resolution ultraviolet line profile evolution of Nova Cygni 1992 using the International Ultraviolet Explorer (IUE) satellite and the Goddard High Resolution Spectrograph (GHRS) on the Hubble Space Telescope (HST). Our observations cover the period from discovery in 1992 February through 1993 April. The initial expansion velocity, derived from P Cyg profiles on Mg II and other resonance lines, was about 4500 km/s. All resonance transitions displayed P Cyg profiles around the time of UV maximum. We first discuss the spectral development as the initially optically thick atomic absorption curtain became optically thin. We then present the interpretation of the nebular spectral stage. The high resolution line profiles show that the shell rapidly developed nearly symmetric knots, or filaments, of emission. The optically thin transitions show an emission weighted expansion velocity of about 1800 km/s, consistent with the velocity inferred from the radio and infrared data. The emission lines display a symmetric set of filaments that appeared as soon as the line profiles became optically thin. The GHRS observations demonstrate that the filaments were located in the inner, slower moving parts of the ejecta. These probably record an initial low wave number instability imposed on the ejecta at the time of outburst. We suggest that the likely cause is a Rayleigh-Taylor instability. The emission at later stages is dominated by the filaments and, since this phenomenon is seen in virtually all novae, nebular line formation codes will have to account for the density inhomgeneities in order to adequately determine abundances for nove ejecta.

Shore, Steven N.↗

Exploiting Intersubband Plasmons in Vertically Aligned Carbon Nanotubes for Near-Infrared Electrochromic Windows

Optically transparent materials with switchable near-infrared (NIR) transmissivity are of significant interest for energy-saving smart window technologies. To this end, we demonstrate that semitransparent films of vertically aligned carbon nanotubes (CNTs) incorporated into electrochemically gated devices exhibit NIR transmittance changes up to 47% and bistable optical states that are appealing for low-power, large-area operation. The tunable NIR electrochromic response is driven by a doping-induced intersubband plasmon (ISBP) absorption, an optical feature in CNTs that is selective to light polarized perpendicular to the CNT axis. Vertically aligned CNT films (as opposed to more conventional planar CNT mats) thus allow us to isolate and study the ISBP resonance changes with applied voltage, electrode material, and film thickness.

absorption↗

Photodriven electron-transfer dynamics in a series of heteroleptic Cu(I)–anthraquinone dyads

Solar fuels catalysis is a promising route to efficiently harvesting, storing, and utilizing abundant solar energy. To achieve this promise, however, molecular systems must be designed with sustainable components that can balance numerous photophysical and chemical processes. To that end, here we report on the structural and photophysical characterization of a series of Cu(I)–anthraquinone-based electron donor–acceptor dyads. The dyads utilized a heteroleptic Cu(I) bis-diimine architecture with a copper(I) bis-phenanthroline chromophore donor and anthraquinone electron acceptor. We characterized the structures of the complexes using x-ray crystallography and density functional theory calculations and the photophysical properties via resonance Raman and optical transient absorption spectroscopy. The calculations and resonance Raman spectroscopy revealed that excitation of the Cu(I) metal-to-ligand charge-transfer (MLCT) transition transfers the electron to a delocalized ligand orbital. The optical transient absorption spectroscopy demonstrated that each dyad formed the oxidized copper–reduced anthraquinone charge-separated state. Unlike most Cu(I) bis-phenanthroline complexes where increasingly bulky substituents on the phenanthroline ligands lead to longer MLCT excited-state lifetimes, here, we observe a decrease in the long-lived charge-separated state lifetime with increasing steric bulk. The charge-separated state lifetimes were best explained in the context of electron-transfer theory rather than with the energy gap law, which is typical for MLCT excited states, despite the complete conjugation between the phenanthroline and anthraquinone moieties.

14 SOLAR ENERGY↗

Mechanisms of the Cu(I)-Catalyzed Intermolecular Photocycloaddition Reaction Revealed by Optical and X-ray Transient Absorption Spectroscopies

The [2 + 2] photocycloaddition provides a simple, single-step route to cyclobutane moieties that would otherwise be disfavored or impossible due to ring strain and/or steric interactions. We have used a combination of optical and X-ray transient absorption spectroscopies to elucidate the mechanism of the Cu(I)-catalyzed intermolecular photocycloaddition reaction using norbornene and cyclohexene as model substrates. We find that for norbornene the reaction proceeds through an initial metal-to-ligand charge transfer (MLCT) state that persists for 18 ns before the metal returns to the monovalent oxidation state. The Cu K-edge spectrum continues to evolve until ~5 μs and then remains unchanged for the 50 μs duration of the measurement, reflecting product formation and ligand dissociation. We hypothesize that the MLCT transition and reverse electron transfer serve to sensitize the triplet excited state of one of the norbornene ligands, which then dimerizes with the other to give the product. For the case of cyclohexene, however, we do not observe a charge transfer state following photoexcitation and instead find evidence for an increase in the metal–ligand bond strength that persists for several ns before product formation occurs. This is consistent with a mechanism in which ligand photoisomerization is the initial step, which was first proposed by Salomon and Kochi in 1974 to explain the stereoselectivity of the reaction. Furthermore, our investigation reveals how this photocatalytic reaction may be directed along strikingly disparate trajectories by only very minor changes to the structure of the substrate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Connecting Femtosecond Transient Absorption Microscopy with Spatially Coregistered Time Averaged Optical Imaging Modalities

Multimodal all-optical imaging involving coregistered femtosecond transient absorption microscopy (TAM), time-integrated photoluminescence (PL), and steady-state modalities such as confocal reflectance and transmission offers an appealing approach to gain a comprehensive understanding of complex electronic excited-state phenomena in spatially heterogeneous systems. A unique combination of these modalities allows us to unravel not only the competing electronic excited-state dynamical processes but also the underlying morphological information with simultaneous high temporal and spatial resolution. However, correlating the various images obtained from time-resolved and time-independent modalities is generally nontrivial and particularly challenging when the electronic dynamics under study evolve in both time and space. Here, we demonstrate a new approach for rationally correlating time-resolved microscopy with coregistered time-integrated or steady-state modalities. Specifically, our approach involves an extended global lifetime analysis of the time-resolved microscopic data set to separate distinct dynamical processes taking place on commensurate time scales, and the resulting decay-associated amplitude maps (DAAMs) were applied to explore correlations with the images acquired using time-independent modalities. The feasibility of our approach was validated through analyzing a multimodal data set acquired from a thin film of chloride-containing mixed lead halide perovskites (CH 3 NH 3 PbI 3–x Cl x ) using femtosecond transient absorption, time-integrated PL, and confocal reflectance microscopies. Analysis of the results obtained enable us to gain new insight into the complex ultrafast relaxation dynamics in this highly heterogeneous system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗