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At least 109 records · Page 6

Plasmonic Ag nanocomposite phosphate glasses produced via γ-ray irradiation as reduction route

This paper reports on the impact of γ-ray irradiation (10, 100 kGy) on melt-quenched Ag + -doped phosphate glass and the effects of subsequent thermal processing leading to the production of plasmonic Ag nanocomposites. The γ-irradiated glasses were characterized alongside the pristine by differential scanning calorimetry (DSC), Raman spectroscopy, electron paramagnetic resonance (EPR) spectroscopy, optical absorption, and photoluminescence (PL) spectroscopy. DSC characterization showed consistent glass transition temperatures (T g ) before and after γ-irradiation whereas the crystallization temperatures tended to decrease with increasing γ-ray dose. However, a lack of alteration of the glass network structure was supported by Raman spectroscopy. Room temperature EPR spectra clearly showed the formation of phosphorus oxygen hole center (POHC) defects in the undoped host, in addition to another doublet likely associated with a P 3 defect. The presence of paramagnetic silver species encompassing Ag 2+ and 107/109 Ag 0 atoms was also indicated in the silver-activated glass together with POHC defects. Optical absorption spectra were also consistent with the presence of various radiation-induced centers. Further analyzing the glass absorption edge via Tauc plots suggested the formation of electron center (EC) defects in γ-irradiated samples wherein the silver-doped glass exhibited decreasing band gap energies with increasing γ-ray dose. The PL characterization showed the silver-related radio-PL effect was induced exhibiting broad band emission with two maxima around 500 and 625 nm stemming from various molecular Ag$^{x+}_{n}$ clusters. Emission decay analyses revealed that the longer wavelength emission exhibited slower decay. The highest radiation dose of 100 kGy however resulted in weaker emission and faster decay kinetics attributed to energy transfer between the luminescent silver species and POHC defects. Finally subjecting the γ-irradiated Ag-doped glasses to heat treatment near the T g at 490 °C led to the development of the surface plasmon resonance of Ag nanoparticles (NPs) and the vanishing of the Ag$^{x+}_{n}$ clusters luminescence. In conclusion, the presence of the matrix-related EC defects was deemed accountable for the thermally induced reduction and consequent precipitation of Ag NPs making the plasmonic glasses attractive for photonic applications such as nonlinear optics.

36 MATERIALS SCIENCE

Topography of the Flattest Surface on Earth: using ICESAT, GPS, and MISR to Measure Salt Surface Topography on Salar de Uyuni, Bolivia

Salt flats are aptly named: they are composed largely of salt, and are maintained as nearly equipotential surfaces via frequent flooding. The salar de Uyuni, on the Altiplano in southwestern Bolivia, is the largest salt flat on Earth, with an area of 9,800 sq km. Except for a few bedrock islands, it has less than 40 cm of relief. The upper-most salt unit averages 5 m thick and contains 50 cu km of nearly pure halite. It includes most of the salt that was in solution in paleolake Minchin, which attained a maximum area of 60,000 sq km and a maximum depth of 150 m, roughly 15 kyr ago. Despite approx. 10 m of differential isostatic rebound since deposition, the salar surface has been actively maintained as an extraordinarily flat and smooth surface by annual flooding during the rainy season. We have used the strong optical absorption properties of water in the visible band to map spatial variations in water depth during a time when the salar was flooded. As water depth increases, the initially pure white surface appears both darker and bluer. We utilized MISR images taken during the interval from April to November 2001. The red and infra-red bands (672 and 867 nm wavelength) were most useful since the water depth is small and the absorption at those wavelengths is quite strong. Nadir pointed MISR images have 275 m spatial resolution. To aid in our evaluation of water depth variations over the saiar surface, we utilized two sources of direct topographic measurements: several ICESAT altimetry tracks cross the area, and a 40x50 km GPS grid was surveyed to calibrate ICESAT. A difficulty in using these data types is that both give salt surface elevations relative to the ellipsoid, whereas the water surface will, in the absence of wind or tidal disturbances, follow an equipotential surface. Geoid height is not known to the required accuracy of a few cm in the central Andes. As a result, before comparing optical absorption from MISR to salt surface topography from GPS or ICESAT, we removed the longest wavelengths from both.

Comstock, Robert L.

Combining Organic Cations of Different Sizes Grants Improved Control over Perovskitoid Dimensionality and Bandgap

Because mixed-halide wide-bandgap (1.6-2.0 eV) perovskite solar cells suffer from operating instability related to light-induced halide segregation, it is of interest to study alternative means of bandgap widening. Perovskitoids combine wide bandgaps and structural stability resulting from face- or edge-sharing octahedral connections in their crystal structures. Unfortunately, there existed no prior reports of three-dimensional (3D) perovskitoids having direct bandgaps with optical absorption edges less than 2.2 eV. As the most significant predictor of perovskitoid bandgaps is the fraction of corner-sharing in their crystal structures, we hypothesized that increasing the amount of corner-sharing would access lower bandgaps than previously reported. Here, we accomplished this by mixing a spacer cation within the size range for 3D perovskitoid formation with a smaller perovskite-forming cation. We explored three spacer cations of different sizes: ethylammonium (EA), cyclopropylammonium (c-C3A), and cyclobutylammonium (c-C4A), combining these with methylammonium (MA), and found that the middle cation, c-C3A, pairs with MA to form a 3D perovskitoid with the formula (c-C3A) 3 (MA) 3 Pb 5 I 16 and a direct bandgap with an optical absorption edge at 2.0 eV. Solution-processed films of this perovskitoid showed improved light stability over mixed-halide perovskites, and solar cells based on these films exhibit increased maximum power point operating stability compared to reference mixed-halide devices.

Gilley, Isaiah W. [Northwestern University, Evanst

Ozone and Aerosol Retrieval from Backscattered Ultraviolet Radiation

In this presentation we will discuss the techniques to estimate total column ozone and aerosol absorption optical depth from the measurements of backscattered ultraviolet (buv) radiation. The total ozone algorithm has been used to create a unique record of the ozone layer, spanning more than 3 decades, from a series of instruments (BUV, SBUV, TOMS, SBUV/2) flown on NASA, NOAA, Japanese and Russian satellites. We will discuss how this algorithm can be considered a generalization of the well-known Dobson/Brewer technique that has been used to process data from ground-based instruments for many decades, and how it differs from the DOAS techniques that have been used to estimate vertical column densities of a host of trace gases from data collected by GOME and SCIAMACHY instruments. The BUV aerosol algorithm is most suitable for the detection of UV absorbing aerosols (smoke, desert dust, volcanic ash) and is the only technique that can detect aerosols embedded in clouds. This algorithm has been used to create a quarter century record of aerosol absorption optical depth using the BUV data collected by a series of TOMS instruments. We will also discuss how the data from the OM1 instrument launched on July 15,2004 will be combined with data from MODIS and CALIPSO lidar data to enhance the accuracy and information content of satellite-derived aerosol measurements. The OM1 and MODIS instruments are currently flying on EOS Aura and EOS Aqua satellites respectively, part of a constellation of satellites called the "A-train". The CALIPSO satellite is expected to join this constellation in mid 2005.

Bhartia, Pawan K.

Ozone and Aerosol Retrieval from Backscattered Ultraviolet Radiation

In this presentation we will discuss the techniques to estimate total column ozone and aerosol absorption optical depth from the measurements of back scattered ultraviolet (buv) radiation. The total ozone algorithm has been used to create a unique record of the ozone layer, spanning more than 3 decades, from a series of instruments (BUV, SBUV, TOMS, SBUV/2) flown on NASA, NOAA, Japanese and Russian satellites. We will discuss how this algorithm can be considered a generalization of the well-known Dobson/Brewer technique that has been used to process data from ground-based instruments for many decades, and how it differs from the DOAS techniques that have been used to estimate vertical column densities of a host of trace gases from data collected by GOME and SCIAMACHY instruments. The buv aerosol algorithm is most suitable for the detection of UV absorbing aerosols (smoke, desert dust, volcanic ash) and is the only technique that can detect aerosols embedded in clouds. This algorithm has been used to create a quarter century record of aerosol absorption optical depth using the buv data collected by a series of TOMS instruments. We will also discuss how the data from the OMI instrument launched on July 15, 2004 will be combined with data from MODIS and CALIPSO lidar data to enhance the accuracy and information content of satellite-derived aerosol measurements. The OMI and MODIS instruments are currently flying on EOS Aura and EOS Aqua satellites respectively, part of a constellation of satellites called the "A-train".

Bhartia, Pawan K.

Leaf light reflectance, transmittance, absorptance, and optical and geometrical parameters for eleven plant genera with different leaf mesophyll arrangements.

Review of research on radiation interactions within plant canopies and communities and interactions of various leaf structures (mesophyll arrangements) with electromagnetic radiation involved in the interpretation of data sensed from air or spacecraft. The hypothesis underlying the research reported is that leaf mesophyll arrangements influence spectral energy measurements of leaves.

Gausman, H. W.

A comparison of neutral hydrogen 21 cm observations with UV and optical absorption-line measurements

Several absorption components detected in visible or UV lines have been identified with emission features in new high-resolution, high signal-to-noise 21 cm observations. Stars for which direct overlap is obtained are HD 28497, lambda Ori, mu Col, HD 50896, rho Leo, HD 93521, and HD 219881. With the use of the inferred H I column densities from 21 cm profiles, rather than the integrated column densities obtained from L-alpha, more reliable densities can be derived from the existence of molecular hydrogen. Hence the cloud thicknesses are better determined; and 21 cm emission maps near these stars can be used to obtain dimensions on the plane of the sky. It is now feasible to derive detailed geometries for isolated clumps of gas which produce visual absorption features.

Giovanelli, R.

A model for the spectral dependence of optically induced absorption in amorphous silicon

A model based on transitions from localized band tail states to states above the mobility edge is used to explain the broad band induced absorptions observed in recent pump-probe experiments. The model gives the observed decrease of absorption with frequency at subband gap photo energies and high carrier densities (of about 10 to the 20th/cu cm). At lower carrier densities, the absorption has a maximun which is sensitive to the spatial extent of the band tail states.

Lawandy, N. M.

Participation in TOMS missions

In the past year we have been investigating a new algorithm for the derivation of column sulfur dioxide, column ozone, and aerosol optical depth from the Total Ozone Mapping Spectrometer (TOMS) High Density TOMS (HDT) archived albedos. Simulations of the measured albedos were made using a radiative transfer model, and a technique developed to separate the effects of the aerosol optical depth from the absorption optical depth. The retrieval adopted obtained values from the three parameters with high accuracy. This retrieval was then applied to the TOMS data.

Hudson, Robert D.

Interstellar Mg II and C IV absorption toward Markarian 205 by NGC 4319 - An 'optically thick' QSO absorption system

We have used the Goddard High-Resolution Spectrograph aboard HST to detect interstellar Mg II and C IV absorption lines toward Mrk 205, a QSO whose sightline passes within 3/h kpc of the foreground galaxy NGC 4319. Absorption is detected from both local Milky Way gas and from NGC 4319, making this the first observation of an isolated, low-redshift galaxy causing an 'optically thick' QSO absorption system. We also observed for the first time Mg II absorption from two local High Velocity Clouds along this same sightline. The data support the premise that metal absorption lines seen at higher redshift in QSO spectra originate in gas associated with intervening galaxies. However, neither the strong absorption by (half) of our own Galaxy, nor the weak absorption by NGC 4319, may be typical of absorbers in general.

Bowen, David V.

Ultrafast exciton and trion dynamics in highly 𝑛-doped Mo⁢S 2 monolayers: Many-body effects

Understanding many-body interactions of excitons and charge carriers in monolayer semiconductors is crucial for tuning their unique optical properties and optimizing their performance in optoelectronic devices. However, the sensitivity of these atomically thin semiconductors to doping, defects, and strain–arising from synthesis, substrate, and environmental conditions–hinders consistent observation of many-body effects. In this work, we employed linear and ultrafast transient optical absorption spectroscopy to investigate the influence of background doping on exciton many-body interactions in Mo⁢S 2 monolayers. Using reversible molecular physisorption gating, we achieved a high background doping density of 4.9 × 10 13 c⁢m −2 in an argon environment, which is significantly higher than those attainable with conventional electrical gating. Our results reveal a photoinduced 𝐴-exciton resonance redshift, attributed to band-gap renormalization at a low background-doping density of 4.3 × 10 12 c⁢m −2 in an air environment, transitioning to a blueshift at a high background-doping density of 4.9 × 10 13 c⁢m −2 due to dominant Pauli blocking effects and vertical excitation shifts. We further observed transient energy splitting between free-exciton and -trion states up to 57 meV due to exciton-electron interactions. The ultrafast spectroscopy further revealed exciton and trion dynamics, including fast energy splitting of exciton and trion resonances within 1 picosecond (ps) followed by a rapid decay having a lifetime of ∼5.4 ps. Furthermore, our results demonstrate the critical role of background-doping conditions in tuning many-body interactions and quasiparticle dynamics in 2D semiconductors, providing valuable insights for future device design and material engineering.

Doped semiconductors

TPSAS-NF1676L-34010-DND

We invert global black carbon (BC), organic carbon (OC) and desert dust (DD) aerosol emissions from POLDER/PARASOL spectral aerosol optical depth (AOD) and aerosol absorption optical depth (AAOD) using the GEOSChem inverse modelling framework. Our inverse modeling framework uses standard a priori emissions to provide a posteriori emissions that are constrained by POLDER/PARASOL AODs and AAODs. Our satellite-derived global aerosol emission database indicates an increase of BC and OC, while a decrease of DD with respect to the a priori emission inventories used in standard GEOS-Chem runs. The model simulations using a posteriori emissions (i.e. retrieved emissions) provide new estimate of global aerosol extinction and absorption constrained by observations. Additionally, the a posteriori model simulation of AOD, AAOD, single scattering albedo, Angstrom exponent, and absorption Angstrom exponent show better agreement with independent AERONET, MODIS, and OMI measurements than the a priori simulation. Thus, this study suggests that using satellite-constrained global aerosol emissions in aerosol transport models can improve the accuracy of simulated global aerosol properties and have potential to better understanding global aerosol effects on climate and human health.

Cheng Chen

Constraining global aerosol emissions using POLDER/PARASOL satellite remote sensing observations

We invert global black carbon (BC), organic carbon (OC) and desert dust (DD) aerosol emissions from POLDER/PARASOL spectral aerosol optical depth (AOD) and aerosol absorption optical depth (AAOD) using the GEOS-Chem inverse modeling framework. Our inverse modeling framework uses standard a priori emissions to provide a posteriori emissions that are constrained by POLDER/PARASOL AODs and AAODs. The following global emission values were retrieved for the three aerosol components: 18.4 Tg/yr for BC, 109.9 Tg/yr for OC and 731.6 Tg/yr for DD for the year 2010. These values show a difference of +166.7 %, +184.0 % and −42.4 %, respectively, with respect to the a priori values of emission inventories used in “standard” GEOS-Chem runs. The model simulations using a posteriori emissions (i.e., retrieved emissions) provide values of 0.119 for global mean AOD and 0.0071 for AAOD at 550 nm, which are +13.3 % and +82.1 %, respectively, higher than the AOD and AAOD obtained using the a priori values of emissions. Additionally, the a posteriori model simulation of AOD, AAOD, single scattering albedo, Ångström exponent and absorption Ångström exponent show better agreement with independent AERONET, MODIS and OMI measurements than the a priori simulation. Thus, this study suggests that using satellite-constrained global aerosol emissions in aerosol transport models can improve the accuracy of simulated global aerosol properties.

chemical transport model (CTM) simulations

The 27-28 October 1986 FIRE IFO Cirrus Case Study: Cirrus Parameter Relationships Derived from Satellite and Lidar Data

Cirrus cloud radiative and physical characteristics are determined using a combination of ground based, aircraft, and satellite measurements taken as part of the First ISCCP Region Experiment (FIRE) cirrus intensive field observations (IFO) during October and November 1986. Lidar backscatter data are used with rawinsonde data to define cloud base, center and top heights and the corresponding temperatures. Coincident GOES-4 4-km visible (0.65 micrometer) and 8-km infrared window (11.5 micrometer) radiances are analyzed to determine cloud emittances and reflectances. Infrared optical depth is computed from the emittance results. Visible optical depth is derived from reflectance using a theoretical ice crystal scattering model and an empirical bidirectional reflectance model. No clouds with visible optical depths greater than 5 or infrared optical depths less than 0.1 were used in the analysis. Average cloud thickness ranged from 0.5 km to 8.0 km for the 71 scenes. Mean vertical beam emittances derived from cloud-center temperatures were 062 for all scenes compared to 0.33 for the case study (27-28 October) reflecting the thinner clouds observed for the latter scenes. Relationships between cloud emittance , extinction coefficients, and temperature for the case study are very similar to those derived from earlier surface-based studies. The thicker clouds seen during the other IFO days yield different results. Emittances derived using cloud-top temperature wer ratioed to those determined from cloud-center temperature. A nearly linear relationship between these ratios and cloud-center temperature holds promise for determining actual cloud-top temperature and cloud thickness from visible and infrared radiance pairs. The mean ratio of the visible scattering optical depth to the infrared absorption optical depth was 2.13 for these data. This scattering efficiency ratio shows a significant dependence on cloud temperature. Values of mean scattering efficiency as high as 2.6 suggest the presence of small ice particles at temperatures below 230 K. the parameterization of visible reflectance in terms of cloud optical depth and clear sky reflectance shows promise as a simplified method for interpreting visible satellite data reflected from cirrus clouds. Large uncertainties in the optical parameters due to cloud reflectance anisotropy and shading were found by analyzing data for various solar zenith angles and for simultaneous advanced very high resolution radiometer (AVHRR) data. Inhomogeneities in the cloud fields result in uneven cloud shading that apparently causes the occurrence of anomalously dark, cloud pixels in the GOES data. These shading effects complicate the interpretation of the satellite data. The results highlight the need for additional study or cirrus cloud scattering processes and remote sensing techniques.

Minnis, Patrick

The 27-28 October 1986 FIRE IFO Cirrus Case Study: Cirrus Parameter Relationships Derived from Satellite and Lidar Data

Cirrus cloud radiative and physical characteristics are determined using a combination of ground-based, aircraft, and satellite measurements taken as part of the FIRE Cirrus Intensive Field Observations (IFO) during October and November 1986. Lidar backscatter data are used with rawinsonde data to define cloud base, center, and top heights and the corresponding temperatures. Coincident GOES 4-km visible (0.65 micro-m) and 8-km infrared window (11.5 micro-m) radiances are analyzed to determine cloud emittances and reflectances. Infrared optical depth is computed from the emittance results. Visible optical depth is derived from reflectance using a theoretical ice crystal scattering model and an empirical bidirectional reflectance model. No clouds with visible optical depths greater than 5 or infrared optical depths less than 0.1 were used in the analysis. Average cloud thickness ranged from 0.5 km to 8.0 km for the 71 scenes. Mean vertical beam emittances derived from cloud-center temperatures were 0.62 for all scenes compared to 0.33 for the case study (27-28 October) reflecting the thinner clouds observed for the latter scenes. Relationships between cloud emittance, extinction coefficients, and temperature for the case study are very similar to those derived from earlier surface- based studies. The thicker clouds seen during the other IFO days yield different results. Emittances derived using cloud-top temperature were ratioed to those determined from cloud-center temperature. A nearly linear relationship between these ratios and cloud-center temperature holds promise for determining actual cloud-top temperatures and cloud thicknesses from visible and infrared radiance pairs. The mean ratio of the visible scattering optical depth to the infrared absorption optical depth was 2.13 for these data. This scattering efficiency ratio shows a significant dependence on cloud temperature. Values of mean scattering efficiency as high as 2.6 suggest the presence of small ice particles at temperatures below 230 K. The parameterization of visible reflectance in terms of cloud optical depth and clear-sky reflectance shows promise as a simplified method for interpreting visible satellite data reflected from cirrus clouds. Large uncertainties in the optical parameters due to cloud reflectance anisotropy and shading were found by analyzing data for various solar zenith angles and for simultaneous AVHRR data. Inhomogeneities in the cloud fields result in uneven cloud shading that apparently causes the occurrence of anomalously dark, cloudy pixels in the GOES data. These shading effects complicate the interpretation of the satellite data. The results highlight the need for additional study of cirrus cloud scattering processes and remote sensing techniques.

Minnis, Patrick

Emissivity physics

Space environment effects on emissivity and optical absorption of thermal control surfaces

THERMOPHYSICS