Broadband electrically tunable VO 2 -Metamaterial terahertz switch with suppressed reflection
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Engineering↗
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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Graded Buffer Bragg Reflectors with High Reflectivity and Transparency for Metamorphic Optoelectronics
A graded buffer Bragg reflector (GBBR) is a bifunctional device component that provides the reflection of a distributed Bragg reflector and the adjustable lattice constant of a compositionally graded buffer. Prior work showed that these properties can be combined with low threading dislocation density and high reflectivity. Here, we design and demonstrate complex GBBRs for specific metamorphic solar cell applications. We design buffers that provide (1) high reflectivity over a narrow bandwidth, for quantum well solar cells, (2) reflectivity over a wide bandwidth, for optically thin solar cells, and (3) low sidelobe reflection, for multijunction devices that demand low out-of-band reflection. Apodized and triple GBBRs are demonstrated, and transparency is always considered, requiring designs with carefully engineered material combinations. A GBBR with a reflection of 99% is demonstrated, as well as a triple GBBR that has over 80% reflection for 100?nm of the spectrum around 800?nm. We also analyze potential deviations in a baseline GBBR from that of a perfect DBR using transmission electron microscopy to analyze imperfections in the material and modeling to analyze the impact of imperfect refractive index data for lattice-mismatched AlGaInAs. Minimal crosshatch roughness and unintentional thickness variation occur throughout the buffer, which likely influences reflection slightly. Small deviations between the calculated AlGaInAs and utilized AlGaAs refractive index exist, giving methods for future GBBR improvement. While the GBBR designs are intended for metamorphic solar cells, the broad and high reflection may also be useful for other optoelectronic devices such as light-emitting diodes or lasers.
41 EE - Solar Energy Technologies Office (EE-4S)↗
Super-resolution stimulated X-ray Raman spectroscopy
Propagation of intense X-ray pulses through dense media has led to the observation of phenomena such as atomic X-ray lasing, self-induced transparency and stimulated X-ray Raman scattering (SXRS)4. SXRS has been long predicted as a means to launch and probe valence-electron wavepackets and as a building block for nonlinear X-ray spectroscopies. However, experimental observations of SXRS to date have not provided spectroscopic information, and theoretical modelling has largely implemented hard-to-realize phase-coherent attosecond pulses. Here we demonstrate SXRS with spectroscopic precision, that is, detection of valence-excited states in neon with a near Fourier-limited joint energy–time resolution of 0.1 eV–40 fs. We used a new covariance analysis between statistically spiky broadband incident X-ray and scattered X-ray Raman pulses. Using 18,000 single shots, we beat not only the incident (about 8 eV) bandwidth but also the approximately 0.2 eV instrumental energy resolution, thus creating super-resolution conditions, in analogy to super-resolved fluorescence microscopy. Our experimental results, supported by ab initio propagation simulations, reveal the competition between lasing in the ion and stimulated Raman scattering in the neutral. We demonstrate enhanced signal collection efficiency and a broad excitation window, surpassing spontaneous Raman efficiencies by orders of magnitude. This stochastic SXRS approach represents a first step towards tracking elementary events that determine chemical outcomes.
nonlinear x-ray spectroscopy↗
Sequential Infiltration Synthesis of Bilayer Porous Alumina Nanostructures for Broad-Angle, Broadband Antireflective Coatings
Antireflective coatings (ARCs) are thin films engineered to reduce light reflections. Delivering broadband, wide-angle performance is essential for photovoltaics, imaging, and sensing, yet truly omnidirectional antireflection remains difficult due to angle-dependent optical paths and a narrow palette of suitable refractive indices. Here, in this study, we systematically investigate an emerging class of multilayer inorganic ARCs based on conformally coated nanoporous alumina templated by intrinsically microporous polymers (PIMs) and block copolymers (BCPs). We establish a design framework that maps thickness reflectance relationships to identify thickness pairs minimizing reflection across wavelength and incidence angle. We show that deliberately separating the local reflectance minima of the top and bottom layers in bilayer nanostructures broadens the antireflective bandwidth and angular range. We show that 235-nm single-side bilayer porous alumina nanostructures achieves under 2 % reflectance from 380–750 nm for incidence angles up to 45° with less than 0.6% reflectance for incidence angles under 20°. The approach is readily extensible to additional layers or materials with refractive indices tuned via templated nanoporosity and composition, enabling practical, etch-free ARC fabrication without HF or fluorinated precursors and advancing straightforward design of broadband, wide-angle (quasi-omnidirectional) ARCs for next-generation optical systems.
antireflective coatings↗
Review of Radio Frequency Interference and Potential Impacts on the CMB-S4 Cosmic Microwave Background Survey
CMB-S4 will map the cosmic microwave background to unprecedented precision, while simultaneously surveying the millimeter-wave time-domain sky, in order to advance our understanding of cosmology and the universe. CMB-S4 will observe from two sites, the South Pole and the Atacama Desert of Chile. A combination of small- and large-aperture telescopes with hundreds of thousands of polarization-sensitive detectors will observe in several frequency bands from 20-300 GHz, surveying more than 50% of the sky to arcminute resolution with unprecedented sensitivity. CMB-54 seeks to make a dramatic leap in sensitivity while observing across a broad range of largely unprotected spectrum which is increasingly being utilized for terrestrial and satellite transmissions. Fundamental aspects of CMB instrument technology leave them vulnerable to radio frequency interference (RFI) across a wide range of frequencies, including frequencies outside of their observing bands. Ground-based CMB instruments achieve their extraordinary sensitivities by deploying large focal planes of superconducting bolometers to extremely dry, high-altitude sites, with large fractional bandwidths, wide fields of view, and years of integration time. Suitable observing sites have historically offered significant protection from RFI, both naturally through their extremely remote locations as well as through restrictions on local emissions. Since the coupling mechanisms are complex, "safe" levels or frequencies of emission that would not interfere with CMB measurements cannot always be determined through straightforward calculations. We discuss models of interference for various types of RFI relevant to CMB-54, mitigation strategies, and the potential impacts on survey sensitivity.
Cosmic Microwave Background↗
Integrated microwave acousto-optic frequency shifter on thin-film lithium niobate
Electrically driven acousto-optic devices that provide beam deflection and optical frequency shifting have broad applications from pulse synthesis to heterodyne detection. Commercially available acousto-optic modulators are based on bulk materials and consume Watts of radio frequency power. Here, we demonstrate an integrated 3-GHz acousto-optic frequency shifter on thin-film lithium niobate, featuring a carrier suppression over 30 dB. Further, we demonstrate a gigahertz-spaced optical frequency comb featuring more than 200 lines over a 0.6-THz optical bandwidth by recirculating the light in an active frequency shifting loop. Our integrated acousto-optic platform leads to the development of on-chip optical routing, isolation, and microwave signal processing.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Ultra-broadband mid-infrared generation in dispersion-engineered thin-film lithium niobate
Thin-film lithium niobate (TFLN) is an emerging platform for compact, low-power nonlinear-optical devices, and has been used extensively for near-infrared frequency conversion. Recent work has extended these devices to mid-infrared wavelengths, where broadly tunable sources may be used for chemical sensing. To this end, we demonstrate efficient and broadband difference frequency generation between a fixed 1-µm pump and a tunable telecom source in uniformly-poled TFLN-on-sapphire by harnessing the dispersion-engineering available in tightly-confining waveguides. We show a simultaneous 1–2 order-of-magnitude improvement in conversion efficiency and ∼5-fold enhancement of operating bandwidth for mid-infrared generation when compared to equal-length conventional lithium niobate waveguides. We also examine the effects of mid-infrared loss from surface-adsorbed water on the performance of these devices.
47 OTHER INSTRUMENTATION↗
Characterization of Peripheral Neurophotonic Systems for High-Performance Human-Computer Interfaces (CRADA Final Report)
As part of the Cyclotron Road program, Morphosis Inc. sought to investigate a non-invasive neuromuscular sensing approach for use as an intuitive and secure human–computer interface. These highly miniaturized, wearable neural interfaces were completely non-invasive and maintained stable, high-bandwidth, long-term access to a user’s actions, intent, and identity, while offering an exceptionally high signal-to-noise ratio compared to contemporary neural recording technologies. The widespread adoption of neural interfaces had the potential to reshape how people interact with technology, with profound societal impacts. Millions worldwide suffered from movement and/or speech disabilities, and these tools had the potential to democratize access to technology to enhance autonomy and quality of life. More broadly, interfaces capable of accurately conveying intentions and safeguarding identities could serve as a cornerstone for privacy, trust, and personal authenticity in digital environments. The use of thought-driven control of digitally enabled devices and governance of digital identities had the potential to revolutionize relationships with technology, transforming how people learn, communicate, and interact with the world.
42 ENGINEERING↗
A 24-channel ultra-low-noise preamplifier for dN/dx measurements with drift tube detectors
Cluster counting $(dN/dx)$ is a promising method to enhance particle identification for gaseous detectors, especially in next-generation collider experiments like the FCC-ee, where good $π/K$ separation over a broad momentum range is essential. However, its implementation in large-scale systems has been limited by the challenging requirements for high-resolution signal amplification and readout. This paper presents a 24-channel ultra-low-noise preamplifier board designed for drift tube detectors to enable $dN/dx$ measurements. The three-stage amplification topology employs SiGe transistors and integrates dedicated noise-minimization techniques, achieving a charge gain of 21.11 mV/fC from 0.3 fC to 50 fC, a bandwidth of 542 MHz, and a voltage gain of 47.8 dB. The measured voltage noise density is 0.35 nV/$\sqrt{\textrm{Hz}}$ , surpassing most of the state-of-the-art preamplifiers for gaseous and silicon detectors. Validation tests conducted on the sMDT chambers at the CERN Proton Synchrotron test beam facility demonstrate that the proposed design meets the stringent preamplifier requirements for implementing the $dN/dx$ method in drift-tube detector systems, achieving an equivalent noise charge of 0.14 fC and a signal-to-noise ratio of 73 when operated with a He:iC 4 H 10 (90:10) gas mixture. The design also shows promise for broader application in other gaseous or semiconductor detectors.
Drift tube detector↗
A High-Speed, High-Resolution Transition Edge Sensor Spectrometer for Soft X-Rays at the Advanced Photon Source
This project explores the design and development of a transition edge sensor (TES) spectrometer for resonant soft X-ray scattering (RSXS) measurements developed in collaboration between Argonne National Laboratory (ANL) and the National Institute of Standards and Technology (NIST). Soft X-ray scattering is a powerful technique for studying the electronic and magnetic properties of materials on a microscopic level. However, the lack of high-performance soft X-ray spectrometers has limited the potential of this technique. TES spectrometers have the potential to overcome these limitations due to their high energy resolution, high efficiency, and broad energy range. This project aims to optimize the design of a TES spectrometer for RSXS measurements and more generally soft X-ray spectroscopy at the Advanced Photon Source (APS) 29-ID, leading to improved understanding of advanced materials. We will present a detailed description of the instrument design and implementation. The spectrometer consists of a large array of approximately 250 high-speed and high-resolution pixels. The pixels have saturation energies of approximately 1 keV, sub-ms pulse duration and energy resolution of approximately 1 eV. The array is read out using microwave multiplexing chips with MHz bandwidth per channel, enabling efficient data throughput. To facilitate measurement of samples in situ under ultra-high vacuum conditions at the beamline, the spectrometer is integrated with an approximately 1 m long snout.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Bandwidth Control and Symmetry Breaking in a Mott‐Hubbard Correlated Metal
Abstract In Mott materials strong electron correlation yields a spectrum of complex electronic structures. Recent synthesis advancements open realistic opportunities for harnessing Mott physics to design transformative devices. However, a major bottleneck in realizing such devices remains the lack of control over the electron correlation strength. This stems from the complexity of the electronic structure, which often veils the basic mechanisms underlying the correlation strength. This study presents control of the correlation strength by tuning the degree of orbital overlap using picometer‐scale lattice engineering. This study illustrates how bandwidth control and concurrent symmetry breaking can govern the electronic structure of a correlated SrVO 3 model system. This study shows how tensile and compressive biaxial strain oppositely affect the SrVO 3 in‐plane and out‐of‐plane orbital occupancy, resulting in the partial alleviation of the orbital degeneracy. The spectral weight redistribution under strain is derived and explained, which illustrates how high tensile strain drives the system toward a Mott insulating state. Implementation of such concepts can push correlated electron phenomena closer toward new solid‐state devices and circuits. These findings therefore pave the way for understanding and controlling electron correlation in a broad range of functional materials, driving this powerful resource for novel electronics closer toward practical realization.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Efficient Broadband Terahertz Generation by Above‐Band‐Gap Excitation of the Pyroelectric ZnSnN 2
Terahertz (THz) radiation is a powerful probe of low-energy excitations in all phases of matter. However, it remains a challenge to find materials that efficiently generate THz radiation in a broad range of frequencies following optical excitation. Here, we investigate a pyroelectric material, ZnSnN 2 , and find that its above-band-gap excitation results in the efficient formation of an ultrafast photocurrent generating THz radiation. The resulting THz electric field spans a frequency range from below 1 THz to above 30 THz. The results suggest that the photocurrent is primarily driven by an ultrafast pyroelectric effect where the photo-excited carriers screen the spontaneous electric polarization of ZnSnN 2 . Strong structural disorder reduces the photocarrier lifetime significantly and, thus, enables broadband operation. ZnSnN2 shows a similar THz-emitter performance as the best spintronic THz emitters regarding bandwidth and amplitude. The study unveils the large potential of pyroelectric materials as efficient and broadband THz emitters with built-in bias fields.
36 MATERIALS SCIENCE↗
Adjoint Waveform Tomography for Crustal and Upper Mantle Structure the Middle East and Southwest Asia for Improved Waveform Simulations Using Openly Available Broadband Data
We present a new model of radially anisotropic seismic wavespeeds for the crust and upper mantle of a broad region of the Middle East and Southwest Asia (MESWA) derived from adjoint waveform tomography. We inverted waveforms from 192 Global Centroid Moment Tensor earthquakes (MW 5.5-7.0) recorded by over 1000 openly available broadband seismic stations from permanent and temporary networks in the region. Spatial coverage of the available data is highly uneven due to earthquakes clustered along plate boundaries and sparse coverage of open seismic networks in the region. We considered three possible starting models: the SPiRaL global model (Simmons et al., 2021); MEC-1 (Kaviani et al., 2020); and CSEM2.0 (Noe et al., 2023). Because the SPiRaL model provides good fits to the observed waveforms measured by the time-bandwidth product of selected windows in several period bands, provides all the necessary parameters and covers the entire domain we used it for the starting model with the period band 50-100 seconds. Inversion iterations proceeded using time-frequency phase misfits in six stages and 54 total iterations reducing the minimum period to 30 seconds. Our final model, MESWA, provides improved waveform fits compared to the starting model for both the data used in the inversion and an independent validation data set of 66 events. Two metrics of waveform fit (the time-frequency phase misfit used in the optimization and normalized L2 misfit) were both reduced by nearly 60% for both data sets and MESWA provides significantly larger misfit reductions relative to the SPiRaL model than the MEC-1 or CSEM models. We also find that MESWA provides a larger time-bandwidth product of selected windows indicating that more information content of the observed waveforms is explained by MESWA than the other models. Our new model reveals tectonic features imaged by other studies and methods but in a new holistic model of shear and compressional wavespeeds (v S and v P , respectively) with anisotropy covering the crust and uppermost mantle of a larger domain. MESWA has smaller scale-length features and tends to sharpen some features relative to the SPiRaL starting model. Examples include: low crustal v S in the TurkishIranian Plateau, Zagros Mountains, Afghan Central Blocks and Sulaiman Fold Belt; low mantle vSfollowing divergent (Gulf of Aden, Red Sea) and transform (Dead Sea Fault) margins of the Arabian Plate; low and high v S in the mantle beneath the Arabian Shield and Platform, respectively. Low vS is imaged below Cenozoic volcanic centers of the Arabian Peninsula, the so-called Mecca-Madina-Nafud (MMN) Line. Positive anisotropy (v SH > v SV ) is inferred for asthenospheric depths across the region except where up/downwelling may influence fabric alignment (e.g. Afar, Red Sea, Arabian Shield). Elevated vS tracks Makran subduction under southeast Iran. MESWA resembles the SPiRaL model in its long-wavelength structure, but enhances shorter wavelengths features on the order of 200 km and smaller. The resulting model could be used for as a starting model for further improvements, say using waveforms from in-country seismic networks that are not openly available or smaller-scale studies targeting shorter period waveforms. The model also could be used for source characterization and moment tensor inversion to improve earthquake hazard studies and nuclear explosion monitoring.
58 GEOSCIENCES↗
High field magnetometry with hyperpolarized nuclear spins
Abstract Quantum sensors have attracted broad interest in the quest towards sub-micronscale NMR spectroscopy. Such sensors predominantly operate at low magnetic fields. Instead, however, for high resolution spectroscopy, the high-field regime is naturally advantageous because it allows high absolute chemical shift discrimination. Here we demonstrate a high-field spin magnetometer constructed from an ensemble of hyperpolarized 13 C nuclear spins in diamond. They are initialized by Nitrogen Vacancy (NV) centers and protected along a transverse Bloch sphere axis for minute-long periods. When exposed to a time-varying (AC) magnetic field, they undergo secondary precessions that carry an imprint of its frequency and amplitude. For quantum sensing at 7T, we demonstrate detection bandwidth up to 7 kHz, a spectral resolution < 100mHz, and single-shot sensitivity of 410pT $$/\sqrt{{{{{{{{\rm{Hz}}}}}}}}}$$ / Hz . This work anticipates opportunities for microscale NMR chemical sensors constructed from hyperpolarized nanodiamonds and suggests applications of dynamic nuclear polarization (DNP) in quantum sensing.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Evaluation of Clamshell Current Coupler for Online Frequency Domain and Spread Spectrum Time Domain Reflectometry to Detect Anomalies in Energized Cables
This document describes adaptation and evaluation of a clamshell inductive current coupler for online reflectometry testing (both frequency domain reflectometry and spread spectrum time domain reflectometry) to evaluate cable insulation degradation and anomalies. Safety-critical nuclear power plant cables were initially qualified for 40 years. However, as plants extend their operating licenses to 60 and 80 years, justification for continued safe operation includes test and monitoring programs. These will become more important as the industry moves to condition based qualification programs. Cable test programs traditionally involve manual interventions to disconnect cables, perform one or several tests, then reconnect the systems, usually during refueling outages occurring only every 18 to 24 months. This poses an operational burden that can be minimized by online testing or periodic connection to a coupler that may remain on the cable of interest or be clamped onto the cable without de-termination. This work investigates the adaptation of a clamshell inductive current coupler for either frequency domain reflectometry or spread-spectrum time domain reflectometry. The reflectometry test instrument injects a broad-band chirp or pseudo-noise signal onto a cable conductor and monitors for a reflected signal indicative of an impedance change caused by a damage condition. The instrument maximum input signal levels are typically 10 to 30 volts or less and the instruments will be damaged if subjected to 60 Hz power line voltages of 110, 220, or 480 VAC. One commercial spread-spectrum time domain reflectometry system has circuitry suitable for voltages up to 1 kV, but typical reflectometry tests are performed on de-energized cables. The clamshell inductive coupler provides >60 dB of 60 Hz attenuation with less than 10 dB loss in the 1-500 MHz test bandwidth of interest. An energized cable was successfully tested up to 6.7 kVp-p and frequency response plots imply that the tests could be extended to 10 kV or higher energized levels.
36 MATERIALS SCIENCE↗
Uncovering surface plasmon optical resonances in nanohole arrays through interferometric photoemission electron microscopy
In this work, the role of surface plasmon polaritons (SPPs) in nanohole array optical extinction spectra is explored using a time-resolved technique capable of isolating the air/metal interfacial SPP contribution to the typical Fano profile in optical transmission curves. A pair of interferometrically locked broad-band femtosecond pulses is used to launch SPPs from lithographically patterned plasmonic nanohole arrays. SPPs launched in the co- and counter-propagating directions are probed using a third probe pulse in a photoemission electron microscope. Using this approach, we record interferometric SPP–SPP linear autocorrelations that selectively report on the resonances of SPPs launched from arrays of varying pitches and hole diameters. Aside from advancing an approach to selective SPP spectroscopy, we illustrate that resonant coupling in the counter-propagating direction may be exploited to control the spatial, temporal, and spectral characteristics of SPPs. For the counter-propagating direction, we show that tuning the array pitch near the fundamental plasmon resonance generates color-tuned (~770–820 nm), narrow bandwidth SPPs, and the bandwidth may be controlled by changing the ratio of pitch to hole diameter. The SPP resonances we recover through Fourier transforms of the interferometric autocorrelations shed light on the classical problem of Fano interference in nanohole array extinction spectra.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
SSTDR and FDR Detection of Un-Energized and Energized Cable Anomalies Including Thermal Degradation Using Machine Learning
Historically, cables are initially qualified for nuclear power plant use for 40 years. As plants extend their operating license to 60 and 80 years, continued use of these cables must shift to a performance-based approach since it is cost prohibitive to completely replace cables that are likely still capable of performing their design function. A variety of cable tests are available and are commonly applied during outages when the cables can be taken out of service. Frequency domain reflectometry (FDR) is one of these test methods that is being more broadly accepted and used because it not only detects anomalies along the cable with a low-voltage signal that does not stress the cable insulation, but the technique also locates the anomalies. This supports follow-up local inspection and local repair or partial replacement of a damaged cable segment. Currently, FDR testing is only applied to cables that are taken out of service since the test instrument would be damaged by operational voltages. A related technology that has found some acceptance in the aircraft and rail industry is spread spectrum time domain reflectometry (SSTDR). This technology has been implemented with a custom commercial instrument by LiveWire Innovation that is designed to operate on live cables up to 1000 volts and with a bandwidth of 48 MHz. Initial evaluation by the Pacific Northwest National Laboratory (PNNL) of the Live Wire system indicated that a broader bandwidth (BW) SSTDR may be better for many kinds of flaws. This led PNNL to develop an SSTDR laboratory instrument suitable for tests up to 500 MHz bandwidth. Testing on energized cables is also desirable for online monitoring systems so an inductive clamshell coupler was developed that allows energized cables to be tested up to at least 5 kV and likely higher voltage levels. Dielectric spectroscopy and tan delta testing plus various laboratory destructive tests were included in this data acquisition campaign directed to feed a machine learning (ML) study. With these kinds of developments, online energized cable tests may be possible with industrial adoption of such hardware advances but it will be completely impractical to have highly skilled data analysts continually examine these complex signals for indications of damage or compromised conditions. If online testing is to be implemented in new test hardware, it must be accompanied by software that can interpret the signals and alert plant operators of changing or degraded conditions. The thermally aged, shielded cable investigated here was separately treated for ML analysis. Visual analysis of electrical data showed generally increasing peaks where the cable entered and exited the oven. These peaks were not exactly aligned with expected locations, but these differences were attributed to velocity of propagation calibration errors. Only supervised ML was applied to the thermally aged data as this data was only available shortly before the committed publication date of this report. The supervised ML was structured to divide the 0 to 70-day responses as ‘normal’ from 0 to 35 days or ‘anomalous’ from 36 to 70 days, based on cable tensile elongation at break (EAB) insulation characterization. Using 80% of the data for training and 20% for testing, the supervised ML predicted normal versus anomalous was 70% accurate. Important conclusions include: • Accuracy to predict the presence of cable damage is improved from the 2023 effort by more training data. Weighted accuracies for comparisons among the instruments ranged from 67 to 89 % for unsupervised ML and 71 to 99% for supervised ML. • Based on the synthetic data tests, the unsupervised models are more generalizable to unseen anomalies. The Multi-Layer Perceptron classifier (MLP) model reported as high as 99.7% accuracy on the test data, but this dropped to 58.3% when tested on the synthetic data. In contrast, the unsupervised Pointwise model only achieved 89.7% accuracy on the experimental data but reported 78.3% accuracy on the synthetic data. • The best anomaly indicators are higher frequency (400 MHz BW) FDR data. Other tests may be interesting but for this study, this was the best predicter.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Spin and charge excitations in the correlated multiband metal Ca 3 Ru 2 O 7
We use Ru $L_3$-edge resonant inelastic x-ray scattering to study the full range of excitations in Ca 3 Ru 2 O 7 from meV-scale magnetic dynamics through to the eV-scale interband transitions. This bilayer 4d-electron correlated metal expresses a rich phase diagram, displaying long-range magnetic order below 56 K followed by a concomitant structural, magnetic, and electronic transition at 48 K. In the low-temperature phase, we observe a magnetic excitation with a bandwidth of ~30 meV and a gap of ~8 meV at the zone center, in excellent agreement with inelastic neutron scattering data. The dispersion can be modeled using a Heisenberg Hamiltonian for a bilayer S = 1 system with single-ion anisotropy terms. At a higher energy loss, dd-type excitations show heavy damping in the presence of itinerant electrons, giving rise to a fluorescencelike signal appearing between the $t_{2g}$ and $e_g$ bands. At the same time, we observe a resonance originating from localized $t_{2g}$ excitations, in analogy to the structurally related Mott insulator Ca 2 RuO 4 . But whereas Ca 2 RuO 4 shows sharp separate spin-orbit excitations and Hund’s-rule driven spin-state transitions, here we identify only a single broad asymmetric feature. These results indicate that local intraionic interactions underlie the correlated physics in Ca 3 Ru 2 O 7 , even as the excitations become strongly mixed in the presence of itinerant electrons.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗