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NASA NTRS2023

Polarization Calibration Using Solar Radiation Background Signal Scattered from Dense Cirrus Clouds in the Visible and Ultraviolet Wavelength Regimes

In this presentation we describe the application of a previously developed technique that is now being used to correct the daytime polarization calibration of the CALIPSO lidar. The technique leverages the fact that the solar radiation background signals from dense cirrus clouds are largely unpolarized due to the internal multiple reflections within the non-spherical ice particles and the multiple scattering that occurs among these particles. Therefore, the ratio of polarization components of the cirrus background signals provides a good estimate for the polarization gain ratio (PGR) of the lidar. Using airborne backscatter lidar measurements, this technique was demonstrated to work well in the infrared regime. However, in the visible and ultraviolet regime, the molecular contribution is too large to be ignored, and thus corrections must be applied to account for the highly polarizing characteristics of the molecular scattering. Ignoring molecular scattering contributions can cause PGR errors of 2-3% at 532 nm, where the CALIPSO lidar makes its depolarization measurement. Because of the wavelength dependence of -4 of the molecular scattering, the PGR error can be even larger at the 355 nm wavelength that will be used by ESA’s EarthCARE lidar. To correct the molecular scattering contributions to the lidar received solar background signal, a look-up table has been created using a polarization-sensitive radiative transfer model. This presentation describes the theory and implementation of the molecular scattering correction.

Zhaoyan Liu↗

DOE OSTI2022

Reflective metasurfaces for broadband terahertz linear-to-circular polarization conversion and circular dichroism spectroscopy

Metasurface polarization convertors permit conversion of an input linear polarization to right- or left-handed circular polarization based on the orientation of the input linear polarization, over a broad bandwidth and with high efficiency. The reflected circular polarizations can be used to evaluate samples for circular dichroism. A THz time-domain detection provides a time domain terahertz signal that is Fourier transformed to produce a THz circular dichroism spectrum.

Chen, Hou-Tong↗

DOE OSTI2023

Design and Contruction of a Longitudinally Polarized Solid Nuclear Target for CLAS12

A new polarized nuclear target has been developed, constructed, and deployed at Jefferson Laboratory in Newport News, VA for use with the upgraded 12 GeV CEBAF (Continuous Electron Beam Accelerator Facility) accelerator and the Hall B CLAS12 (12 GeV CEBAF Large Acceptance Spectrometer) detector array. This ?APOLLO? (Ammonia PO-Larized LOngitudinally) target is a longitudinally polarized, solid ammonia, nuclear target which employs DNP (Dynamic Nuclear Polarization) to induce a net polarization in samples of protons (NH3) and deuterons (ND3) cooled to 1 K via helium evaporation, held in a 5 T polarizing field supplied by the CLAS12 spectrometer, and irradiated with 140 GHz microwave radiation. It was utilized in the RGC (Run Group C) experiment suite through a collaboration of the JLab Target Group, Old Dominion University, Christopher Newport University, the University of Virginia, and the CLAS Collaboration. RGC comprised six experiments which measured multiple spin-dependent observables across a wide kinematic phase space for use in nucleon spin studies. The dimensional constraints necessary for the incorporation of APOLLO into CLAS12, as well as the considerations necessary to utilize the CLAS12 solenoid, introduced unique challenges to the target design. This document presents the innovative solutions developed for these challenges including a novel material transport system, superconducting magnetic correction coils, and an all new bespoke NMR (Nuclear Magnetic Resonance) system. In addition to a detailed description of the complete target system and an initial report of the RGC experimental run, it will also present a study of Quark-Hadron Duality in the g1 spin structure function based on Hall B EG1b data and pQCD fits from the JAM (Jefferson Lab Angular Momentum) Collaboration.

Lagerquist, Victoria Lagerquist↗

DOE OSTI2026

A new cw-NMR Q-meter for dynamically polarized targets for particle physics

Polarized solid targets produced via Dynamic Nuclear Polarization rely on Continuous-Wave Nuclear Magnetism Resonance measurements to accurately determine the degree of polarization of bulk samples polarized to nearly 100%. Since the late 1970's phase sensitive detection methods have been utilized to observe the magnetization of a sample as a small change in inductance under RF excitation near the Larmor frequency of the nuclear species of interest, using a device known as a Q-meter. Liverpool Q-meters, produced in the UK in the 80's and 90's, have been the workhorse devices for these targets for decades, however their age and scarcity has meant new systems are needed. In conclusion, we describe a Q-meter system designed and built at Jefferson Lab in the Liverpool style to have comparable electronic performance with several improvements to update and adapt the devices for modern use.

Dynamic nuclear polarization↗

DOE OSTI2021

Global Λ-hyperon polarization in Au + Au collisions at $\sqrt{S_{NN}}$ = 3 GeV

Global hyperon polarization, $\overline{P}$ H , in Au + Au collisions over a large range of collision energy, $\sqrt{S_{NN}}$, was recently measured and successfully reproduced by hydrodynamic and transport models with intense fluid vorticity of the quark-gluon plasma. While na¨ıve extrapolation of data trends suggests a large $\overline{P}$ H as the collision energy is reduced, the behavior of $\overline{P}$ H at small $\sqrt{S_{NN}}$ < 7.7 GeV is unknown. Operating the STAR experiment in fixed-target mode, we measured the polarization of Λ hyperons along the direction of global angular momentum in Au + Au collisions at $\sqrt{S_{NN}}$ = 3 GeV. As a result, the observation of substantial polarization of 4.91 ± 0.81 (stat.) ± 0.15 (syst.) % in these collisions may require a reexamination of the viscosity of any fluid created in the collision, of the thermalization timescale of rotational modes, and of hadronic mechanisms to produce global polarization.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

A polarization-switch effect of silicon crystals under multiple-beam diffraction geometry

On the basis of rigorous dynamical-theory calculations, a complete X-ray polarization-switch effect of silicon crystals at the exact multiple-beam diffraction condition is demonstrated in this paper. The underlying physical mechanism of this unique phenomenon can be revealed using a simple multiple-wave propagation and interference model. The constructive and destructive interference of the multiple detoured-diffraction beams along the direction of the primary diffracted beam directly leads to the complete polarization switch. This phenomenon can be realized using both synchrotron and laboratory X-ray sources at many discrete wavelengths, and used to design a novel crystal-based polarizer to achieve a 90° polarization rotation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS2009

Continuous Lidar Monitoring of Polar Stratospheric Clouds at the South Pole

Polar stratospheric clouds (PSC) play a primary role in the formation of annual ozone holes over Antarctica during the austral sunrise. Meridional temperature gradients in the lower stratosphere and upper troposphere, caused by strong radiative cooling, induce a broad dynamic vortex centered near the South Pole that decouples and insulates the winter polar airmass. PSC nucleate and grow as vortex temperatures gradually fall below equilibrium saturation and frost points for ambient sulfate, nitrate, and water vapor concentrations (generally below 197 K). Cloud surfaces promote heterogeneous reactions that convert stable chlorine and bromine-based molecules into photochemically active ones. As spring nears, and the sun reappears and rises, photolysis decomposes these partitioned compounds into individual halogen atoms that react with and catalytically destroy thousands of ozone molecules before they are stochastically neutralized. Despite a generic understanding of the ozone hole paradigm, many key components of the system, such as cloud occurrence, phase, and composition; particle growth mechanisms; and denitrification of the lower stratosphere have yet to be fully resolved. Satellite-based observations have dramatically improved the ability to detect PSC and quantify seasonal polar chemical partitioning. However, coverage directly over the Antarctic plateau is limited by polar-orbiting tracks that rarely exceed 80 degrees S. In December 1999, a NASA Micropulse Lidar Network instrument (MPLNET) was first deployed to the NOAA Earth Systems Research Laboratory (ESRL) Atmospheric Research Observatory at the Amundsen-Scott South Pole Station for continuous cloud and aerosol profiling. MPLNET instruments are eye-safe, capable of full-time autonomous operation, and suitably rugged and compact to withstand long-term remote deployment. With only brief interruptions during the winters of 2001 and 2002, a nearly continuous data archive exists to the present.

OZONE DESTRUCTION↗

DOE OSTI2020

Large Polarization and Susceptibilities in Artificial Morphotropic Phase Boundary PbZr 1– x Ti x O 3 Superlattices

The ability to produce atomically precise, artificial oxide heterostructures allows for the possibility of producing exotic phases and enhanced susceptibilities not found in parent materials. Typical ferroelectric materials either exhibit large saturation polarization away from a phase boundary or large dielectric susceptibility near a phase boundary. Both large ferroelectric polarization and dielectric permittivity are attained wherein fully epitaxial (PbZr 0.8 Ti 0.2 O 3 ) n /(PbZr 0.4 Ti 0.6 O 3 ) 2 n ( n = 2, 4, 6, 8, 16 unit cells) superlattices are produced such that the overall film chemistry is at the morphotropic phase boundary, but constitutive layers are not. Here, long- ( n ≥ 6) and short-period ( n = 2) superlattices reveal large ferroelectric saturation polarization ( P s = 64 µC cm –2 ) and small dielectric permittivity (ε r ≈ 400 at 10 kHz). Intermediate-period ( n = 4) superlattices, however, exhibit both large ferroelectric saturation polarization ( P s = 64 µC cm –2 ) and dielectric permittivity (ε r = 776 at 10 kHz). First-order reversal curve analysis reveals the presence of switching distributions for each parent layer and a third, interfacial layer wherein superlattice periodicity modulates the volume fraction of each switching distribution and thus the overall material response. This reveals that deterministic creation of artificial superlattices is an effective pathway for designing materials with enhanced responses to applied bias.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Design of High Efficient Mid-Wavelength Infrared Polarizer on ORMOCHALC Polymer

While an organically modified chalcogenide (ORMOCHALC) can be used to fabricate a polymeric mid-wavelength infrared (MWIR) polarizer with competitive extinction ratio compared to the commercial wire-grid polarizers, which are composed of fragile inorganic materials, there is still a knowledge gap regarding the systematic design process to obtain high transmission efficiency and extinction ratio. As such, a computational parameter study for design optimization is conducted with the geometric parameters of the bilayer grating ORMOCHALC polarizer. The computational study shows that the Fabry–Pérot cavity is the primary mechanism that determines the transmission behaviors and the extinction ratio. A bilayer grating design, guided by the parameter study, is realized through the thermal nanoimprint and metal deposition processes. The extinction ratios measured with the Fourier-transform infrared are 245, 304, and 351 at the wavelength of 3, 4, and 5 μm, respectively. Compared to the state-of-the-art of the polymeric MWIR linear polarizers, the extinction ratio is improved by 1.4 times, and the transmission efficiency is increased by 2.5 times. Theoretical analysis with the multiple-layer model based on the transfer matrix method predicts a matched transmission behavior with the experiment and a full-wave electromagnetic simulation.

42 ENGINEERING↗

DOE OSTI2023

Insights into the relation between vertical cloud structure and dynamics of three polar lows: Observations from COMBLE

The vertical structure of three polar lows is described using profiling radar, lidar, and passive remote sensors deployed at a coastal site in northern Norway. The data were collected as part of the Cold-air Outbreaks in the Marine Boundary Layer Experiment (COMBLE). These data are examined in the context of satellite imagery, operational weather radar reflectivity imagery, and output from the AROME-Arctic model. A comparison to satellite images shows that AROME-Arctic captured the polar lows well. All three polar lows form in marine cold-air outbreaks and are surrounded by open-cellular convection typical of such outbreaks. Two of the lows form in a forward shear environment, and one under reverse shear. Initially, the three polar lows are comma-shaped; two of them transition to be more spirali-form at their mature stage and have mostly cloud-free warm cores. The warm cores are the result of a warm-seclusion process. All three lows have stratiform precipitation bands, marked by little cloud liquid water, and rather high surface precipitation rate. The vertical drafts and turbulence in these stratiform clouds are generally weak. In conclusion, all three lows also have convective clouds, which have stronger vertical drafts, stronger turbulence, and pockets of high liquid water content.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Effect of data assimilation in the Polar WRF with 3DVAR on the prediction of radiation, heat flux, cloud, and near surface atmospheric variables over Svalbard

Although the Polar Weather Research and Forecasting (PWRF) model has been developed for polar environments, simulations of atmospheric states in the polar region still have large uncertainties. Therefore, the effects of data assimilation (DA) to improve forecasts in the polar region were investigated for September 2017 using PWRF and the three-dimensional variational (3DVAR) DA method. The experiments without DA and those with DA assimilating only conventional observations and both conventional observations and satellite radiance data were performed. The forecasts from all experiments both without and with DA underestimated (overestimated) the downward longwave (shortwave) radiation flux due to the underestimation of the amount of Arctic clouds. When satellite radiance data (i.e., the Advanced Microwave Sounding Unit-A (AMSU-A) and Microwave Humidity Sounder (MHS)) were assimilated in addition to conventional observations in the PWRF, the distribution and amount of water vapor became closer to observations, which improves cloud liquid water forecasts. Therefore, when both conventional observations and radiance data were assimilated, the 25–30 h forecast errors of the downward longwave and shortwave radiation fluxes and sensible and latent heat fluxes decreased by 12.7%, 8.1%, 3.2%, and 7.8% with the WSM5 scheme and by 17.1%, 4.7%, 2.5%, and 3.1% with the 2-moment Morrison scheme, respectively, compared to those in the experiments without DA. The forecast errors of the 10 m wind and 2 m temperature with DA were smaller than those without DA at most observation stations. Therefore, the uncertainties of the Arctic forecasts in the PWRF decreased when using DA. To further improve Arctic forecasts, the assimilation of various additional satellite data is necessary.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Polarizing 3 He via metastability exchange optical pumping using a 1.2 mbar sealed cell at magnetic fields up to 5 T

Here, we report high nuclear polarization of 1.2 mbar 3 He gas in a sealed cell in magnetic fields up to 5 T using Metastability Exchange Optical Pumping (MEOP). The creation of a highly polarized 3 He gas target for use in the 5 T field of Jefferson Lab’s CLAS12 spectrometer would enable new studies of spin-dependent asymmetries on the neutron. We describe a systematic study which was conducted for the first time up to the full 5 T field required for the final target design to evaluate the effects of discharge intensity, pump laser power, and optical pumping transition schemes on nuclear polarization and pumping rates. Steady-state polarizations up to 86% in magnetic fields between 2 and 5 T were achieved, with a discharge-on relaxation time of 898 s at 5 T. These results underscore the potential of MEOP for high-field applications in nuclear physics experiments.

3He polarization↗

DOE OSTI2020

Dislocation-induced large local polarization inhomogeneity of ferroelectric materials

Dislocations in ferroelectrics play important roles in ferroelectricity, piezoelectricity, and dielectricity. However, the intrinsic charge-lattice coupling mechanism in ferroelectric crystals containing dislocations is still not well understood. Here, we report a large local polarization inhomogeneity of ~100 μCcm –2 induced by a single a[001] dislocation in the PbZr 0.2 Ti 0.8 O 3 /SrTiO 3 film/substrate heterostructure, the tensile region (~120 μCcm –2 ) and the compressive strain region (~21 μCcm –2 ) around the dislocation forms a butterfly-like area. Furthermore, this study reveals the dramatic effects of dislocations on local polarization and provides a strategy to manipulate the polarization magnitude and orientation of local polarization by defect engineering.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Assessing Implicit and Explicit Polarizable Solvation Models for Nuclear–Electronic Orbital Systems: Quantum Proton Polarization and Solvation Energetics

Accurate simulations of many chemical processes require the inclusion of both nuclear quantum effects and a solvent environment. The nuclear–electronic orbital (NEO) approach, which treats electrons and select nuclei quantum mechanically on the same level, combined with a polarizable continuum model (PCM) for the solvent environment, addresses this challenge in a computationally practical manner. In this work, the NEO-PCM approach is extended beyond the IEF-PCM (integral equation formalism PCM) and C-PCM (conductor PCM) approaches to the SS(V)PE (surface and simulation of volume polarization for electrostatics) and ddCOSMO (domain decomposed conductor-like screening model) approaches. IEF-PCM, SS(V)PE, C-PCM, and ddCOSMO all exhibit similar solvation energies as well as comparable nuclear polarization within the NEO framework. The calculations show that the nuclear density does not leak out of the molecular cavity because it is much more localized than the electronic density. Finally, the polarization of quantized protons is analyzed in both continuum solvent and explicit solvent environments described by the polarizable MB-pol model, illustrating the impact of specific hydrogen-bonding interactions captured only by explicit solvation. Furthermore, these calculations highlight the relationship among solvation formalism, nuclear polarization, and energetics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Mixed-Polarity Copolymers Based on Ethylene Oxide and Cyclic Carbonate: Insights into Li-Ion Solvation and Conductivity

Here, this study investigates the relationship between polarity and ionic conductivity in random and block copolymer electrolytes comprising highly flexible oligo(ethylene oxide) methyl ether methacrylate (OEM) and highly polar but glassy glycerol carbonate methacrylate (GCMA) monomers, blended with either lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) or lithium triflate. Interestingly, the high polarity of GCMA did not significantly enhance ionic dissociation, and the random copolymers (POEM-r-PGCMA) showed similar or lower ionic conductivities than the POEM homopolymer. Further analysis revealed that Li + only interacts with OEM and its counterion, not with GCMA. The less-intermixed and weakly phase-separated block copolymer (POEM-b-PGCMA) exhibited even lower conductivities than the random copolymer. Our results suggest that Li + solvation occurs only in the POEM-rich phase and that the larger PGCMA regions, depleted of Li + , disrupt long-range ion transport. These findings provide valuable insights into the design of polymer electrolytes and how segmental mobility and functional groups with contrasting polarities affect ion transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Triplet Photosensitized para -Hydrogen Induced Polarization

Despite its enormous utility in structural characterization, nuclear magnetic resonance (NMR) spectroscopy is inherently limited by low spin polarization. One method to address the low polarization is para-hydrogen (p-H 2 ) induced polarization (PHIP) which uses the singlet spin isomer of H 2 to generate disparate nuclear spin populations to amplify the associated NMR signals. PHIP often relies on thermal catalysis or, more infrequently, UV-activated catalytic hydrogenation. Light-activated hydrogenation enables direct and timed control over the hyperpolarization of target substrates, critical for identifying short-lived intermediates. Here, we use an established Ir(III) triplet photosensitizer (PS) to visible light sensitize the triplet ligand-field states in the d6-transition metal dihydride Ru(CO)(PPh 3 ) 3 (H) 2 (1). Excitation inside a 9.4 T NMR spectrometer with the PS and a 420 nm blue LED, under 3 atm of p-H 2 , successfully photosensitized hyperpolarization in 1 and in a range of unsaturated substrates at and below room temperature, up to 1630-fold. In otherwise identical experimental conditions without light activation, no polarization was realized in 1 or the substrates evaluated. We believe triplet-sensitized PHIP (Trip- PHIP) represents a facile experimental means for probing triplet sensitized light activation in transition metal catalysts possessing low-lying triplet ligand-field states, providing mechanistic insight of potentially tremendous value in chemical catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Performance Restoration of Iron Electrodes by Polarity Reversal after Long-Term Surface Fouling in Wastewater Electrocoagulation

Iron electrocoagulation (Fe-EC) performance often declines with time, producing lower contaminant removal efficiencies and higher energy requirements due to formation of a fouling layer on the electrodes. Here, we investigate the formation of the fouling layer and the effectiveness of polarity reversal to restore the Fe-EC performance. A thin, porous iron oxide layer initially forms on the anode, thickening into a dense, over 150-μm thick crystalline layer after extended operation. This fouling layer restricts dissolution and diffusion of Fe ions into the bulk solution, thus increasing the anode potential required to maintain a desired electrical current and decreasing Faradaic efficiency. Polarity reversal applied when performance decline is observed effectively removes the fouling layer, thereby restoring Faradaic and contaminant removal efficiencies and decreasing energy consumption. Our findings suggest that gas generation at the cathode surface after polarity reversal causes removal of the fouling layer. This study enhances the current understanding of fouling-layer formation in Fe-EC and offers a practical approach, involving polarity reversal, to maintain electrode reactivity and optimal Fe-EC performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Intercalation-Engineered Out-of-Plane Polarized van der Waals Ferromagnetic Superlattice with Room-Temperature Néel-Type Skyrmions

Superlattices (SLs) based on two-dimensional (2D) van der Waals (vdW) materials, abbreviated as 2D-SLs, have garnered significant attention due to their customizable properties. 2D-SLs can be engineered by mechanical stacking or chemical intercalation to achieve diverse forms of symmetry breaking, resulting in exotic phenomena like the quantum anomalous Hall effect and topological magnetism. Hitherto, broken symmetries in 2D-SLs have been widely produced within lateral planes or three dimensions. However, symmetry breaking along the vertical direction, specifically as an out-of-plane one-dimensional (1D) polarized superlattice, has not yet been achieved. Here, in this paper, we report a so far unseen out-of-plane 1D polarized vdW ferromagnetic superlattice achieved through an approach of two-step intercalation and de-embedding of chromium (Cr)-based 2D vdW magnets. The off-centering polarization of both intrinsic and intercalated Cr atoms in this (1 × 1 × 2) superstructure breaks the mirror symmetry vertically, yielding a Dzyaloshinskii–Moriya interaction (DMI). This results in high-density Néel-type magnetic skyrmions over a broad temperature range. Notably, sub-100 nm Néel-type skyrmions at room temperature (RT) can be achieved by tuning the Cr intercalation ratio, marking the first binary compound RT Néel-type skyrmionic vdW magnet. Our work expands the 2D-SL family with a class of out-of-plane 1D polarized ferromagnetic superlattice with tunable topological magnetism.

1D polarized superlattice↗