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DOE OSTI2023

BeyondPlanck: XV. Limits on large-scale polarized anomalous microwave emission from Planck LFI and WMAP

We constrained the level of polarized anomalous microwave emission (AME) on large angular scales using Planck Low-Frequency Instrument (LFI) and WMAP polarization data within a Bayesian cosmic microwave background (CMB) analysis framework. We modeled synchrotron emission with a power-law spectral energy distribution, as well as the sum of AME and thermal dust emission through linear regression with the Planck High-Frequency Instrument (HFI) 353 GHz data. This template-based dust emission model allowed us to constrain the level of polarized AME while making minimal assumptions on its frequency dependence. We neglected CMB fluctuations, but show through simulations that these fluctuations have a minor impact on the results. We find that the resulting AME polarization fraction confidence limit is sensitive to the polarized synchrotron spectral index prior. In addition, for prior means β s < -3.1 we find an upper limit of p AME max ≲ 0.6% (95% confidence). In contrast, for means β s = -3.0, we find a nominal detection of p AME = 2.5 ± 1.0% (95% confidence). These data are thus not strong enough to simultaneously and robustly constrain both polarized synchrotron emission and AME, and our main result is therefore a constraint on the AME polarization fraction explicitly as a function of β s . Combining the current Planck and WMAP observations with measurements from high-sensitivity low-frequency experiments such as C-BASS and QUIJOTE will be critical to improve these limits further.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Negatively Charged Excitons in CdSe Nanoplatelets

The low-temperature emission spectrum of CdSe colloidal nanoplatelets (NPLs) consists of two narrow lines. The high-energy line stems from the recombination of neutral excitons. The origin of the low-energy line is currently debated. Here, we experimentally study the spectral shift, emission dynamics, and spin polarization of both lines at low temperatures down to 1.5 K and in high magnetic fields up to 60 T and show that the low-energy line originates from the recombination of negatively charged excitons (trions). This assignment is confirmed by the NPL photocharging dynamics and associated variations in the spectrum. We show that the negatively charged excitons are considerably less sensitive to the presence of surface spins than the neutral excitons. The trion binding energy in three-monolayer-thick NPLs is as large as 30 meV, which is 4 times larger than its value in the two-dimensional limit of a conventional CdSe quantum well confined between semiconductor barriers. A considerable part of this enhancement is gained by the dielectric enhancement effect, which is due to the small dielectric constant of the environment surrounding the NPLs.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2025

Selective concentration of multivalent cations via electrodialysis through tandem membranes

Selective electrodialysis is attractive for recovering and recycling valuable ions. However, most studies in this field focus on membranes that are selective for monovalent ions. Multivalent cations preferentially partition into cation-exchange membranes, but low mobilities and concentration polarization limit electrodialysis selectivities for these cations. This work employs electrodialysis through an “in-series” combination of a Nafion membrane and a multilayer polyelectrolyte film (MPF)-coated Nafion membrane to concentrate and isolate La 3+ or Mg 2+ from monovalent ions. The bare Nafion membrane gives a La 3+ /Na + selectivity up to 4 (depending on conditions), which enables concentration of La 3+ with a high current efficiency. The MPF-coated membrane allows selective passage of Na + while rejecting La 3+ to increase the purity of the concentrated multivalent cation. For example, the concentration of La 3+ in the accumulation solution can reach 9 times its original concentration in the feed solution with a purity of 93 mol% (99 wt%) when starting with equimolar mixtures of NaNO 3 and La(NO 3 ) 3 . This study examines how the separation varies with the type of polyelectrolyte, the applied voltage, and the composition of feed, accumulation, and cathode solutions. Here, a high nitric acid concentration (0.5 M) in the cathode compartment allows monovalent anions to pass through the MPF-coated Nafion membrane to maintain the electroneutrality of the accumulation solution. With a low acid concentration (0.04 M) in the cathode chamber, water splitting occurs at the MPF-coated membrane and La(OH) 3 precipitates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

MIRC-X: A Highly Sensitive Six-telescope Interferometric Imager at the CHARA Array

Michigan InfraRed Combiner-eXeter (MIRC-X) is a new highly sensitive six-telescope interferometric imager installed at the CHARA Array that provides an angular resolution equivalent of up to a 330 m diameter baseline telescope in J- and H-band wavelengths ((λ/(2B))∼0.6 mas). We upgraded the original Michigan InfraRed Combiner (MIRC) instrument to improve sensitivity and wavelength coverage in two phases. First, a revolutionary sub-electron noise and fast-frame-rate C-RED ONE camera based on an SAPHIRA detector was installed. Second, a new-generation beam combiner was designed and commissioned to (i) maximize sensitivity, (ii) extend the wavelength coverage to J band, and (iii) enable polarization observations. A low-latency and fast-frame-rate control software enables high-efficiency observations and fringe tracking for the forthcoming instruments of the CHARA Array. Since mid-2017, MIRC-X has been offered to the community and has demonstrated best-case H-band sensitivity down to 8.2 correlated magnitude. MIRC-X uses single-mode fibers to coherently combine the light from six telescopes simultaneously with an image-plane combination scheme and delivers a visibility precision better than 1%, and closure phase precision better than 1°. MIRC-X aims at (i) imaging protoplanetary disks, (ii) detecting exoplanets with precise astrometry, and (iii) imaging stellar surfaces and starspots at an unprecedented angular resolution in the near-infrared. In this paper, we present the instrument design, installation, operation, and on-sky results, and demonstrate the imaging capability of MIRC-X on the binary system ι Peg. The purpose of this paper is to provide a solid reference for studies based on MIRC-X data and to inspire future instruments in optical interferometry.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Investigation of startup, performance and cycling of a residential furnace integrated with micro-tubular flame-assisted fuel cells for micro-combined heat and power

Solid Oxide Fuel Cells (SOFCs) offer advantages for micro-Combined Heat and Power (μCHP), but currently suffer from slow startup (>1 h) and limited thermal cycling which reduces the applications, energy savings and economics. In this work, a micro-Tubular SOFC stack is integrated into a residential furnace to create a micro-Tubular Flame-assisted Fuel Cell (mT-FFC) μCHP system. A high power density of 202 mW cm -2 is reported operating in synthesis gas generated from fuel-rich combustion of natural gas/air. Unlike previous reports, instabilities in the polarization are attributed to low temperature of the oxygen reduction reaction at the cathode. The mT-FFC stack achieved peak power density in 6 min after ignition. 200 thermal cycles at an average heating rate of 215 °C.min -1 and average cooling rate of 176 °C.min -1 were conducted and a low degradation rate of 0.0325 V per 100 cycles per fuel cell was achieved. Low NO x emissions (10 ppm) and high combined efficiency is reported.

25 ENERGY STORAGE↗

DOE OSTI2021

A naphthalene diimide side-chain polymer as an electron-extraction layer for stable perovskite solar cells

Poly(N-(5-(5-norbornene-2-carbonyl)oxy)pentyl)-N'-n-hexyl-naphthalene-1,8:4,5-bis(dicarboximide) has been synthesized by esterification of (N-(5-hydroxypentyl)-N'-n-hexyl-naphthalene-1,8:4,5-bis(dicarboximide)) with exo-5-norbornene-2-carboxylic acid, and has been polymerized using the first-generation Grubbs initiator. This side-chain polymer exhibits good transparency throughout the visible (absorption onset at ca. 400 nm), good solubility in common low- and medium-polarity organic solvents, good resistance to dimethylformamide, and appropriate electron affinity for use as an electron-extraction layer in lead-halide perovskite solar cells. The performance of this polymer in n-i-p perovskite solar cells was compared to that of several small-molecule naphthalene-1,8:4,5-bis(dicarboximide) derivatives and of SnO 2 . Solar cells using the polymer exhibited open-circuit voltages of up to 1.02 V, short-circuit currents of over 21 mA cm –2 , and power conversion efficiencies (PCE) reaching 14% which stabilize at 13.8% upon 90 s of illumination. Meanwhile control SnO 2 devices exhibited a PCE of ca. 16%, and small-molecule devices gave PCE values of less than 10%. Here, the devices employing the polymer exhibited improved long-term stability relative to the SnO 2 control devices under continuous illumination.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Preferred Spin Excitations in the Bilayer Iron-Based Superconductor $CaK(Fe_{0.96}Ni_{0.04})_4As_4$ with Spin-Vortex Crystal Order

Spin-orbit coupling (SOC) is a key to understand the magnetically driven superconductivity in iron-based superconductors, where both local and itinerant electrons are present and the orbital angular momentum is not completely quenched. Here, we report a neutron scattering study on the bilayer compound CaK(Fe 0.96 Ni 0.04 ) 4 As 4 with superconductivity coexisting with a noncollinear spin-vortex crystal magnetic order that preserves the tetragonal symmetry of the Fe-Fe plane. In the superconducting state, two spin resonance modes with odd and even L symmetries due to the bilayer coupling are found similar to the undoped compound CaKFe 4 As 4 but at lower energies. Polarization analysis reveals that the odd mode is c-axis polarized, and the low-energy spin anisotropy can persist to the paramagnetic phase at high temperature, which closely resembles other systems with in-plane collinear and c-axis biaxial magnetic orders. Overall, these results provide the missing piece of the puzzle on the SOC effect in iron-pnictide superconductors, and also establish a common picture of c-axis preferred magnetic excitations below T c regardless of the details of magnetic pattern or lattice symmetry.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Optimal filtering and generation of entangled photons for quantum applications in the presence of noise

Filtering is commonly used in quantum optics to reject noise photons, and also to enable interference between independent photons. However, filtering the joint spectrum of photon pairs can reduce the inherent coincidence probability or loss-independent heralding efficiency. Here we investigate filtering for multiphoton applications based on entanglement and interference (e.g., quantum teleportation). We multiplex C-band entangled photons and C-band classical communications into the same long-distance fibers, which enables scalable low-loss quantum networking but requires filtering of spontaneous Raman scattering noise from classical light. Using tunable-bandwidth filters, low-jitter detectors, and polarization filters, we distribute wavelength-degenerate time-bin entangled photons in the C band (1536.5 nm) over 25 km/25 km standard fibers (50 km) each carrying 10 Gbit/s C-band classical data signals. Narrow filtering enables milliwatt-level C-band power, which exceeds the power achieved by comparable studies by roughly an order of magnitude and could feasibly support terabit per second classical rates. We evaluate how performance depends on pump and filter bandwidths, multipair emission, filter shapes, loss, phase matching, and how quantum information is measured. We find a trade-off between reducing noise impact and increasing single-mode purity, and discuss mitigation methods toward optimal multiphoton applications. Importantly, these results apply to noise in free space and in quantum devices (sources, frequency converters, switches, detectors, etc.) and provide insight into filter-induced degradation of single-photon purity and rates even in noise-free environments.

Thomas, Jordan M. [Fermilab; Northwestern U.]↗

DOE OSTI2022

On the Feasibility of 1T Ferroelectric FET Memory Array

To fully exploit the ferroelectric field effect transistor (FeFET) as compact embedded nonvolatile memory for various computing and storage applications, it is desirable to use a single FeFET (1T) as a unit cell and arrange the cells into an array. However, many write mechanisms for an 1T FeFET array reported in the literature are yet to be validated experimentally. In this work, we performed a comprehensive experimental characterization on the write operations in an 1T- NOR and 1T- AND array using n-channel bulk FeFETs. We discovered that: 1) the source/drain contact can only supply minority carriers (i.e., electrons) to the channel for polarization screening during the low- V TH state programming; 2) the body contact can not only supply majority carriers (i.e., holes) for efficient high- V TH state write, but also depletion charge for low- V TH state programming, though with lower efficiency; and 3) during the low/high- V TH programming, only the path that can supply negative/positive screening charges, respectively, need to respond, which necessitates the application of proper write biases on the corresponding terminal. Based on the understanding of these write mechanisms, we show the importance of localized body contact or column-wise body contact for the successful high- V TH state programming. We also show that the previously proposed C- AND write scheme fails to program the FeFET to the low- V TH state for our devices. Finally, we propose several write schemes for both 1T- AND and 1T- NOR arrays for various scenarios providing insights for choosing the appropriate write scheme, which will facilitate the adoption of 1T FeFET memory arrays for emerging applications.

FeFET↗

DOE OSTI2020

Plasmonic gold-cellulose nanofiber aerogels

Assembly of plasmonic nanomaterials into a low refractive index medium, such as an aerogel, holds a great promise for optical metamaterials, optical sensors, and photothermal energy converters. However, conventional plasmonic aerogels are opaque and optically isotropic composites, impeding them from being used as low-loss or polarization-dependent optical materials. Here we demonstrate a plasmonic-cellulose nanofiber composite aerogel that comprises of well-dispersed gold nanorods within a cellulose nanofiber network. The cellulose aerogel host is highly transparent owing to the small scattering cross-section of the nanofibers and forms a nematic liquid crystalline medium with strong optical birefringence. We find that the longitudinal surface plasmon resonance peak of gold nanorods shows a dramatic shift when probed for the cellulose aerogel compared with the wet gels. Simulations reveal the shift of surface plasmon resonance peak with gel drying can be attributed to the change of the effective refractive index of the gels. This composite material may provide a platform for three- dimensional plasmonic devices ranging from optical sensors to metamaterials.

36 MATERIALS SCIENCE↗

DOE OSTI2021

32 Gbps heterogeneously integrated quantum dot waveguide avalanche photodiodes on silicon

We report a heterogeneous GaAs-based quantum dot (QD) avalanche photodiode (APD) on silicon with an ultralow dark current of 10 pA at − <#comment/> 1 V , 3 dB bandwidth of 20 GHz and record gain-bandwidth product (GBP) of 585 GHz. Furthermore, open eye diagrams up to 32 Gb/s are demonstrated at 1310 nm. The k-factor has been measured for these devices to be as low as 0.14. A polarization dependence on gain and bandwidth has been observed and investigated. This shows the potential to integrate a high-speed receiver in a wavelength division multiplexing (WDM) system on a QD-based silicon photonics platform.

Tossoun, Bassem↗

DOE OSTI2022

Measuring the Electric Dipole Moment of the Electron in a Two-Energy Spin-Transparent Storage Ring

We will present a new design of a two-energy storage ring for low energy (0.2 to 2 MeV) polarized electron bunches [1]. The new design is based on the transparent spin methodology that cancels the spin precession due to the magnetic dipole moment at any energy while allowing for spin precession induced by the fundamental physics of interest to accumulate. The buildup of the vertical component of beam polarization can be measured using standard Mott polarimetry that is optimal at low electron energy. These rings can be used to measure the permanent electric dipole moment of the electron, relevant to CP violation and matter-antimatter asymmetry in the universe, and to search for dark energy and ultra-light dark matter.

Suleiman, R.↗

DOE OSTI2022

Measuring the Electric Dipole Moment of the Electron in a Two-Energy Spin-Transparent Storage Ring

Suleiman, R.↗

DOE OSTI2021

Ferroelectric Self-Polarization Controlled Magnetic Stratification and Magnetic Coupling in Ultrathin La 0.67 Sr 0.33 MnO 3 Films

Multiferroic oxide heterostructures consisting of ferromagnetic and ferroelectric components hold the promise for nonvolatile magnetic control via ferroelectric polarization, advantageous for the low-dissipation spintronics. Modern understanding of the magnetoelectric coupling in these systems involves structural, orbital, and magnetic reconstructions at interfaces. Previous works have long proposed polarization-dependent interfacial magnetic structures; however, direct evidence is still missing, which requires advanced characterization tools with near-atomic-scale spatial resolutions. Here, extensive polarized neutron reflectometry (PNR) studies have determined the magnetic depth profiles of PbZr 0.2 Ti 0.8 O 3 /La 0.67 Sr 0.33 MnO 3 (PZT/LSMO) bilayers with opposite self-polarizations. When the LSMO is 2–3 nm thick, the bilayers show two magnetic transitions on cooling. However, temperature-dependent magnetization is different below the lower-temperature transition for opposite polarizations. PNR finds that the LSMO splits into two magnetic sublayers, but the inter-sublayer magnetic couplings are of opposite signs for the two polarizations. Near-edge X-ray absorption spectroscopy further shows contrasts in both the Mn valences and the Mn–O bond anisotropy between the two polarizations. Finally, this work completes the puzzle for the magnetoelectric coupling model at the PZT/LSMO interface, showing a synergic interplay among multiple degrees of freedom toward emergent functionalities at complex oxide interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Born effective charges and electric polarization in bulk ε-Fe 2 O 3 : An ab-initio approach

Limitation in the synthesis of single-crystal has restricted the complete understanding of the magnetoelectric properties of bulk ε-Fe 2 O 3 . In order to understand the electric polarization of bulk ε-Fe 2 O 3 , we have employed a first-principles Berry-phase method and the density functional perturbation theory to calculate the spontaneous electric polarization and Born effective charges (BECs) of ε-Fe 2 O 3 . The polarization quanta of the ferroelectric bulk ε-Fe 2 O 3 and its polarization lattice are also reported. The polarization switching through a paraelectric transition phase of a low barrier is found to be favorable. The polarization and BECs calculated by both methods are in good agreement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Sn-modified BaTiO 3 thin film with enhanced polarization

Hybrid molecular beam epitaxy (MBE) growth of Sn-modified BaTiO 3 films was realized with varying domain structures and crystal symmetries across the entire composition space. Macroscopic and microscopic structures and the crystal symmetry of these thin films were determined using a combination of optical second harmonic generation (SHG) polarimetry and scanning transmission electron microscopy (STEM). SHG polarimetry revealed a variation in the global crystal symmetry of the films from tetragonal (P4mm) to cubic (PM3¯m) across the composition range, x = 0 to 1 in BaTi 1–x Sn x O 3 (BTSO). STEM imaging shows that the long-range polar order observed when the Sn content is low (x = 0.09) transformed to a short-range polar order as the Sn content increased (x = 0.48). Consistent with atomic displacement measurements from STEM, the largest polarization was obtained at the lowest Sn content of x = 0.09 in Sn-modified BaTiO 3 as determined by SHG. Furthermore, these results agree with recent bulk ceramic reports and further identify this material system as a potential replacement for Pb-containing relaxor-based thin film devices.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Room temperature multiferroicity and magnetodielectric coupling in 0–3 composite thin films

Magnetoelectric (ME) composite thin films are promising candidates for novel applications in future nanoelectronics, spintronics, memory and other multifunctional devices as they exhibit much higher ME coupling and transition temperatures (Tc) than well-known single phase multiferroics discovered to date. Among the three types of multiferroic composite nanostructures, (2-2) layered and (1-3) vertically aligned composite nanostructures exhibit comparatively smaller ME coupling due to different shortcomings which restrict their use in many applications. Here we study the morphological, piezoresponse force microscopic (PFM), ferroelectric, magnetic, and magnetodielectric properties of 0-3 (magnetic nanoparticles (0) homogeneously distributed in ferroelectric matrices (3)) multiferroic composite thin films. The Pb(Fe 0.5 Nb 0.5 )O 3 (PFN) - Ni 0.65 Zn 0.35 Fe 2 O 4 (NZFO) particulate composite films were synthesized by pulsed laser deposition (PLD). These particulate composite thin films are completely c-axis oriented with very low surface roughness. We observed magnetic and ferroelectric T c above room temperature (RT) for all composite thin films. The PFN-NZFO 0-3 composites exhibit large polarization, high saturated magnetization with low coercive field, low dielectric loss along with magnetodielectric coupling at RT. These nanocomposites might be utilized in next generation nano/microelectronics and spintronic devices.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Optical control of integer and fractional Chern insulators

Optical control of topology, particularly in the presence of electron correlations, is an interesting topic with broad scientific and technological impact. Twisted MoTe 2 bilayer (tMoTe 2 ) is a zero-field fractional Chern insulator (FCI), exhibiting the fractionally quantized anomalous Hall effect. As the chirality of the edge states and sign of the Chern number are determined by the underlying ferromagnetic polarization, manipulation of ferromagnetism would realize control of the Chern insulator (CI)/FCI states. Here, in this work, we demonstrate control of ferromagnetic polarization, and thus the CI and FCI states, by circularly polarized optical pumping in tMoTe 2 . At low excitation power, we achieve on-demand preparation of ferromagnetic polarization by optical training, that is, electrically tuning the system from non-ferromagnetic to desirable ferromagnetic states under helicity-selective optical pumping. With increased excitation power, we further realize direct optical switching of ferromagnetic polarization at a temperature far below the Curie temperature. Both optical training and direct switching are most effective near CI and FCI states, which we attribute to a gap-enhanced valley polarization of optically pumped holes. The magnetization can be dynamically switched by modulating the helicity of optical excitation. Spatially resolved measurements further demonstrate optical writing of ferromagnetic, and thus CI (or FCI) domains. Our work realizes precise optical control of a topological quantum many-body system with potential applications in topological spintronics, quantum memories and creation of exotic edge states by programmable patterning of integer and fractionally quantized anomalous Hall domains.

ferromagnetism↗