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At least 991 records · Page 55

Tailoring diamond’s optical properties via direct femtosecond laser nanostructuring

We demonstrate a rapid, accurate, and convenient method for tailoring the optical properties of diamond surfaces by employing laser induced periodic surface structuring (LIPSSs). The characteristics of the fabricated photonic surfaces were adjusted by tuning the laser wavelength, number of impinging pulses, angle of incidence and polarization state. Using Finite Difference Time Domain (FDTD) modeling, the optical transmissivity and bandwidth was calculated for each fabricated LIPSSs morphology. The highest transmission of ~99.5% was obtained in the near-IR for LIPSSs structures with aspect ratios of the order of ~0.65. The present technique enabled us to identify the main laser parameters involved in the machining process, and to control it with a high degree of accuracy in terms of structure periodicity, morphology and aspect ratio. We also demonstrate and study the conditions for fabricating spatially coherent nanostructures over large areas maintaining a high degree of nanostructure repeatability and optical performance. While our experimental demonstrations have been mainly focused on diamond anti-reflection coatings and gratings, the technique can be easily extended to other materials and applications, such as integrated photonic devices, high power diamond optics, or the construction of photonic surfaces with tailored characteristics in general.

36 MATERIALS SCIENCE↗

Interpretation of the 6818.9-A methane feature observed on Jupiter, Saturn, and Uranus

High-resolution (0.1-A) spectra of the 6818.9-A methane feature obtained for Jupiter, Saturn, and Uranus by Baines, Schempp, and Smith (1969) are modeled using a doubling and adding code after Hansen (1983). The feature's rotational quantum number is estimated using the relatively homogeneous atmosphere of Saturn, with only J = 0 and J = 1 fitting the observational constraints. The aerosol content within Saturn's northern temperate region is shown to be substantially less than at the equator, indicating a haze only half as optically thick. Models of Jupiter's atmosphere are consistent with the rotational quantum-number assignment. Synthetic line profiles of the 6818.9-A feature observed on Uranus reveal that a substantial haze exists at or above the methane condensation region with an optical depth eight times greater than previously reported. Seasonal effects are indicated. The methane column abundance is 5 + or - 1 km-am. The mixing ratio of methane to hydrogen within the deep unsaturated region of the planet is 0.045 + or - 0.025, based on an H2 column abundance of 240 + or - 60 km-am (Smith, Macy, and Pilcher /1980/), thus indicating that methane comprises between one-sixth and one-half of the planet's mass. However, proper reevaluation of H2 quadrupole features accounting for the haze reported here may significantly reduce the relative methane abundance.

Baines, K. H.↗

SILICATE COMPOSITION OF THE INTERSTELLAR MEDIUM

The composition of silicate dust in the diffuse interstellar medium and in protoplanetary disks around young stars informs our understanding of the processing and evolution of the dust grains leading up to planet formation. An analysis of the well-known 9.7 μ m feature indicates that small amorphous silicate grains represent a significant fraction of interstellar dust and are also major components of protoplanetary disks. However, this feature is typically modeled assuming amorphous silicate dust of olivine and pyroxene stoichiometries. Here, we analyze interstellar dust with models of silicate dust that include non-stoichiometric amorphous silicate grains. Modeling the optical depth along lines of sight toward the extinguished objects Cyg OB2 No. 12 and ζ Ophiuchi, we find evidence for interstellar amorphous silicate dust with stoichiometry intermediate between olivine and pyroxene, which we simply refer to as “polivene.” Finally, we compare these results to models of silicate emission from the Trapezium and protoplanetary disks in Taurus.

79 ASTRONOMY AND ASTROPHYSICS↗

AeroCom Phase III Multi-Model Evaluation of the Aerosol Life Cycle and Optical Properties Using Ground and Space-Based Remote Sensing as Well as Surface In Situ Observations

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2∕3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AODf, AODc), Ångström exponent (AE), dry surface scattering (SCdry), and absorption (ACdry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from −37 % (MODIS-Terra) to −16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AODc (∼ −45 % ± 25 %) than in fine AODf (∼ −15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AODc bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AODc. Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of −35 % ± 25 % and −20 % ± 18 % for SCdry and ACdry, respectively. The larger underestimate of SCdry than ACdry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. −15 %, however, with a considerably large interquartile range, suggesting a spread between −35 % and +10 %.

space-based remote sensing↗

Efficient Modeling of Structural, Electronic, and Optical Properties of Silver and Gold Metal Nanoclusters and Alloys Using Optimized SCC-DFTB Parameters

Computation of optical properties using conventional time-dependent density functional theory (TD-DFT) is time-consuming and memory-intensive. In this study, we investigate the accuracy and efficiency of the density functional tight binding (DFTB) framework with newly optimized Slater–Koster (SK) parameters for modeling the structural, electronic properties, and absorption spectra of silver and gold nanoclusters and their alloys. Our investigation of the ground state (GS) properties demonstrates that the newly developed GS-SK parameters enable DFTB to closely approximate DFT-calculated bond lengths for octahedron, tetrahedron, icosahedra, and truncated octahedron with sizes Ag n /Au n (n = 19, 20, 38, 55), nanoclusters and Ag 20 /Au 20 nanoalloys, with a maximum deviation of approximately 0.15 Å. Formation energy results indicate that the GS-SK parameters can closely estimate changes in formation energies with alloy composition, and the comparison of electronic structures for Ag 20 , Au 20 , and AgAu alloy nanoclusters using the DFTB approximation reveals good agreement in the projected density of states (DOS) profiles and energy levels. A second set of SK parameters, ES-SK, has been developed to describe excited state (ES) properties, including the absorption spectra of silver octahedron Ag 19 , tetrahedral Ag n (n = 20, 56, 84), truncated octahedron Ag 38 , and icosahedra Ag 55 closed-shell clusters and their gold and alloy counterparts over a broad range of alloy compositions. This parametrization uses TD-DFTB calculations and fine-tunes the d and p eigenvalues by comparing them to reference absorption spectra from first-principles TD-DFT. This enables the generation of absorption spectra that closely match the reference spectra when plasmon excitation is dominant, as demonstrated by studying the plasmonic properties of icosahedral Ag n and Au n (n = 309 and 561) nanoparticles. This includes the rapid loss in plasmon quality when Au partially replaces Ag in alloy clusters. Furthermore, these results provide a foundation for addressing computational bottlenecks in plasmonics and with new prospects for applications in the quantum plasmonics for bimetallic alloys.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Design and Construction of a Field Capable Snapshot Hyperspectral Imaging Spectrometer

The computed-tomography imaging spectrometer (CTIS) is a device which captures the spatial and spectral content of a rapidly evolving same in a single image frame. The most recent CTIS design is optically all reflective and uses as its dispersive device a stated the-art reflective computer generated hologram (CGH). This project focuses on the instrument's transition from laboratory to field. This design will enable the CTIS to withstand a harsh desert environment. The system is modeled in optical design software using a tolerance analysis. The tolerances guide the design of the athermal mount and component parts. The parts are assembled into a working mount shell where the performance of the mounts is tested for thermal integrity. An interferometric analysis of the reflective CGH is also performed.

Arik, Glenda H.↗

Modeling Time Dispersion Due to Optical Path Length Differences in Scintillation Detectors

In this paper, we characterize the nature of the time dispersion in scintillation detectors caused by path length differences of the scintillation photons as they travel from their generation point to the photodetector. Using Monte Carlo simulation, we find that the initial portion of the distribution (which is the only portion that affects the timing resolution) can usually be modeled by an exponential decay. The peak amplitude and decay time depend both on the geometry of the crystal, the position within the crystal that the scintillation light originates from, and the surface finish. In a rectangular parallelpiped LSO crystal with 3 mm × 3 mm cross section and polished surfaces, the decay time ranges from 10 ps (for interactions 1 mm from the photodetector) up to 80 ps (for interactions 50 mm from the photodetector). Over that same range of distances, the peak amplitude ranges from 100% (defined as the peak amplitude for interactions 1 mm from the photodetector) down to 4% for interactions 50 mm from the photodetector. Higher values for the decay time are obtained for rough surfaces, but the exact value depends on the simulation details. Finally, estimates for the decay time and peak amplitude can be made for different cross section sizes via simple scaling arguments.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Optical reprocessing of gamma-ray bursts

One model for the optical flashes associated with three cosmic gamma-ray burst sources invokes the reprocessing of some of the gamma-radiation emitted by a hypothesized collapsed object in the surface layers of a nearby companion star. This model was investigated by carrying out detail, fully hydrodynamical calculations of such reprocessing in the surface layers of very low mass stars. It is found that, at most, 7 percent of the gamma-ray fluence incident on the companion star is reprocessed into the blue band; the time scale for this reprocessing is typically 100 s, which is long compared to the duration of the gamma-ray burst itself. Using this result, it is shown that there is marginal agreement between the observed and calculated ratios of gamma-ray fluence to optical fluence at earth.

Melia, F.↗

Influence of electron transport layer thickness on optical properties of organic light-emitting diodes

We investigate experimentally and theoretically the influence of electron transport layer (ETL) thickness on properties of typical N,N′-diphenyl-N,N′-bis(1-naphthyl)-[1,1′-biphthyl]-4,4′-diamine (NPB)/tris-(8-hydroxyquinoline) aluminum (Alq{sub 3}) heterojunction based organic light-emitting diodes (OLEDs), where the thickness of ETL is varied to adjust the distance between the emitting zone and the metal electrode. The devices showed a maximum current efficiency of 3.8 cd/A when the ETL thickness is around 50 nm corresponding to an emitter-cathode distance of 80 nm, and a second maximum current efficiency of 2.6 cd/A when the ETL thickness is around 210 nm corresponding to an emitter-cathode distance of 240 nm. We adopt a rigorous electromagnetic approach that takes parameters, such as dipole orientation, polarization, light emitting angle, exciton recombination zone, and diffusion length into account to model the optical properties of devices as a function of varying ETL thickness. Our simulation results are accurately consistent with the experimental results with a widely varying thickness of ETL, indicating that the theoretical model may be helpful to design high efficiency OLEDs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

On the structure of the drifton phase space and its relation to the Rayleigh–Kuo criterion of the zonal-flow stability

The phase space of driftons (drift-wave quanta) is studied within the generalized Hasegawa–Mima collisionless-plasma model in the presence of zonal flows. This phase space is made intricate by the corrections to the drifton ray equations that were recently proposed by Parker [J. Plasma Phys. 82, 595820602 (2016)] and Ruiz et al. [Phys. Plasmas 23, 122304 (2016)]. Contrary to the traditional geometrical-optics (GO) model of the drifton dynamics, it is found that driftons can not only be trapped or passing but also accumulate spatially while experiencing indefinite growth of their momenta. In particular, it is found that the Rayleigh–Kuo threshold known from geophysics corresponds to the regime when such “runaway” trajectories are the only ones possible. On one hand, this analysis helps to visualize the development of the zonostrophic instability, particularly its nonlinear stage, which is studied here both analytically and through wave-kinetic simulations. On the other hand, the GO theory predicts that zonal flows above the Rayleigh–Kuo threshold can only grow; hence, the deterioration of intense zonal flows cannot be captured within a GO model. In particular, this means that the so-called tertiary instability of intense zonal flows cannot be adequately described within the quasilinear wave kinetic equation, contrary to some previous studies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Modeling the Electronic Absorption Spectra of the Indocarbocyanine Cy3

Accurate modeling of optical spectra requires careful treatment of the molecular structures and vibronic, environmental, and thermal contributions. The accuracy of the computational methods used to simulate absorption spectra is limited by their ability to account for all the factors that affect the spectral shapes and energetics. The ensemble-based approaches are widely used to model the absorption spectra of molecules in the condensed-phase, and their performance is system dependent. The Franck–Condon approach is suitable for simulating high resolution spectra of rigid systems, and its accuracy is limited mainly by the harmonic approximation. In this work, the absorption spectrum of the widely used cyanine Cy3 is simulated using the ensemble approach via classical and quantum sampling, as well as, the Franck–Condon approach. The factors limiting the ensemble approaches, including the sampling and force field effects, are tested, while the vertical and adiabatic harmonic approximations of the Franck–Condon approach are also systematically examined. Our results show that all the vertical methods, including the ensemble approach, are not suitable to model the absorption spectrum of Cy3, and recommend the adiabatic methods as suitable approaches for the modeling of spectra with strong vibronic contributions. We find that the thermal effects, the low frequency modes, and the simultaneous vibrational excitations have prominent contributions to the Cy3 spectrum. The inclusion of the solvent stabilizes the energetics significantly, while its negligible effect on the spectral shapes aligns well with the experimental observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Integrated Optical Design Analysis (IODA): New Test Data and Modeling Features

A general overview of the capabilities of the IODA ("Integrated Optical Design Analysis") exchange of data and modeling results between thermal, structures, optical design, and testing engineering disciplines. This presentation focuses on new features added to the software that allow measured test data to be imported into the IODA environment for post processing or comparisons with pretest model predictions. software is presented. IODA promotes efficient

Moore, Jim↗

A statistical model of the photomultiplier gain process with applications to optical pulse detection

A Markov diffusion model was used to determine an approximate probability density for the random gain. This approximate density preserves the correct second-order statistics and appears to be in reasonably good agreement with experimental data. The receiver operating curve for a pulse counter detector of PMT cathode emission events was analyzed using this density. The error performance of a simple binary direct detection optical communication system was also derived.

Tan, H. H.↗

A statistical model of the photomultiplier gain process with applications to optical pulse detection

A Markov diffusion model was used to determine an approximate probability density for the random gain. This approximate density preserves the correct second-order statistics and appears to be in reasonably good agreement with experimental data. The receiver operating curve for a pulse counter detector of PMT cathode emission events was analyzed using this density. The error performance of a simple binary direct detection optical communication system was also derived. Previously announced in STAR as N82-25100

Tan, H. H.↗

Transport and optical conductivity in the Hubbard model: A high-temperature expansion perspective

We derive analytical expressions for the spectral moments of the dynamical response functions of the Hubbard model using the high-temperature series expansion. We consider generic dimension d as well as the infinite- d limit, arbitrary electron density n, and both finite and infinite repulsion U. We use moment-reconstruction methods to obtain the one-electron spectral function, the self-energy, and the optical conductivity. They are all smooth functions at high temperature and, at large U, they are featureless with characteristic widths of the order of the lattice hopping parameter t. In the infinite-d limit, we compare the series expansion results with accurate numerical renormalization group and interaction expansion quantum Monte Carlo results. We find excellent agreement down to surprisingly low temperatures, throughout most of the bad-metal regime, which applies for T≳ (1 - n)D, the Brinkman-Rice scale. The resistivity increases linearly in T at high temperature without saturation. This results from the 1/T behavior of the compressibility or kinetic energy, which play the role of the effective carrier number. In contrast, the scattering time (or diffusion constant) saturates at high T. We find that σ( n,T) ≈ (1 - n)σ(n = 0,T) to a very good approximation for all n, with σ(n = 0,T) ∝ t/T at high temperatures. The saturation at small n occurs due to a compensation between the density dependence of the effective number of carriers and that of the scattering time. The T dependence of the resistivity displays a kneelike feature which signals a crossover to the intermediate-temperature regime where the diffusion constant (or scattering time) starts increasing with decreasing T. At high temperatures, the thermopower obeys the Heikes formula, while the Wiedemann-Franz law is violated with the Lorenz number vanishing as 1/T 2 . The relevance of our calculations to experiments probing high-temperature transport in materials with strong electronic correlations or ultracold atomic gases in an optical lattice is briefly discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Impact of Multiple Scattering on Longwave Radiative Transfer Involving Clouds

Abstract General circulation models (GCMs) are extensively used to estimate the influence of clouds on the global energy budget and other aspects of climate. Because radiative transfer computations involved in GCMs are costly, it is typical to consider only absorption but not scattering by clouds in longwave (LW) spectral bands. In this study, the flux and heating rate biases due to neglecting the scattering of LW radiation by clouds are quantified by using advanced cloud optical property models, and satellite data from Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), CloudSat, Clouds and the Earth's Radiant Energy System (CERES), and Moderate Resolution Imaging Spectrometer (MODIS) merged products (CCCM). From the products, information about the atmosphere and clouds (microphysical and buck optical properties, and top and base heights) is used to simulate fluxes and heating rates. One‐year global simulations for 2010 show that the LW scattering decreases top‐of‐atmosphere (TOA) upward flux and increases surface downward flux by 2.6 and 1.2 W/m 2 , respectively, or approximately 10% and 5% of the TOA and surface LW cloud radiative effect, respectively. Regional TOA upward flux biases are as much as 5% of global averaged outgoing longwave radiation (OLR). LW scattering causes approximately 0.018 K/d cooling at the tropopause and about 0.028 K/d heating at the surface. Furthermore, over 40% of the total OLR bias for ice clouds is observed in 350–500 cm −1 . Overall, the radiative effects associated with neglecting LW scattering are comparable to the counterpart due to doubling atmospheric CO 2 under clear‐sky conditions.

54 ENVIRONMENTAL SCIENCES↗

Development Fiber Optic Distributed System for Direct Detection of Subsurface Gases Leakages

Carbon, natural gas, and hydrogen gas storage is an emerging solution to safeguard us against pollution, support goals of negative carbon emission, and protect sources of renewable energy. Properly constructed storage wells provide a virtually impervious barrier to any unintended subsurface transmission. The ability to ensure the long-term integrity of such wells is vital to the success of any storage operation and be successful in the public eyes. Therefore, robust monitoring of any gas migration into the subsurface is highly sought. A fiber-optic distributed chemical sensor (DCS) enables monitoring of long-term well integrity along its depth, ensuring the success of any storage operation and bolsters public acceptance of the safety of the reservoir via leak early detection. The same technique can be applied to gas monitoring in pipeline networks and nuclear stockpile monitoring applications. Fiber based Raman spectroscopy enables DCS, as optical fibers can be deployed in virtually any environment and relay spectroscopic information over long distances back to the user. Hollow core fibers (HCF) make excellent DCSs as the air core of the fiber allows gas from the environment to diffuse into the core, which interacts with the laser signal that is carried in the air core. This work builds upon the previous LDRD project, Fiber Optic System for Direct Detection of Carbon Dioxide Leakage in Carbon Storage Wells (21-FS-003), in which the feasibility of Raman spectroscopy detection of Carbon Dioxide (CO2) in HCF detection was demonstrated. We mitigated the risk of this DCS technology by establishing and completing five objectives. The first objective was to model and optically characterize HCF uptake of CO2, establishing the relationship between HCF length, gas diffusion time, detectable gas concentration, and measured Raman intensity. In objective two, we developed a fiber core drilling recipe to enable additional diffusion ports in the fiber core and established a method for maintaining fiber strength and integrity post drilling. Objective three characterized the drilled fibers against the undrilled fibers, establishing the differences in the gas mechanics and optical properties and provided parameters to iterate the drilling process. In objective four, a fusion splicing technique was developed to join the HCF to conventional single-mode fibers, localizing the gas detection point at the drilled HCF hole, emulating a DCS. Lastly, objective five was the testing of the sensor in Edgar Mines at Colorado School of Mines on a CO2 pipeline with a simulated leak, to showcase the ability to detect CO2 leaks. This capstone result showed CO2 leak detection in < 10 minutes, raising the technology readiness level of HCF segments as deployable DCS.

organic↗

Optical polarimetry of PKS 2155 - 304 and constraints on accretion disk models for BL Lacertae objects

Optical broad-band polarimetry and photometry of the BL Lacertae object PKS 2155 - 304 during late 1990 are presented. Variability in both flux and linear polarization was moderate during this period. The optical polarization ranged from 2 to 7 percent while photometric variations were within 0.2 mag (V = 13.2-13.4). Accurate multicolor measurements were made to study any wavelength dependence of the polarization with an eye to using these data to test the model of Wandel and Urry (1991) which proposes that the UV to soft X-ray continuum of this object arises from an accretion disk. Wavelength-dependent polarization (WDP) is observed in PKS 2155 - 304. However, the polarization is always seen to decrease with wavelength when WDP is observed. This is opposite to the expected sense of WDP if the UV continuum is dominated by an accretion disk.

Smith, Paul S.↗