Results for “Diffuse Scattering” — Page 86

DOE OSTI2023

The anisotropic nature of singlet fission in single crystalline organic semiconductors

The escalating global energy predicament implores for a revolutionary resolution—one that converts sunlight into electricity—holding the key to supreme conversion efficiency. This comprehensive review embarks on the exploration of the principle of generating multiple excitons per absorbed photon, a captivating concept that possesses the potential to redefine the fundamental confines of conversion efficiency, albeit its application remains limited in photovoltaic devices. At the nucleus of this phenomenon are two principal processes: multiple exciton generation (MEG) within quantum-confined environments, and singlet fission (SF) inside molecular crystals. The process of SF, characterized by the cleavage of a single photogenerated singlet exciton into two triplet excitons, holds promise to potentially amplify photon-to-electron conversion efficiency twofold, thereby laying the groundwork to challenge the detailed balance limit of solar cell efficiency. Our discourse primarily dissects the complex nature of SF in crystalline organic semiconductors, laying special emphasis on the anisotropic behavior of SF and the diffusion of the subsequent triplet excitons in single-crystalline polyacene organic semiconductors. We initiate this journey of discovery by elucidating the principles of MEG and SF, tracing their historical genesis, and scrutinizing the anisotropy of SF and the impact of quantum decoherence within the purview of functional mode electron transfer theory. We present an overview of prominent techniques deployed in investigating anisotropic SF in organic semiconductors, including femtosecond transient absorption microscopy and imaging as well as stimulated Raman scattering microscopies, and highlight recent breakthroughs linked with the anisotropic dimensions of Davydov splitting, Herzberg–Teller effects, SF, and triplet transport operations in single-crystalline polyacenes. Through this comprehensive analysis, our objective is to interweave the fundamental principles of anisotropic SF and triplet transport with the current frontiers of scientific discovery, providing inspiration and facilitating future ventures to harness the anisotropic attributes of organic semiconductor crystals in the design of pioneering photovoltaic and photonic devices.

Chemistry↗

DOE OSTI2012

RESONANCE BROADENING AND HEATING OF CHARGED PARTICLES IN MAGNETOHYDRODYNAMIC TURBULENCE

The heating, acceleration, and pitch-angle scattering of charged particles by magnetohydrodynamic (MHD) turbulence are important in a wide range of astrophysical environments, including the solar wind, accreting black holes, and galaxy clusters. We simulate the interaction of high-gyrofrequency test particles with fully dynamical simulations of subsonic MHD turbulence, focusing on the parameter regime with {beta} {approx} 1, where {beta} is the ratio of gas to magnetic pressure. We use the simulation results to calibrate analytical expressions for test particle velocity-space diffusion coefficients and provide simple fits that can be used in other work. The test particle velocity diffusion in our simulations is due to a combination of two processes: interactions between particles and magnetic compressions in the turbulence (as in linear transit-time damping; TTD) and what we refer to as Fermi Type-B (FTB) interactions, in which charged particles moving on field lines may be thought of as beads sliding along moving wires. We show that test particle heating rates are consistent with a TTD resonance that is broadened according to a decorrelation prescription that is Gaussian in time (but inconsistent with Lorentzian broadening due to an exponential decorrelation function, a prescription widely used in the literature). TTD dominates the heating for v{sub s} >> v{sub A} (e.g., electrons), where v{sub s} is the thermal speed of species s and v{sub A} is the Alfven speed, while FTB dominates for v{sub s} << v{sub A} (e.g., minor ions). Proton heating rates for {beta} {approx} 1 are comparable to the turbulent cascade rate. Finally, we show that velocity diffusion of collisionless, large gyrofrequency particles due to large-scale MHD turbulence does not produce a power-law distribution function.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

Regioisomeric Spirobifluorene CANAL Ladder Polymers and Their Gas Separation Performance

For this work, we synthesized and characterized two isomeric microporous hydrocarbon ladder polymers from catalytic arene norbornene annulation (CANAL) of regioisomeric bis-norbornene fused spirobifluorenes, where the ladder chains are connected either through the same fluorene unit or across two different fluorene units in spirobifluorene. This pair of isomeric polymers was used to investigate the effect of ladder macromolecular structures on the microporosity and transport properties. Both polymers form mechanically intact films with thermal stability up to 480 °C and relatively high BET surface areas. The polymer formed from 2,7-dibromospirobifluorene showed higher BET surface area and higher gas permeability than the polymer from 2,2'-dibromospirobifluorene despite similar intersegmental spacing as indicated by X-ray scattering. The aging behavior for both polymers followed the same trend as the previously reported CANAL-fluorene polymers, with dramatically increased permselectivities over time, resulting in gas separation performance above the 2008 upper bounds for H 2 /CH 4 and O 2 /N 2 .

36 MATERIALS SCIENCE↗

DOE OSTI2012

sashevis (b1)

The shortwave array spectroradiometer—hemispheric (SASHE) uses a hemispheric spectralon diffuser and rotating shadowband similar to the MFRSR and RSS instruments, so it also provides spectrally resolved, direct-normal, diffuse-horizontal, and total-horizontal irradiances, and can be calibrated in situ via Langley regression. The SASHE incorporates two Avantes fiber-coupled spectroradiometers (Avaspec ULS 2048 CCD and Avaspec NIR256-1.7) for visible and near-infrared detection in the wavelength range 350-1700 nm. The spectral resolution is 2.4 nm for the ULS 2048 CCD and 6 nm for the NIR256-1.7. Like the SWS and SASZE, an external collector mounted outdoors is connected via fiber-optic cable to a pair of spectroradiometers housed indoors, so the entire spectral range is measured simultaneously for both spectroradiometers. For the typical shadowband measurement, the spectroradiometers are operated with one measurement per second, but the entire shadowband sequence takes about 20 seconds, so this is the measurement interval for the irradiances. The SASHE operating sequence is configurable and supports alternate programmed sequences as a function of solar zenith angle. For example, it currently employs different sequences for high sun angles, low sun angles, and twilight conditions when the sun is below the horizon but the sky is not yet fully dark. It also includes a mode where visible spectra are collected rapidly while the band is moved over a range of near-sun angles to characterize the forward-scattered radiation. The SASHE data are preliminarily calibrated through comparison with calibrated lamps. The accuracy of irradiance produced by the SASHE is expected to be better than ±5%, which includes calibration and instrument stability errors. Under suitably uniform atmospheric conditions, higher calibration accuracy and precisions (±1%) can be obtained when the responsivity is tied to the solar extraterrestrial irradiance via Langley regression plots. This approach is recommended when high-precision measurements of optical depth are required.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2012

sashemfr (b1)

The shortwave array spectroradiometer—hemispheric (SASHE) uses a hemispheric spectralon diffuser and rotating shadowband similar to the MFRSR and RSS instruments, so it also provides spectrally resolved, direct-normal, diffuse-horizontal, and total-horizontal irradiances, and can be calibrated in situ via Langley regression. The SASHE incorporates two Avantes fiber-coupled spectroradiometers (Avaspec ULS 2048 CCD and Avaspec NIR256-1.7) for visible and near-infrared detection in the wavelength range 350-1700 nm. The spectral resolution is 2.4 nm for the ULS 2048 CCD and 6 nm for the NIR256-1.7. Like the SWS and SASZE, an external collector mounted outdoors is connected via fiber-optic cable to a pair of spectroradiometers housed indoors, so the entire spectral range is measured simultaneously for both spectroradiometers. For the typical shadowband measurement, the spectroradiometers are operated with one measurement per second, but the entire shadowband sequence takes about 20 seconds, so this is the measurement interval for the irradiances. The SASHE operating sequence is configurable and supports alternate programmed sequences as a function of solar zenith angle. For example, it currently employs different sequences for high sun angles, low sun angles, and twilight conditions when the sun is below the horizon but the sky is not yet fully dark. It also includes a mode where visible spectra are collected rapidly while the band is moved over a range of near-sun angles to characterize the forward-scattered radiation. The SASHE data are preliminarily calibrated through comparison with calibrated lamps. The accuracy of irradiance produced by the SASHE is expected to be better than ±5%, which includes calibration and instrument stability errors. Under suitably uniform atmospheric conditions, higher calibration accuracy and precisions (±1%) can be obtained when the responsivity is tied to the solar extraterrestrial irradiance via Langley regression plots. This approach is recommended when high-precision measurements of optical depth are required.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2012

sashenir (b1)

The shortwave array spectroradiometer—hemispheric (SASHE) uses a hemispheric spectralon diffuser and rotating shadowband similar to the MFRSR and RSS instruments, so it also provides spectrally resolved, direct-normal, diffuse-horizontal, and total-horizontal irradiances, and can be calibrated in situ via Langley regression. The SASHE incorporates two Avantes fiber-coupled spectroradiometers (Avaspec ULS 2048 CCD and Avaspec NIR256-1.7) for visible and near-infrared detection in the wavelength range 350-1700 nm. The spectral resolution is 2.4 nm for the ULS 2048 CCD and 6 nm for the NIR256-1.7. Like the SWS and SASZE, an external collector mounted outdoors is connected via fiber-optic cable to a pair of spectroradiometers housed indoors, so the entire spectral range is measured simultaneously for both spectroradiometers. For the typical shadowband measurement, the spectroradiometers are operated with one measurement per second, but the entire shadowband sequence takes about 20 seconds, so this is the measurement interval for the irradiances. The SASHE operating sequence is configurable and supports alternate programmed sequences as a function of solar zenith angle. For example, it currently employs different sequences for high sun angles, low sun angles, and twilight conditions when the sun is below the horizon but the sky is not yet fully dark. It also includes a mode where visible spectra are collected rapidly while the band is moved over a range of near-sun angles to characterize the forward-scattered radiation. The SASHE data are preliminarily calibrated through comparison with calibrated lamps. The accuracy of irradiance produced by the SASHE is expected to be better than ±5%, which includes calibration and instrument stability errors. Under suitably uniform atmospheric conditions, higher calibration accuracy and precisions (±1%) can be obtained when the responsivity is tied to the solar extraterrestrial irradiance via Langley regression plots. This approach is recommended when high-precision measurements of optical depth are required.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Compton profile of VO 2 across the metal-insulator transition: Evidence of a non-Fermi liquid metal

Many-body diffusion Monte Carlo is used to obtain the first-principles momentum distribution and Compton profile of vanadium dioxide. Our results for the Compton profile are in good agreement with the experimental values, and we show that good qualitative agreement in the scaled Compton profile difference across the monoclinic to rutile phase transition depends on an accurate description of electron correlation. The electron momentum distribution enables new insights into the metal-insulator phase transition. For example, the probability for electron scattering in the proximity of the Fermi surface (forward scattering) is suppressed in the vanadium chain direction (rutile c axis) but enhanced in perpendicular directions. However, along the c axis we observe an increase at ~2k F in the momentum distribution, which is characteristic for Friedel oscillations (backscattering). Our analysis of the momentum distribution supports experimentally observed anisotropies and provides an explanation for the anomalously low electronic thermal conductivity observed recently in the metallic phase. Furthermore, our results indicate non-Fermi liquid behavior as well as quasi-one-dimensional Friedel oscillations in the metallic rutile phase, which is reminiscent of a Tomanaga-Luttinger liquid with impurities.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Control-Affine Schrödinger Bridge and Generalized Bohm Potential

From a stochastic control perspective, the Schrödinger bridge is a density-valued continuous curve parameterized by time that connects a given pair of initial and terminal probability densities via minimum effort controlled Brownian motion. The control-affine Schrödinger bridge extends this idea to a generic control-affine Itô diffusion, possibly with an additive state cost. Here, in this letter, we recast the necessary conditions of optimality for the control-affine Schrödinger bridge problem as a two point boundary value problem for a quantum mechanical Schrödinger PDE with complex potential. This complex-valued potential is a generalization of the real-valued Bohm potential in quantum mechanics. Our derived potential is akin to the optical potential in nuclear physics where the real part of the potential encodes elastic scattering (transmission of wave function), and the imaginary part encodes inelastic scattering (absorption of wave function). The key takeaway is that the process noise that drives the evolution of probability densities induces an absorbing medium in the evolution of wave function. These results make new connections between control theory and non-equilibrium statistical mechanics through the lens of quantum mechanics.

Markov processes↗

DOE OSTI2015

SU-D-210-03: Limited-View Multi-Source Quantitative Photoacoustic Tomography

Purpose: This work is to investigate a novel limited-view multi-source acquisition scheme for the direct and simultaneous reconstruction of optical coefficients in quantitative photoacoustic tomography (QPAT), which has potentially improved signal-to-noise ratio and reduced data acquisition time. Methods: Conventional QPAT is often considered in two steps: first to reconstruct the initial acoustic pressure from the full-view ultrasonic data after each optical illumination, and then to quantitatively reconstruct optical coefficients (e.g., absorption and scattering coefficients) from the initial acoustic pressure, using multi-source or multi-wavelength scheme.Based on a novel limited-view multi-source scheme here, We have to consider the direct reconstruction of optical coefficients from the ultrasonic data, since the initial acoustic pressure can no longer be reconstructed as an intermediate variable due to the incomplete acoustic data in the proposed limited-view scheme. In this work, based on a coupled photo-acoustic forward model combining diffusion approximation and wave equation, we develop a limited-memory Quasi-Newton method (LBFGS) for image reconstruction that utilizes the adjoint forward problem for fast computation of gradients. Furthermore, the tensor framelet sparsity is utilized to improve the image reconstruction which is solved by Alternative Direction Method of Multipliers (ADMM). Results: The simulation was performed on a modified Shepp-Logan phantom to validate the feasibility of the proposed limited-view scheme and its corresponding image reconstruction algorithms. Conclusion: A limited-view multi-source QPAT scheme is proposed, i.e., the partial-view acoustic data acquisition accompanying each optical illumination, and then the simultaneous rotations of both optical sources and ultrasonic detectors for next optical illumination. Moreover, LBFGS and ADMM algorithms are developed for the direct reconstruction of optical coefficients from the acoustic data. Jing Feng and Hao Gao were partially supported by the NSFC (#11405105), the 973 Program (#2015CB856000) and the Shanghai Pujiang Talent Program (#14PJ1404500)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2018

Method of solar power prediction

Techniques for estimating direct and diffuse sunlight reaching a location as a function of time using color whole sky images are provided. In one aspect, a method for forecasting solar insolation is provided that includes the steps of: obtaining color whole sky images using a digital camera which are taken at different times, and wherein an image of a solar disk is present in at least one of the color whole sky images; creating sky transparency images from the color whole sky images; determining atmospheric solar scattering based on a width of the solar disk in the color whole sky images; determining cloud motion trajectories from a time series of the sky transparency images; and calculating the solar insolation as a function of time using the sky transparency, the atmospheric solar scattering, and the cloud motion trajectories. A system for forecasting solar insolation is also provided.

Hamann, Hendrik F.↗

DOE OSTI2021

Analysis of the EMCCD point-source response using x-rays

Electron Multiplying Charge Coupled Devices, EMCCD are used as x-ray detectors. The NSLS-II Soft Inelastic x-ray Scattering (SIX) beam line has two EMCCDs for x-ray detection in the spectrometer arm. The spectrometer with high resolving power disperses x-rays vertically. The x-ray vertical position on the sensor plane is related to its energy. This allows for very accurate x-ray energy measurements through x-ray coordinates. X-rays interact with silicon and create a number of electron-hole pairs proportional to the x-ray energy. Electrons drift and diffuse toward pixel gates and are collected there. The diffused electrons form a charge cloud distributed over several neighboring pixels. This charge sharing enables coordinate measurements with accuracy better than the pixel pitch. The charge distribution shape has to be taken into account to achieve ultimate accuracy in coordinate measurements. In this paper, we present a method of the charge distribution shape analysis and demonstrate its applications. The drift and diffusion of electrons ftom the point of generation to pixel gates results in the bell-shaped electron cloud usually approximated by Gaussian shape. The number of electrons collected under a pixel is proportional to the shape function integral. These electron packets get transferred to the sense node of the output amplifier. The transfer process could introduce distortions to the original charge distribution. For example, during transfers, electrons in the packet could be exposed to traps if they are present in the sensor. The trapping and later the release processes distort the apparent shape of the charge distribution. Therefore, deviations of the charge distribution shape ftom the originally symmetrical form can indicate the presence of trap centers in the sensor and can be used for sensor diagnostics.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Exciton Coherence Length and Dynamics in Graphene Quantum Dot Assemblies

Abstract not provided

Singh, Varun↗

DOE OSTI2017

Dynamics of water bound to crystalline cellulose

Interactions of water with cellulose are of both fundamental and technological importance. Here, we characterize the properties of water associated with cellulose using deuterium labeling, neutron scattering and molecular dynamics simulation. Quasi-elastic neutron scattering provided quantitative details about the dynamical relaxation processes that occur and was supported by structural characterization using small-angle neutron scattering and X-ray diffraction. We can unambiguously detect two populations of water associated with cellulose. The first is “non-freezing bound” water that gradually becomes mobile with increasing temperature and can be related to surface water. The second population is consistent with confined water that abruptly becomes mobile at ~260 K, and can be attributed to water that accumulates in the narrow spaces between the microfibrils. Quantitative analysis of the QENS data showed that, at 250 K, the water diffusion coefficient was 0.85 ± 0.04 × 10-10 m2sec-1 and increased to 1.77 ± 0.09 × 10-10 m2sec-1 at 265 K. MD simulations are in excellent agreement with the experiments and support the interpretation that water associated with cellulose exists in two dynamical populations. Our results provide clarity to previous work investigating the states of bound water and provide a new approach for probing water interactions with lignocellulose materials.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

BEBOP II: sensitivity to sub-Saturn circumbinary planets using radial-velocities

ABSTRACT BEBOP is a radial-velocity survey that monitors a sample of single-lined eclipsing binaries, in search of circumbinary planets by using high-resolution spectrographs. Here, we describe and test the methods we use to identify planetary signals within the BEBOP data and establish how we quantify our sensitivity to circumbinary planets by producing detection limits. This process is made easier and more robust by using a diffusive nested sampler. In the process of testing our methods, we notice that contrary to popular wisdom, assuming circular orbits in calculating detection limits for a radial-velocity survey provides overoptimistic detection limits by up to $40{{\ \rm per\ cent}}$ in semi-amplitude with implications for all radial-velocity surveys. We perform example analyses using three BEBOP targets from our Southern HARPS survey. We demonstrate for the first time a repeated ability to reach a residual root mean squared scatter of $3\, \rm m\, s^{-1}$ (after removing the binary signal), and find that we are sensitive to circumbinary planets with masses down to that of Neptune and Saturn, for orbital periods up to $1000\, \rm d$.

Standing, Matthew R. (ORCID:0000000276088905)↗

DOE OSTI2020

Generalized magnetoelectronic circuit theory and spin relaxation at interfaces in magnetic multilayers

Spin transport at metallic interfaces is an essential ingredient of various spintronic device concepts, such as giant magnetoresistance, spin-transfer torque, and spin pumping. Spin-orbit coupling plays an important role in many such devices. In particular, spin current is partially absorbed at the interface due to spin-orbit coupling. Here, we develop a general magnetoelectronic circuit theory and generalize the concept of spin-mixing conductance, accounting for various mechanisms responsible for spin-flip scattering. For the special case when exchange interactions dominate, we give a simple expression for the spin-mixing conductance in terms of the contributions responsible for spin relaxation (i.e., spin memory loss), spin torque, and spin precession. The spin memory loss parameter d is related to spin-flip transmission and reflection probabilities. There is no straightforward relation between spin torque and spin memory loss. We calculate the spin-flip scattering rates for N|N, F|N, and F|F interfaces using the Landauer-Büttiker method within the linear muffin-tin orbital method and determine the values of d using circuit theory.

36 MATERIALS SCIENCE↗

DOE OSTI2012

On the late-time growth of the two-dimensional Richtmyer–Meshkov instability in shock tube experiments [On the late-time growth of the 2D Richtmyer–Meshkov instability in shock tube experiments]

In the present study, shock tube experiments are used to study the very late-time development of the Richtmyer–Meshkov instability from a diffuse, nearly sinusoidal, initial perturbation into a fully turbulent flow. The interface is generated by two opposing gas flows and a perturbation is formed on the interface by transversely oscillating the shock tube to create a standing wave. The puncturing of a diaphragm generates a Mach $1. 2$ shock wave that then impacts a density gradient composed of air and SF 6 , causing the Richtmyer–Meshkov instability to develop in the 2.0 m long test section. The instability is visualized with planar Mie scattering in which smoke particles in the air are illuminated by a Nd:YLF laser sheet, and images are recorded using four high-speed video cameras operating at 6 kHz that allow the recording of the time history of the instability. In addition, particle image velocimetry (PIV) is implemented using a double-pulsed Nd:YAG laser with images recorded using a single CCD camera. Initial modal content, amplitude, and growth rates are reported from the Mie scattering experiments while vorticity and circulation measurements are made using PIV. Amplitude measurements show good early-time agreement but relatively poor late-time agreement with existing nonlinear models. The model of Goncharov agrees with growth rate measurements at intermediate times but fails at late experimental times. Measured background acceleration present in the experiment suggests that the late-time growth rate may be influenced by Rayleigh–Taylor instability induced by the interfacial acceleration. Numerical simulations conducted using the LLNL codes Ares and Miranda show that this acceleration may be caused by the growth of boundary layers, and must be accounted for to produce good agreement with models and simulations. Adding acceleration to the Richtmyer–Meshkov buoyancy–drag model produces improved agreement. It is found that the growth rate and amplitude trends are also modelled well by the Likhachev–Jacobs vortex model. Here, circulation measurements also show good agreement with the circulation value extracted by fitting the vortex model to the experimental data.

42 ENGINEERING↗

DOE OSTI2018

Spin diffusion length and spin Hall angle in Pd 1– x Pt x /YIG heterostructures: Examination of spin relaxation mechanism

The thickness, temperature, and composition studies of spin diffusion length (SDL) and spin Hall angle (SHA) are performed by measuring the spin Hall magnetoresistance in Pd 1–x Pt x /Y 3 Fe 5 O 12 (=YIG) heterostructures. The SDL is found to be invariant to changes in the electron momentum relaxation time by varying the temperature, the normal metal (NM) thickness, or the alloy composition, while the SHA exhibits a nonmonotonic dependence on temperature. These findings suggest the appearance of D'yakonov-Perel' spin relaxation mechanism and phonon skew scattering in our heterostructures that is associated with strong interfacial Rashba spin-orbit coupling (IRSOC). At last, we employ the ab initio calculations to quantify the IRSOC at the inversion-symmetry-broken NM/YIG interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2018

Photoluminescence and gain/absorption spectra of a driven-dissipative electron-hole-photon condensate

Here, we investigate theoretically nonequilibrium effects on photoluminescence and gain/absorption spectra of a driven-dissipative exciton-polariton condensate, by employing the combined Hartree-Fock-Bogoliubov theory with the generalized random phase approximation extended to the Keldysh formalism. Our calculated photoluminescence spectra is in semiquantitative agreement with experiments, where features such as a blue shift of the emission from the condensate, the appearance of the dispersionless feature of a diffusive Goldstone mode, and the suppression of the dispersive profile of the mode are obtained. We show that the nonequilibrium nature of the exciton-polariton condensate strongly suppresses the visibility of the Bogoliubov dispersion in the negative energy branch (ghost branch) in photoluminescence spectra. We also show that the trace of this branch can be captured as a hole burning effect in gain/absorption spectra. Our results indicate that the nonequilibrium nature of the exciton-polariton condensate strongly reduces quantum depletion, while a scattering channel to the ghost branch is still present.

74 ATOMIC AND MOLECULAR PHYSICS↗