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All sourcesNASA NTRSDOE OSTI
NASA NTRS1994

The axisymmetric stellar wind of AG Carinae

We present optical linear spectropolarimetry of the Luminous Blue Variable AG Carinae obtained after a recent visual brightness increase. The absence of He II lambda 4686 emission, together with the weakening of the He I spectrum and the appearance of Fe lines in the region around 5300 A, confirm that AG Car has started a new excursion across the HR diagram. The H alpha line profile exhibits very extended line wings that are polarized differently in both amount and position angle from either the continuum or the line core. The polarization changes across H alpha, together with variable continuum polarization, indicate the presence of intrinsic polarization. Coexistence of the line-wing polarization with extended flux-line wings evidences that both are formed by electron scattering in a dense wind. The position angle rotates across the line profiles, in a way that presently available models suggest is due to rotation and expansion of the scattering material. AG Car displays very large variations of its linear polarization with time, Delta P approximately 1.2%, indicating significant variations in envelope opacity. We find that the polarization varies along a preferred position angle of approximately 145 deg (with a scatter of +/- 10 deg) which we interpret as a symmetry axis of the stellar wind (with an ambiguity of 90 deg). This position angle is co-aligned with the major axis of the AG Car ring nebula and perpendicular to the AG Car jet. Our observations thus suggest that the axisymmetric geometry seen in the resolved circumstellar environment at various distances already exists within a few stellar radii of AG Car. From the H alpha polarization profile we deduce an interstellar polarization of Q = 0.31%, U = -1.15% at H alpha. The inferred interstellar polarization implies that the intrinsic polarization is not always of the same sign. This indicates either significant temporal changes in the envelope geometry, or it may arise from effects of multiple scattering in conjunction with density variations.

Schulte-Ladbeck, Regina E.↗
DOE OSTI2024

Universal features of 2 → N scattering in QCD and gravity from shockwave collisions

A remarkable double-copy relation of Einstein gravity to QCD in Regge asymptotics is Γ μ ν = 1 2 C μ C ν − 1 2 N μ N ν , where Γ μ ν is the gravitational Lipatov vertex in the 2 → 3 graviton scattering amplitude, C μ its Yang-Mills counterpart, and N μ the QED bremsstrahlung vertex. In QCD, the Lipatov vertex is a fundamental building block of the BFKL equation describing the 2 → N scattering of gluons at high energies. Likewise, the gravitational Lipatov vertex is a key ingredient in a 2D effective field theory framework describing trans-Planckian 2 → N graviton scattering. We construct a quantitative correspondence between a semiclassical Yang-Mills framework for radiation in gluon shockwave collisions and its counterpart in general relativity. In particular, we demonstrate the Lipatov double copy in a dilute-dilute approximation corresponding to R S , L , R S , H ≪ b , where R S , L , R S , H are the respective emergent Schwarzchild radii generated in shockwave collisions and b is the impact parameter. We outline extensions of the correspondence developed here to the dilute-dense computation of gravitational wave radiation in the close vicinity of one of the black holes, the construction of graviton propagators in the shockwave background, and a renormalization group approach to compute 2 → N amplitudes that incorporates graviton Reggeization and coherent graviton multiple scattering. Published by the American Physical Society 2024

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1995

Ocean observations with EOS/MODIS: Algorithm development and post launch studies

An investigation of the influence of stratospheric aerosol on the performance of the atmospheric correction algorithm was carried out. The results indicate how the performance of the algorithm is degraded if the stratospheric aerosol is ignored. Use of the MODIS 1380 nm band to effect a correction for stratospheric aerosols was also studied. The development of a multi-layer Monte Carlo radiative transfer code that includes polarization by molecular and aerosol scattering and wind-induced sea surface roughness has been completed. Comparison tests with an existing two-layer successive order of scattering code suggests that both codes are capable of producing top-of-atmosphere radiances with errors usually less than 0.1 percent. An initial set of simulations to study the effects of ignoring the polarization of the the ocean-atmosphere light field, in both the development of the atmospheric correction algorithm and the generation of the lookup tables used for operation of the algorithm, have been completed. An algorithm was developed that can be used to invert the radiance exiting the top and bottom of the atmosphere to yield the columnar optical properties of the atmospheric aerosol under clear sky conditions over the ocean, for aerosol optical thicknesses as large as 2. The algorithm is capable of retrievals with such large optical thicknesses because all significant orders of multiple scattering are included.

Gordon, Howard R.↗
NASA NTRS1993

Use of spectral analogy to evaluate canopy reflectance sensitivity to leaf optical property

The spectral variation of canopy reflectance is mostly governed by the absorption properties of the elements, hence the leaves, since their intrinsic scattering properties show very little spectral variation. The relationship between canopy reflectance and leaf reflectance measured at the red edge over sugar beet canopies was used to simulate canopy reflectance from leaf reflectance spectra measured over the whole spectral domain. The results show that the spectral analogies found allows accurate reconstruction of canopy reflectance spectra. Explicit assumptions about the very low spectral variation of leaf intrinsic scattering properties are thus indirectly justified. The sensitivity of canopy reflectance (rho(sub c)) to leaf optical properties can then be investigated from concurrent spectral variations of canopy (delta rho(sub c)/delta lambda) and leaf reflectance (delta rho(sub l)/delta lambda): (delta rho(sub c))/(delta rho(sub l)) = ((delta rho(sub c))/(delta lambda) ((delta rho( sub l))/(delta lambda))(sup -1)). This expression is strictly valid only when the optical properties of the soil background or the other vegetation elements such as bark are either spectrally flat or do not contribute significantly to canopy reflectance. Simulations using the SAIL and PROSPECT models demonstrate that the sensitivity of canopy reflectance to leaf reflectance is significant for large vegetation cover fractions in spectral domains where absorption is low. In these conditions, multiple, scattering enhances the leaf absorption features by a factor that can be greater than 2.0. To override the limitations of the SAIL model for the description of the canopy architecture, we tested the previous findings on experimental data. Concurrent canopy and leaf reflectance spectra were measured for a range of sugar beet canopies. The results show good agreement with the theoretical findings. Conclusions are drawn about the applicability of these findings, with particular attention to the potential detectability of leaf biochemical composition from canopy reflectance sensed from space.

Baret, Frederic↗
NASA NTRS2016

Polarized Radiative Transfer of a Cirrus Cloud Consisting of Randomly Oriented Hexagonal Ice Crystals: The 3 x 3 Approximation for Non-Spherical Particles

The reflection and transmission of polarized light for a cirrus cloud consisting of randomly oriented hexagonal columns were calculated by two very different vector radiative transfer models. The forward peak of the phase function for the ensemble-averaged ice crystals has a value of order 6 x 10(exp 3) so a truncation procedure was used to help produce numerically efficient yet accurate results. One of these models, the Vectorized Line-by-Line Equivalent model (VLBLE), is based on the doubling- adding principle, while the other is based on a vector discrete ordinates method (VDISORT). A comparison shows that the two models provide very close although not entirely identical results, which can be explained by differences in treatment of single scattering and the representation of the scattering phase matrix. The relative differences in the reflected I and Q Stokes parameters are within 0.5 for I and within 1.5 for Q for all viewing angles. In 1971 Hansen showed that for scattering by spherical particles the 3 x 3 approximation is sufficient to produce accurate results for the reflected radiance I and the degree of polarization (DOP), and he conjectured that these results would hold also for non-spherical particles. Simulations were conducted to test Hansen's conjecture for the cirrus cloud particles considered in this study. It was found that the 3 x 3 approximation also gives accurate results for the transmitted light, and for Q and U in addition to I and DOP. For these non-spherical ice particles the 3 x 3 approximation leads to an absolute error 2 x 10(exp -6) for the reflected and transmitted I, Q and U Stokes parameters. Hence, it appears to be an excellent approximation, which significantly reduces the computational complexity and burden required for multiple scattering calculations.

Polarization↗
NASA NTRS1992

Laboratory scaled simulation of lidar cloud sounding experiments

The results of lidar measurements carried out on laboratory scale models of clouds are presented. Measurements on laboratory scale models are important since one has the knowledge of the relevant parameters of the diffusing medium, such as: scattering and absorption coefficients, phase function, homogeneity, shape, etc. Knowledge of these parameters enables one to use the results to test the reliability of theoretical and numerical investigations. To obtain a laboratory scaled model of a lidar system sounding a cloud, it is necessary to scale down all the geometrical quantities by the same factor to reduce distances of the order of kilometers to the order of meters, keeping the size and the optical depth of the diffusers unchanged. If a time resolution of the order of nanoseconds is necessary for a lidar sounding actual clouds, the corresponding time resolution for the laboratory model should be of the order of picoseconds. It is possible to obtain this resolution by using picosecond laser systems and fast electrooptical detectors like the streak camera. The results of the laboratory measurements showed that the multiple scattering effect strongly depends on the size of the diffusers, as well as on the concentration. The experimental results were compared with the numerical results of a Monte Carlo code. A generally good agreement was obtained.

Zaccanti, G.↗
NASA NTRS1999

Vertical Photon Transport in Cloud Remote Sensing Problems

Photon transport in plane-parallel, vertically inhomogeneous clouds is investigated and applied to cloud remote sensing techniques that use solar reflectance or transmittance measurements for retrieving droplet effective radius. Transport is couched in terms of weighting functions which approximate the relative contribution of individual layers to the overall retrieval. Two vertical weightings are investigated, including one based on the average number of scatterings encountered by reflected and transmitted photons in any given layer. A simpler vertical weighting based on the maximum penetration of reflected photons proves useful for solar reflectance measurements. These weighting functions are highly dependent on droplet absorption and solar/viewing geometry. A superposition technique, using adding/doubling radiative transfer procedures, is derived to accurately determine both weightings, avoiding time consuming Monte Carlo methods. Superposition calculations are made for a variety of geometries and cloud models, and selected results are compared with Monte Carlo calculations. Effective radius retrievals from modeled vertically inhomogeneous liquid water clouds are then made using the standard near-infrared bands, and compared with size estimates based on the proposed weighting functions. Agreement between the two methods is generally within several tenths of a micrometer, much better than expected retrieval accuracy. Though the emphasis is on photon transport in clouds, the derived weightings can be applied to any multiple scattering plane-parallel radiative transfer problem, including arbitrary combinations of cloud, aerosol, and gas layers.

Platnick, S.↗
NASA NTRS1992

Radar depolarization signatures of rain in cumulus clouds measured with a dual-frequency air-borne radar

Experimental data are presented on dual-wavelength scattering characteristics of subtropical rain observed during the convection and precipitation/electrification (CaPE) experiment. Linear depolarization ratios (LDRs) are calculated at both X-band and Ka-band channels. In stratiform rain, the cross-polarized return signal is generally below the noise level except within the melting layer where the maximum LDR at both frequencies is typically between -12 and -10 dB. In convective rain the range profiles of the LDR in X-band and those in Ka-band do not coincide. The X-band LDR values in convective rain typically remain smaller than -25 dB at high altitudes and take somewhat larger values of -25 to -15 dB at low altitudes. The Ka-band LDR values, in contrast, typically increase with radar range, sometimes reaching a level of -3 dB just before the cross-polarized signal falls below the noise level. Such high values of LDR in Ka-band are most likely attributable to multiple scattering effects.

Iguchi, Toshio↗
NASA NTRS2018

Active and Passive Radiative Transfer Modeling of the Olympic Mountains Experiment

Sensor forward models are an important tool for interpreting remote sensing observations of geophysical phenomena. By implementing a three-dimensional framework, we can simulate and analyze observations from various sensors on disparate platforms. To demonstrate our model framework, we simulate observations from the Olympic Mountains Experiment (OLYMPEX). The use of cloud model simulations allows us to understand sensor response to cloud ice, falling snow, and other processes and features, and the application of model tools to observations allows us to quantify precipitation.MIIST 3D Forward ModelThe Multi-Instrument Inverse Solver Testbed(MIIST) uses the Atmospheric Radiative TransferSimulator (ARTS) for solving the vector radiativetransfer (RT) equation in up to three spatialdimensions within a spherical geometry• Gas absorptiono Line-by-line calculationso Fast transmittance tables• Hydrometeor scattering solverso Discrete ordinateo RT4 (Evans, 1D)o Radar Single Scattering (1D or 3D)o Monte Carlo (3D)Scattering TablesHigh-fidelity hydrometeor scatteringtables are necessary for accurateand consistent forward modeling ofmulti-frequency observations• Requires full Stokes matriceso And absorption vector• Randomly oriented particleso Discrete Dipole Approximationo Characteristic Basis Function Method(coming soon)• Horizontally-oriented plateso Invariant Imbedding T-matrix MethodCloud Resolving SimulationsCloud resolving simulations (e.g.,NU-WRF) supply output consistentwith ARTS needs• Atmospheric Informationo Temperatureo Pressure / heighto Water vapor• Hydrometeor Profileso ARTS architecture ripe for explicit binmicrophysics• Examples use Morrison 2M schemeThe Olympic Mountains Experiment (OLYMPEX)Validation for GPM of mid-latitudefrontal systems approaching nearcoastalmountains from the ocean• Large collection of ground-based andairborne sensorso Radarso Radiometerso In situ• Contemporaneous with RADEXo Two sets of radar at same frequenciesRadiometer Simulation (3 km NUWRF, 20151203, 15:00)2018.12.14 7Simulate 166 GHz polarizationdifference• Corresponds to the presence of aligned icecrystals• Look at trends for both simulations andobservations• Simulations can tolerate lower resolutiono Larger domainSimulations from Observations: OLYMPEXSimulate sensor response usinggeophysical retrievals as input• Single frequency radar retrievals• Multiple scattering enhancementapparent at W band• Spatially dependent phenomenonModeling Application: 1D Retrievals03 December 2015• DC-8 and ER-2 flightso Focus on APR-3 (DC-8)• Citationo Stacked microphysics legso Qualitative comparisonso Range of frozen habitso Presence of supercooledliquid cloudsResults• Retrievals match probeso Good qualitative match• Bands of increasedreflectivity correspond tolarge Dm and highaggregate fraction• Significant amounts ofsupercooled liquid water

Adams, Ian S.↗
DOE OSTI2025

Results of a Geant4 benchmarking study for bio‐medical applications, performed with the G4‐Med system

Geant4, a Monte Carlo Simulation Toolkit extensively used in bio-medical physics, is in continuous evolution to include newest research findings to improve its accuracy and to respond to the evolving needs of a very diverse user community. In 2014, the G4-Med benchmarking system was born from the effort of the Geant4 Medical Simulation Benchmarking Group, to benchmark and monitor the evolution of Geant4 for medical physics applications. The G4-Med system was first described in our Medical Physics Special Report published in 2021. Results of the tests were reported for Geant4 10.5. Purpose In this work, we describe the evolution of the G4-Med benchmarking system. Methods The G4-Med benchmarking suite currently includes 23 tests, which benchmark Geant4 from the calculation of basic physical quantities to the simulation of more clinically relevant set-ups. New tests concern the benchmarking of Geant4-DNA physics and chemistry components for regression testing purposes, dosimetry for brachytherapy with a 125 I source, dosimetry for external x-ray and electron FLASH radiotherapy, experimental microdosimetry for proton therapy, and in vivo PET for carbon and oxygen beams. Regression testing has been performed between Geant4 10.5 and 11.1. Finally, a simple Geant4 simulation has been developed and used to compare Geant4 EM physics constructors and physics lists in terms of execution times. Results In summary, our EM tests show that the parameters of the multiple scattering in the Geant4 EM constructor G4EmStandardPhysics_option3 in Geant4 11.1, while improving the modeling of the electron backscattering in high atomic number targets, are not adequate for dosimetry for clinical x-ray and electron beams. Therefore, these parameters have been reverted back to those of Geant4 10.5 in Geant4 11.2.1. The x-ray radiotherapy test shows significant differences in the modeling of the bremsstrahlung process, especially between G4EmPenelopePhysics and the other constructors under study (G4EmLivermorePhysics, G4EmStandardPhysics_option3, and G4EmStandardPhysics_option4). These differences will be studied in an in-depth investigation within our Group. Improvement in Geant4 11.1 has been observed for the modeling of the proton and carbon ion Bragg peak with energies of clinical interest, thanks to the adoption of ICRU90 to calculate the low energy proton stopping powers in water and of the Linhard–Sorensen ion model, available in Geant4 since version 11.0. Nuclear fragmentation tests of interest for carbon ion therapy show differences between Geant4 10.5 and 11.1 in terms of fragment yields. In particular, a higher production of boron fragments is observed with Geant4 11.1, leading to a better agreement with reference data for this fragment. Conclusions Based on the overall results of our tests, we recommend to use G4EmStandardPhysics_option4 as EM constructor and QGSP_BIC_HP with G4EmStandardPhysics_option4, for hadrontherapy applications. The Geant4-DNA physics lists report differences in modeling electron interactions in water, however, the tests have a pure regression testing purpose so no recommendation can be formulated.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2024

Elucidating Structural Disorder in Ultra‐Thin Bi‐Rich Bismuth Oxyhalide Photocatalysts

Abstract Advancing the field of photocatalysis requires the elucidation of structural properties that underpin the photocatalytic properties of promising materials. The focus of the present study is layered, Bi‐rich bismuth oxyhalides, which are widely studied for photocatalytic applications yet poorly structurally understood, due to high levels of disorder, nano‐sized domains, and the large number of structurally similar compounds. By connecting insights from multiple scattering techniques, utilizing electron‐, X‐ray‐ and neutron probes, the crystal phase of the synthesized materials is allocated as layered Bi 24 O 31 X 10 (X = Cl, Br), albeit with significant deviation from the reported 3D crystalline model. The materials comprise anisotropic platelet‐shaped crystalline domains, exhibiting significant in‐plane ordering in two dimensions but disorder and an ultra‐thin morphology in the layer stacking direction. Increased synthesis pH tailored larger, more ordered crystalline domains, leading to longer excited state lifetimes determined via femtosecond transient absorption spectroscopy (fs‐TAS). Although this likely contributes to improved photocatalytic properties, assessed via the photooxidation of benzylamine, increasing the overall surface area facilitated the most significant improvement in photocatalytic performance. This study, therefore, enabled both phase allocation and a nuanced discussion of the structure‐property relationship for complicated, ultra‐thin photocatalysts.

Chemistry↗
DOE OSTI2022

Fast and Accurate Predictions of Total Energy for Solid Solution Alloys with Graph Convolutional Neural Networks

We use graph convolutional neural networks (GCNNs) to produce fast and accurate predictions of the total energy of solid solution binary alloys. GCNNs allow us to abstract the lattice structure of a solid material as a graph, whereby atoms are modeled as nodes and metallic bonds as edges. This representation naturally incorporates information about the structure of the material, thereby eliminating the need for computationally expensive data pre-processing which would be required with standard neural network (NN) approaches. We train GCNNs on ab-initio density functional theory (DFT) for copper-gold (CuAu) and iron-platinum (FePt) data that has been generated by running the LSMS-3 code, which implements a locally self-consistent multiple scattering method, on OLCF supercomputers Titan and Summit. GCNN outperforms the ab-initio DFT simulation by orders of magnitude in terms of computational time to produce the estimate of the total energy for a given atomic configuration of the lattice structure. We compare the predictive performance of GCNN models against a standard NN such as dense feedforward multi-layer perceptron (MLP) by using the root-mean-squared errors to quantify the predictive quality of the deep learning (DL) models. We find that the attainable accuracy of GCNNs is at least an order of magnitude better than that of the MLP.

Lupo Pasini, Massimiliano↗
DOE OSTI2025

Power-Capping Metric Evaluation for Improving Energy Efficiency in HPC Applications

With high-performance computing systems now running at exascale, optimizing power-scaling management and resource utilization has become more critical than ever. This paper explores runtime power-capping optimizations that leverage integrated CPU-GPU power management on architectures like the NVIDIA GH200 superchip. We evaluate energy-performance metrics that account for simultaneous CPU and GPU power-capping effects by using two complementary approaches: speedup-energy-delay and a Euclidean distance-based multi-objective optimization method. By targeting a mostly compute-bound exascale science application, the Locally Self-Consistent Multiple Scattering (LSMS), we explore challenging scenarios to identify potential opportunities for energy savings in exascale applications, and we recognize that even modest reductions in energy consumption can have significant overall impacts. Our results highlight how GPU task-specific dynamic power-cap adjustments combined with integrated CPU-GPU power steering can improve the energy utilization of certain GPU tasks, thereby laying the groundwork for future adaptive optimization strategies.

Patrou, Maria [ORNL] (ORCID:0000000339754638)↗
DOE OSTI2024

Optimization using pathwise algorithmic derivatives of electromagnetic shower simulations

Among the well-known methods to approximate derivatives of expectancies computed by Monte-Carlo simulations, averages of pathwise derivatives are often the easiest one to apply. Computing them via algorithmic differentiation typically does not require major manual analysis and rewriting of the code, even for very complex programs like simulations of particle-detector interactions in high-energy physics. However, the pathwise derivative estimator can be biased if there are discontinuities in the program, which may diminish its value for applications. This work integrates algorithmic differentiation into the electromagnetic shower simulation code HepEmShow based on G4HepEm, allowing us to study how well pathwise derivatives approximate derivatives of energy depositions in a sampling calorimeter with respect to parameters of the beam and geometry. We found that when multiple scattering is disabled in the simulation, means of pathwise derivatives converge quickly to their expected values, and these are close to the actual derivatives of the energy deposition. Additionally, we demonstrate the applicability of this novel gradient estimator for stochastic gradient-based optimization in a model example.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Non-destructive measurement and real-time monitoring of apple hardness during ultrasonic contact drying via portable NIR spectroscopy and machine learning

Portable near-infrared spectrometer in the spectral range of 900–1700 nm was evaluated for the first time to assess and monitor apple hardness in real-time during ultrasonic drying. Calibration models were developed using PLS and ANN, and their performances were evaluated by internal leave-one-out cross-validation and an external dataset. Several pre-treatments including standard normal variate (SNV), multiplicative scatter correction (MSC), Savitzky–Golay first and second derivatives were employed to examine the effects of spectral variations in hardness prediction. Seven important wavelengths were selected using weighted regression coefficients to develop a simple MLR model to facilitate the model interpretation and circumvent noise. The models using PLS, MLR, and ANN with selected wavelengths predicted the apple hardness with R 2 p of 0.91, 0.91, 0.95, and RMSEP of 14.78, 14.85, and 12.46 N, respectively. Finally, the results indicate that portable NIR spectrometers are quite promising for real-time monitoring of apple hardness during ultrasonic drying.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Radiation-hard miniature optical engine with high bandwidth

Future silicon trackers will be operated in an intense radiation environment and require large volumes of data to be transmitted off detector. In addition, the optical modules must be of low mass in order to limit multiple scattering and nuclear interactions that would degrade the overall performance of the detector. Here, we present a miniature optical engine that satisfies these constraints. The optical engine consists of an ASIC driving a VCSEL (Vertical Cavity Surface Emitting Laser) array in an optical package. Two ASICs are designed to operate a 12-channel VCSEL array at 1.28 or 5.12 Gb/s per channel, which yields a total data rate of up to 60 Gb/s. The core transistors are fabricated in a 65 nm CMOS process which enhance the radiation-hardness. Each channel contains equalizer (CTLE) and clock-data recovery circuits (CDR) so that the ASIC can restore the highly distorted electrical signal after propagating through several meters of cables of small diameter. The equalizer, CDR, and VCSEL driver are configured via a digital I 2 C chip interface with triple redundant memory to mitigate single event upset (SEU) effects. The bias and modulation currents are controlled by a digital-to-analog converter (DAC). We present the design of the circuit together with the results of the simulations and preliminary measurements.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Reproducible emission from nonlinear random lasers

Multiple scattering of light serves as a mechanism for feedback in random lasers. Consequently, internal spatial mode patterns, lasing wavelengths, and output directionality can all be random. Strong mode interaction can occur in such devices due to spatially overlapping modes resulting in nonlinearity with respect to the pump input power. Nevertheless, temporal coherence and lasing mode amplitude can be fixed at a constant pumping rate. This is a property desirable for applications where unique randomness is exploited but expected to be reliable over time, such as physical unclonable functions. Random lasers can also be cheaply and easily fabricated, exhibit relatively low lasing thresholds and high emission intensity. However, the precise scattering properties of such structures and fluctuations in the pump field can make device emission irreproducible, thereby limiting random laser applications. Here, in this work, we directly compare the random lasing spectra from zinc oxide samples fabricated in four distinct ways: spin-coating, sputtering, solgel deposition, and atomic layer deposition. The particular method of fabrication has a strong impact. Samples made through atomic layer deposition here exhibit both reproducibility and strong nonlinearity desirable for applications. Randomness in emission spectra persists across hundreds of repeated and averaged measurements irrespective of spatial location and is demonstrably nonlinear with respect to input signal intensity.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Origin and Suppression of Beam Damage-Induced Oxygen-K Edge Artifact from γ-Al 2 O 3 using Cryo-EELS

Gamma-alumina (γ-Al 2 O 3 ), like other low-Z oxides, is readily damaged when exposed to an electron beam. This typically results in the formation of a characteristic pre-edge peak in the oxygen-K edge of electron energy-loss spectra (EELS) acquired during or after the damage process. This artifact can mask the presence of intrinsic O-K edge fine structure that would reveal chemical properties of the material; therefore, its suppression is key. In this work, we systematically investigate the conditions that give rise to the damage-induced O-K pre-edge peak and show that it can be effectively suppressed by performing EELS experiments at cryogenic (cryo) temperatures. Prolonged exposure of γ-Al 2 O 3 to a focused electron beam results in a hole bored through the sample; this was used as a reproducible beam damage condition. O-K edge EELS spectra were collected from a single-crystal γ-Al 2 O 3 sample both during and after focused 2 electron beam hole drilling, and at room and cryo temperatures, using a monochromated scanning transmission electron microscope (STEM). Furthermore, the characteristic 531 eV pre-edge peak visible in the room temperature EELS spectra was completely suppressed in the cryo-EELS spectra, even in the presence of a visible drilled hole. We then correlated these experimental observations with multiple-scattering EELS simulations to determine the likely atomistic origin of the damage-induced O-K pre-edge peak. The findings indicate that the pre-edge peak is caused primarily by the presence of surface O dimer (O-O) bonds formed during beam damage, and that operating at cryo temperature suppresses the formation of surface O-O bonds, thus preventing formation of the O-K pre-edge peak. Additionally, Al-L 2,3 edge EELS spectra revealed Al loss primarily from tetrahedral sites during hole drilling.

77 NANOSCIENCE AND NANOTECHNOLOGY↗