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DOE OSTI2024

Bragg Coherent Imaging of Fluctuating Domains

This review presents two examples of domain dynamics in crystalline solid state samples which were imaged recently with synchrotron X-rays by Bragg Coherent Diffraction methods. Domains are associated with sub-atomic phase shifts in the structure which are revealed by the strong phase contrast associated with Bragg diffraction. At low temperatures, La2-xSrxNiO4 has an antiferromagnetic spin-ordered phase with correlation lengths of 200 nm; its domains are imaged with magnetic Bragg Ptychography to visualize their slow fluctuations. Hydrothermally synthesized nanocrystalline BaTiO3 is found to be made up of ~50 nm domains using Bragg Coherent Diffraction Imaging; electric field induced movement of its internal domain walls is a likely explanation of the nano-material's anomalously large dielectric constant, which is used in the manufacture of multilayer ceramic capacitors

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2022

Q-dependent collective relaxation dynamics of glass-forming liquid Ca0.4K0.6(NO3)1.4 investigated by wide-angle neutron spin-echo

Abstract The relaxation behavior of glass formers exhibits spatial heterogeneity and dramatically changes upon cooling towards the glass transition. However, the underlying mechanisms of the dynamics at different microscopic length scales are not fully understood. Employing the recently developed wide-angle neutron spin-echo spectroscopy technique, we measured the Q -dependent coherent intermediate scattering function of a prototypical ionic glass former Ca 0.4 K 0.6 (NO 3 ) 1.4 , in the highly viscous liquid state. In contrast to the structure modulated dynamics for Q < 2.4 Å −1 , i.e., at and below the structure factor main peak, for Q > 2.4 Å −1 , beyond the first minimum above the structure factor main peak, the stretching exponent exhibits no temperature dependence and concomitantly the relaxation time shows smaller deviations from Arrhenius behavior. This finding indicates a change in the dominant relaxation mechanisms around a characteristic length of 2π/(2.4 Å −1 ) ≈ 2.6 Å, below which the relaxation process exhibits a temperature independent distribution and more Arrhenius-like behavior.

42 ENGINEERING↗

DOE OSTI2020

Stochastic Inversion of Gaussian Random Media Using Transverse Coherence Functions for Reflected Waves: Theory and Method

The transverse coherence functions (TCFs) of phase and amplitude fluctuations of a seismic wave are powerful to estimate the spatial distribution, length scales, and strength of random heterogeneities. However, TCFs have been formulated for transmitted waves only, not for reflected waves. In this paper, we derive reflection TCFs for Gaussian random media. Furthermore, we propose to invert for Gaussian random media using the reflection TCFs based on the grid search. We validate the new reflection TCF formulas using 2D finite-difference numerical experiments. The numerical example also illustrates the feasibility and efficiency of the inversion. The stochastic inversion using reflected waves can be used in both exploration and global seismology.

58 GEOSCIENCES↗

DOE OSTI2020

Coherent band-edge oscillations and dynamic longitudinal-optical phonon mode splitting as evidence for polarons in perovskites

The coherence of collective modes, such as phonons and polarons, and their modulation of electronic states is long sought in complex systems, which is a crosscutting issue in photovoltaics and quantum electronics. In photovoltaic cells and lasers based on metal halide perovskites, the presence of polarons, i.e., photocarriers dressed by the macroscopic motion of charged lattice, assisted by terahertz (THz) longitudinal-optical (LO) phonons, has been intensely studied yet is still debated. This may be key for explaining the remarkable properties of the perovskite materials, e.g., defect tolerance, long charge lifetimes, and diffusion lengths. In this work we use the intense single-cycle THz pulse with peak electric field up to E THz = 1000 kV/cm to drive coherent polaronic band-edge oscillations at room temperature in CH 3 NH 3 PbI 3 (MAPbI 3 ). We reveal the oscillatory behavior is dominated by a specific quantized lattice vibration mode at $ω$ LO ~ 4 THz, which is both dipole and momentum forbidden. THz-driven coherent polaron dynamics exhibits distinguishing features: room temperature coherent oscillations at ω LO longer than 1 ps in both single crystals and thin films, mode-selective modulation of different band-edge states assisted by electron-phonon interaction, and dynamic mode splitting at low temperature due to entropy and anharmonicity of organic cations. Our results demonstrate intense THz-driven coherent band-edge modulation is a powerful probe of electron-lattice coupling phenomena and polaronic quantum control in perovskites.

36 MATERIALS SCIENCE↗

DOE OSTI2019

LPSE : A 3-D wave-based model of cross-beam energy transfer in laser-irradiated plasmas

The new component of the “laser–plasma simulation environment” (LPSE) described here is a practical numerical model that solves the coupled vector equations for the propagation of nearly monochromatic, coherent, lectromagnetic waves in inhomogeneous unmagnetized plasmas. It operates efficiently in the numerically challenging semiclassical regime where characteristic plasma scale lengths are many times greater than the wavelength of the light and solutions are highly oscillatory. Solutions can be obtained in one, two, or three spatial dimensions and time. Additionally, the model includes the effects of nonlinear coupling of electromagnetic waves to the low-frequency plasma perturbations (i.e., ion-acoustic response) that are responsible for stimulated Brillouin scattering. Induced plasma perturbations are assumed to be imposed on a prescribed large-scale inhomogeneous background that includes spatially varying plasma density and flow. Our code is directly relevant to the problem of cross-beam energy transfer in laser-driven inertial confinement fusion. Lastly, it may also be applicable in other areas where eikonal solutions of multicomponent wave equations (or coupled wave equations) are insufficient, such as optical scattering from ultrasound, electron dynamics in quantum devices or in nanoscale light–matter interactions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

A Consistent Representation of Cloud Overlap and Cloud Subgrid Vertical Heterogeneity

Many global climate models underestimate the cloud cover and overestimate the cloud albedo, especially for low-level clouds. We determine how a correct representation of the vertical structure of clouds can fix part of this bias. We use the 1D McICA framework and focus on low-level clouds. Using Large Eddy Simulations results as reference, we propose a method based on exponential-random overlap that represents the cloud overlap between layers and the subgrid cloud properties over several vertical scales, with a single value of the overlap parameter. Starting from a coarse vertical grid, representative of atmospheric models, this algorithm is used to generate the vertical profile of the cloud fraction with a finer vertical resolution, or to generate it on the coarse grid but with subgrid heterogeneity and cloud overlap that ensures a correct cloud cover. Doing so we find decorrelation lengths are dependent on the vertical resolution, except if the vertical subgrid heterogeneity and interlayer overlap are taken into account coherently. We confirm that the frequently used maximum-random overlap leads to a significant error by underestimating the low-level cloud cover with a relative error of about 50%, that can lead to an error of SW cloud albedo as big as 70%. Not taking into account the subgrid vertical heterogeneity of clouds can cause a relative error of 20% in brightness, assuming the cloud cover is correct.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Quantitative Scanning Transmission Electron Microscopy for Materials Science: Imaging, Diffraction, Spectroscopy, and Tomography

Scanning transmission electron microscopy (STEM) is one of the most powerful characterization tools in materials science research. Due to instrumentation developments such as highly coherent electron sources, aberration correctors, and direct electron detectors, STEM experiments can examine the structure and properties of materials at length scales of functional devices and materials down to single atoms. STEM encompasses a wide array of flexible operating modes, including imaging, diffraction, spectroscopy, and 3D tomography experiments. This review outlines many common STEM experimental methods with a focus on quantitative data analysis and simulation methods, especially those enabled by open source software. The hope is to introduce both classic and new experimental methods to materials scientists and summarize recent progress in STEM characterization. The review also discusses the strengths and weaknesses of the various STEM methodologies and briefly considers promising future directions for quantitative STEM research.

36 MATERIALS SCIENCE↗

NASA NTRS1981

Two-dimensional turbulence models

Two-dimensional turbulence models are compared with experimental measurements made using an array of instrumented towers. The spatial correlation coefficient, the two-point spectrum or cross spectrum, and the coherence function are discussed. The prediction techniques in general agree reasonably well with the experimental results. Measurements of the integral length scale however, do not correlate well with the prediction model.

Frost, W.↗

NASA NTRS1985

Near field pressure fluctuations of a circular jet

The relationship between the evolution of vortices in a circular jet and the generation of fluctuating pressure was studied, using an apparatus consisting of a jet nozzle connected to a stagnation chamber with a fifth-order polynomial contraction. The data were digitized and computer-processed. The constant pressure contours near the jet shoow that the evolution of coherent structures is the source of pressure perturbations. The data obtained in the vicinity of the jet indicate that two length scales govern the decay of the fluctuating pressure. A thin hydrodynamic near-field extends about 1 instability wavelength from the jet edge, and pressure decays exponentially. A thick acoustic near-field takes about ten acoustic wavelengths to reach the far field. The pressure disturbances decay algebraically in this region.

Lafouasse, B.↗

NASA NTRS1994

A method of measuring the amplitude-modulated vacuum field near a conducting mirror

Electromagnetic fields of the vacuum mode near a conducting mirror are modified with respect to those in free space, with their amplitudes having a sinusoidal spatial dependence from the mirror. Therefore if we combine this spatially amplitude-modulated vacuum field mode and intense coherent light with a beam splitter, we may detect this fluctuation of the vacuum mode in a homodyne detection scheme. It will give a new method to produce squeezed states of light with a single mirror placed close to an unused port of a beam splitter. We show that the amplitude fluctuation of the combined light can be reduced by a factor of 2 below that of the coherent light. We also discuss the limitations due to the finite line width of the laser and the effective absorption length of the photodiodes.

Youn, Sun-Hyun↗

NASA NTRS1997

Error Control Coding Techniques for Space and Satellite Communications

Turbo coding using iterative SOVA decoding and M-ary differentially coherent or non-coherent modulation can provide an effective coding modulation solution: (1) Energy efficient with relatively simple SOVA decoding and small packet lengths, depending on BEP required; (2) Low number of decoding iterations required; and (3) Robustness in fading with channel interleaving.

Costello, Daniel J., Jr.↗

NASA NTRS2022

The Impact of Firn Models on Ultrawideband Brightness Temperatures in the Partially Coherent Model

The density profile of a polar ice sheet is an important parameter for the estimation of ice mass balance. Wave reflections caused by density variations are also a key uncertainty in the retrieval of ice sheet temperature profiles in Ultra-Wide band radiometry. In this paper, we examine different firn density profile models and analyze the subsurface reflections they cause using an analytical partially coherent approach. We also examine firn density profiles obtained from borehole measurements, from past UWBRAD modeling studies, from a community firn model, and from snow radar echo measurements. In previous studies, the ice sheet has been model as a 1D random medium with density variations in depth. However, horizontal density variations also exist, so that the ice sheet is a 3D random medium. Analyses using the partially coherent model show that in the presence of horizontal fluctuations, contributions from short scale variations vanish as the horizontal correlation length decreases due to the diffraction of waves.

Haokui Xu↗

NASA NTRS2023

Polar Firn Properties in Greenland and Antarctica and Related Effects on Microwave Brightness Temperatures

In studying the mass balance of polar ice sheets, fluctuations of firn density near the surface is a major uncertainty. In this paper, we explore these variations at locations in the Greenland Ice Sheet and at the Dome C location in Antarctica. Borehole in situ measurements, Snow Radar echoes, microwave brightness temperatures, and modelling results from the Community firn model (CFM) are used. It is shown that firn density profiles can be represented using 3 processes: “long” and “short” length scale density variations and “refrozen layers”. Consistency with this description is observed in the dynamic range of airborne 0.5-2 GHz brightness temperatures and Snow Radar echo peaks in measurements performed in Greenland in 2017. Based on these insights, a new analytical partially coherent model is implemented to explain the microwave brightness temperatures using the three scale description of the firn. Short and long scale firn processes are modelled as a 3D continuous random medium with finite vertical and horizontal correlation lengths as opposed to past 1D random layered medium descriptions. Refrozen layers are described as deterministic sheets with planar interfaces, with the number of refrozen layer interfaces determined by radar observations. Firn density and correlation length parameters used in forward modelling to match measured 0.5-2 GHz brightness temperatures in Greenland show consistency with similar parameters in CFM predictions. Model predictions also are in good agreement with multi-angle 1.4 GHz vertically and horizontally polarized brightness temperature measured by the SMOS satellite at DOME C, Antarctica. This work shows that co-located active and passive microwave measurements can be used to infer polar firn properties that can be compared with predictions of the CFM. In particular, 0.5-2 GHz brightness temperature measurements are shown to be sensitive to long scale firn density fluctuations with density standard deviations in the range 0.01-0.06 g/cm^3 and vertical correlation lengths of 6-20 cm.

Haokui Xu↗

NASA NTRS1972

Populating excited states of incoherent atoms using coherent light.

Study of the influence of various experimental parameters on the interaction between a multimode high-intensity laser light and the absorbing atoms of an atomic gas. Using a simplified treatment of line broadening which does not include correlations between momentum-changing collisions and pressure-broadening collisions, expressions are obtained that show the effect of pressure, laser-pulse length, and intensity on the excitation. It is found that, as long as the dephasing time of the atomic system is sufficiently short, the interaction reduces to a two-body collision between the atoms and photons, where coherence effects do not occur.

Mcilrath, T. J.↗

DOE OSTI2020

High-Energy Coherent X-Ray Dffraction Microscopy of Polycrystal Grains: First Steps Towards a Multi-Scale Approach

Here, we present proof-of-concept imaging measurements of a polycrystalline material that integrate the elements of conventional high-energy x-ray diffraction microscopy with coherent diffraction-imaging techniques, and that can enable in situ strain-sensitive imaging of lattice structure in ensembles of deeply embedded crystals over five decades of length scale upon full realization. We demonstrate that the combination of these two characterization methods enables a more complete picture of the crystal-lattice strain than either method is capable of providing individually. Such complementary imaging capabilities are critical to addressing questions in a variety of research areas such as materials science and engineering, chemistry, and solid-state physics. Towards this eventual goal, the following key aspects are demonstrated: (1) high-energy Bragg coherent diffraction imaging (HE BCDI) of submicron-scale crystallites at 52 keV at current third-generation synchrotron light sources, (2) HE BCDI performed in conjunction with far-field high-energy diffraction microscopy (FF HEDM) on the grains of a polycrystalline sample in a smoothly integrated manner, and (3) the orientation information of an ensemble of grains obtained via FF HEDM used to perform complementary HE BCDI on multiple Bragg reflections of a single targeted grain. The imaged structures are seen to be 477 ± 50 nm or smaller in size, with an estimated strain resolution of 2.5 x 10 -4 . These steps lay the foundation for integration of HE BCDI, which typically provides a spatial resolution tens of nanometers, into a broad suite of well-established HEDM methods, extending HEDM beyond the few-micrometer resolution bound and into the nanoscale, and positioning the approach to take full advantage of the orders-of-magnitude improvement of x-ray coherence expected at fourth-generation light sources presently being built and commissioned worldwide.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Comprehensive view of microscopic interactions between DNA-coated colloids

Abstract The self-assembly of DNA-coated colloids into highly-ordered structures offers great promise for advanced optical materials. However, control of disorder, defects, melting, and crystal growth is hindered by the lack of a microscopic understanding of DNA-mediated colloidal interactions. Here we use total internal reflection microscopy to measure in situ the interaction potential between DNA-coated colloids with nanometer resolution and the macroscopic melting behavior. The range and strength of the interaction are measured and linked to key material design parameters, including DNA sequence, polymer length, grafting density, and complementary fraction. We present a first-principles model that screens and combines existing theories into one coherent framework and quantitatively reproduces our experimental data without fitting parameters over a wide range of DNA ligand designs. Our theory identifies a subtle competition between DNA binding and steric repulsion and accurately predicts adhesion and melting at a molecular level. Combining experimental and theoretical results, our work provides a quantitative and predictive approach for guiding material design with DNA-nanotechnology and can be further extended to a diversity of colloidal and biological systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1988

Holocinematographic Velocimeter

Holographic movies used to study turbulent flows. High-speed movie composed of single-exposure holograms of tracer particles in each of two simultaneous orthogonal views of flow. Time resolution set by movie frame rate, and total time limited by length of movie. Data from system used to verify results of theoretical models and numerical simulations of turbulence, visualize and measure coherent structures in "non-simple" turbulent flows, to examine mechanisms operative in various turbulence-control/drag-reduction concepts.

Weinstein, Leonard M.↗

NASA NTRS2000

Dynamics of Active Separation Control at High Reynolds Numbers

A series of active flow control experiments were recently conducted at high Reynolds numbers on a generic separated configuration. The model simulates the upper surface of a 20% thick Glauert-Goldschmied type airfoil at zero angle of attack. The flow is fully turbulent since the tunnel sidewall boundary layer flows over the model. The main motivation for the experiments is to generate a comprehensive data base for validation of unsteady numerical simulation as a first step in the development of a CFD design tool, without which it would not be possible to effectively utilize the great potential of unsteady flow control. This paper focuses on the dynamics of several key features of the baseline as well as the controlled flow. It was found that the thickness of the upstream boundary layer has a negligible effect on the flow dynamics. It is speculated that separation is caused mainly by the highly convex surface while viscous effects are less important. The two-dimensional separated flow contains unsteady waves centered on a reduced frequency of 0.8, while in the three dimensional separated flow, frequencies around a reduced frequency of 0.3 and 1 are active. Several scenarios of resonant wave interaction take place at the separated shear-layer and in the pressure recovery region. The unstable reduced frequency bands for periodic excitation are centered on 1.5 and 5, but these reduced frequencies are based on the length of the baseline bubble that shortens due to the excitation. The conventional swept wing-scaling works well for the coherent wave features. Reproduction of these dynamic effects by a numerical simulation would provide benchmark validation.

Pack, LaTunia G.↗