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At least 469 records · Page 26

A New Route Toward Atomically Flat and Defect-Free Ge/SiGe Planar Heterostructures

Germanium-based planar heterostructures are emerging as versatile platforms for realizing quantum devices. In particular, planar Ge/SiGe quantum wells (QWs) host hole states with exceptionally high mobility and strong, electrically tunable spin–orbit interactions, enabling full electrical control of quantum information. A key requirement for these systems is the growth of microscopic, defect-free, atomically flat Ge QW heterostructures on relaxed or reverse-graded SiGe buffer layers, as well as on commercial Ge substrates. While several physical deposition techniques have demonstrated high-quality planar Ge/SiGe QWs, a major challenge remains: minimizing defect density typically requires high growth temperatures, which are incompatible with standard CMOS process flows. Here, we present a convenient low-temperature process for realizing high-quality planar SiGe/Ge heterostructures using a combination of thermal and electron-beam evaporation. We systematically map the effects of ex-situ and in-situ substrate preparation protocols, growth temperature, and post-deposition annealing conditions, and correlate these parameters with surface roughness and defect density. We find that in-situ oxide desorption conditions and post-annealing parameters have the most pronounced impact on improving surface quality. Under optimized conditions, we achieve atomically smooth surfaces with root-mean-square roughness σrms​ ≤ 10 Å and negligible defect density. Interestingly, thermally evaporated Ge layers exhibit oriented triangular crystallites that elongate upon post-annealing in the presence of high Ge vapor pressure. These results demonstrate that this simple, low-temperature deposition approach is a viable and effective route for achieving high-quality Ge QW heterostructures, with strong potential for scalable quantum computing and sensing applications.

Tripathi, Malvika [Fermilab] (ORCID:00000001989251↗

Relaxation and frequency shifts in the ground state of Rb-85

Results are presented on the relaxation and frequency shifts measured for the 0-0 transition of the ground state of Rb-85 at 3.03 GHz in various physical environments. These results include data on spin-exchange, buffer-gas, and wall interactions.

Vanier, J.↗

Ultrafast population and structural dynamics of a Ni-bipyridine photoredox catalyst reveal a significant deactivation pathway

The ultrafast excited state pathways and dynamics of NiII-bipyridine complexes influence the yield of photochemical processes involved in their catalytic cross-coupling reactions. Here we present ultrafast Ni K x-ray emission spectroscopy (XES) and x-ray solution scattering (XSS) of a NiII-bipyridine aryl halide complex, [Ni(t-Bubpy)(o-tol)Br], to quantify the excited state population dynamics and structural changes of the pre-catalyst. Due to the local spin-sensitivity of XES, the population dynamics of metal-to-ligand charge transfer (MLCT) and metal-centered (MC) excited states is established. A rapid ground state recovery pathway is newly identified, representing a significant deactivation pathway during photocatalysis. Furthermore, the pseudotetrahedral structure of the long-lived MC excited state is unambiguously identified and refined by XSS. The results advance our understanding of the ultrafast relaxation mechanisms that impact the photocatalytic mechanism and yield for NiII-bipyridine aryl halide cross-coupling catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Extended flexibility of neutron Larmor diffraction for increased diffraction range in mosaicity measurements

Larmor diffraction (LD) is a neutron scattering technique that offers enhanced resolution by harnessing the Larmor precession of neutron spins in a magnetic field. By encoding subtle changes in neutron momentum transfer into significant alterations in the Larmor phase of neutron spins, LD can be employed to measure lattice expansion, lattice distortion, and mosaicity with exceptional resolution. As originally proposed by Rekveldt et al., LD necessitates the magnetic field boundaries to be tilted to be parallel to the crystal plane of interest. Here, this report explores the fundamental principles shared between LD and spin-echo small-angle neutron scattering (SESANS). Drawing inspiration from the flexibility of SESANS to adjust magnetic field boundaries to optimize the resolution in the measurement of the neutron momentum transfers q, we will demonstrate that the strict requirement of parallel alignment between the magnetic field boundaries and the crystal plane can be relaxed for the measurements of mosaicity. Such relaxation will expand the accessible diffraction angles for these situations that are highly constrained.

Larmor diffraction↗

Universality of Collective Density Fluctuations in Liquids at and away from Equilibrium – An Integrated Neutron Scattering, Theoretical, and Computational Study (Final Technical Report)

Liquids, ubiquitous on earth, are prototypical disordered condensed matter. As the mediate phase between non-structured gases and ordered solids, liquids p ossess intriguing complexities that are absent on either extreme counter phase, especially when they are driven away from equilibrium. Despite decades of studies, the physics of liquids still keeps surprising us and challenges our understanding of condensed matter, emergent phenomena, and complex systems. Among the many interesting properties, the nature of collective dynamics in liquids remains elusive because of both the presence of strong interactions and the absence of translational invariance. This project studied the universal features of collective density fluctuations (or collective modes), which include both phonon-like excitations and collective relaxations, in the Q-dependent generalized hydrodynamic regime in liquids and liquid-like matter both at and away from equilibrium. We performed systematic studies of the fast collective dynamics (including both phonon-like excitations and collective relaxations) of four classes of liquids characterized by different fragilities and interactions using synergistically integrated coherent neutron scattering experiments (Inelastic Neutron Scattering (INS), Quasi-Elastic Neutron Scattering (QENS), and Neutron Spin Echo (NSE)), a ViscoElastic Hydrodynamics theory we have been developing, andMolecular Dynamics (MD) simulations and our analysis package LiquidLib. The transformative knowledge of the collective dynamics in liquids is important to understand and ultimately control the transport of mass, energy, and charge in liquids, both at and away from thermal equilibrium, which may will likely impact a wide range of disciplines.

36 MATERIALS SCIENCE↗

Flexible Microstrip Circuits for Superconducting Electronics

Flexible circuits with superconducting wiring atop polyimide thin films are being studied to connect large numbers of wires between stages in cryogenic apparatus with low heat load. The feasibility of a full microstrip process, consisting of two layers of superconducting material separated by a thin dielectric layer on 5 mil (approximately 0.13 mm) Kapton sheets, where manageable residual stress remains in the polyimide film after processing, has been demonstrated. The goal is a 2-mil (approximately 0.051-mm) process using spin-on polyimide to take advantage of the smoother polyimide surface for achieving highquality metal films. Integration of microstrip wiring with this polyimide film may require high-temperature bakes to relax the stress in the polyimide film between metallization steps.

Chervenak, James↗

Direct observation of two-dimensional magnons in atomically thin CrI 3

Magnons are collective spin excitations in crystals with long-range magnetic order. The emergent van der Waals magnets provide a highly tunable platform to explore magnetic excitations in the two-dimensional limit with intriguing properties, manifesting from their honeycomb lattice structure and switchable magnetic configurations. Here, we report the direct observation of two-dimensional magnons through magneto-Raman spectroscopy with optical selection rules determined by the interplay between crystal symmetry, layer number and magnetic states in atomically thin CrI 3 . In monolayers, we observe an acoustic magnon mode at ~0.3 meV. It has strict cross-circularly polarized selection rules locked to the magnetization direction that originates from the conservation of angular momentum of photons and magnons dictated by three-fold rotational symmetry. Additionally, we reveal optical magnon modes at ~17 meV. This mode is Raman silent in monolayers, but optically active in bilayers and bulk due to a relaxation of the parity criterion resulting from the layer index. In the layered antiferromagnetic states, we directly resolve two degenerate optical magnon modes with opposite angular momentum and conjugate optical selection rules. From these measurements, we quantitatively extract the spin-wave gap, magnetic anisotropy and intralayer and interlayer exchange constants, and establish two-dimensional magnets as a new platform for exploring magnon physics.

36 MATERIALS SCIENCE↗

Mitigating Sodium Ordering for Enhanced Solid Solution Behavior in Layered NaNiO 2 Cathodes

Abstract The O‐type layered nickel oxides suffer from undesired cooperative Jahn–Teller distortion stemming from Ni 3+ ions and undergo multiple biphasic structural transformations during the insertion/extraction of large Na + ions, posing a significant challenge to stabilize the structural integrity. We present here a systematic investigation of the impact of substituting 5 % divalent (Mg 2+ ) or trivalent (Al 3+ or Co 3+ ) ions for Ni 3+ to alleviate Na + ion ordering and perturb the Jahn–Teller effect to enhance structural stability. We gauge a fundamental understanding of the Mg−O and Na−O or Mg−O−Na bonding interactions, noting that the ionicity of the Mg−O bond deshields the electronic cloud of oxygen from Na + ions. Furthermore, calculations of the Van Vleck distortion modes reveal a relaxation of NiO 6 octahedra from Jahn–Teller distortion and a reduced electron density at the interlayer with Mg 2+ substitution. Long‐range ( operando X‐ray diffraction) and short‐range (magic angle spinning nuclear magnetic resonance) structural analyses provide insights into reduced ordering, allowing a stable continuous solid solution. Overall, Mg‐substitution results in a high‐capacity retention of ~96 % even after 100 cycles, showcasing the potential of this strategy for overcoming the structural instabilities and enhancing the performance of sodium‐ion batteries.

Sada, Krishnakanth↗

Pursuing Heteroleptic Ligand Design Principles for Photoactive Fe Complexes with Ultrafast X-ray Emission and Variable-Temperature Optical Spectroscopies

Understanding the key parameters that govern the photophysical and photochemical properties of transition metal complexes is essential for the development of efficient photosensitizers for photocatalytic applications. Achieving this objective necessitates clear and detailed investigations of their electronic excited states, for which time-resolved metal Kβ X-ray emission spectroscopy (XES) has proven highly effective. Here, we present a time-resolved Fe Kβ XES study of a heteroleptic Fe(II) polypyridyl carbene complex, [Fe(phen) 2 (C 4 H 10 N 4 )] 2+ (1; phen = 1,10-phenanthroline), utilizing both the valence-to-core and Kβ mainline spectral regions, complemented by variable-temperature transient optical absorption (VT-TA) spectroscopy. Detailed analysis of the time-resolved Kβ XES data, supported by density functional theory (DFT) calculations and an Eyring analysis of the VT-TA data, reveals parallel excited state relaxation dynamics that support an assignment of the long-lived excited state to a triplet metal-centered state. Placing these results in the context of prior studies of heteroleptic Fe(II) polypyridyl cyanide complexes motivated a series of DFT calculations to investigate the effects of ligand structural flexibility and arrangement. These calculations reinforce the experimentally derived conclusion that constraining structural flexibility with multidentate ligands significantly impacts the excited state relaxation dynamics. Furthermore, our study emphasizes that the arrangement of strong field ligands in heteroleptic complexes substantially affects the energy of Jahn–Teller active triplet metal-centered states in low-spin d 6 metal complexes. Together, these findings provide synthetic design principles for extending metal-to-ligand charge transfer excited state lifetimes of heteroleptic Fe complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Low-temperature T -linear resistivity due to umklapp scattering from a critical mode

In this study, we consider the transport properties of a model of fermions scattered by a critical bosonic mode. The mode is overdamped and scattering is mainly in the forward direction. Such a mode appears at the quantum critical point for an electronic nematic phase transition and in gauge theories for a U(1) spin liquid. It leads to a short fermion lifetime, violating Landau's criterion for a Fermi liquid. In spite of this, transport can be described by a Boltzmann equation. We include momentum relaxation by umklapp scattering, supplemented by weak impurity scattering. We find that above a very low temperature which scales with Δ q 3 , where Δ q is the minimum umklapp scattering vector, the resistivity is linear in T with a coefficient which is independent of the amount of disorder. This picture holds until the temperature dependent part of the resistivity exceeds that due to impurity scattering. We compare the relaxation time approximation with an exact numerical solution of the Boltzmann equation. Surprisingly we find that, unlike the resistivity, the Hall coefficient strongly deviates from the relaxation time approximation and shows a strong reduction with increasing temperature. We comment on possible comparisons with experiments on high T c cuprates.

36 MATERIALS SCIENCE↗

Chemical Analysis of Fluorobenzenes via Multinuclear Detection in the Strong Heteronuclear J-Coupling Regime

Chemical analysis via nuclear magnetic resonance (NMR) spectroscopy using permanent magnets, rather than superconducting magnets, is a rapidly developing field. Performing the NMR measurement in the strong heteronuclear J-coupling regime has shown considerable promise for the chemical analysis of small molecules. Typically, the condition for the strong heteronuclear J-coupling regime is satisfied at µT magnetic field strengths and enables high resolution J-coupled spectra (JCS) to be acquired. However, the JCS response to systematic chemical structural changes has largely not been investigated. In this report, we investigate the JCS of C6H6−xFx (x = 0, 1, 2, …, 6) fluorobenzene compounds via simultaneous excitation and detection of 19F and 1H at 51.5 µT. The results demonstrate that JCS are quantitative, and the common NMR observables, including Larmor frequency, heteronuclear and homonuclear J-couplings, relative signs of the J-coupling, chemical shift, and relaxation, are all measurable and are differentiable between molecules at low magnetic fields. The results, corroborated by ab initio calculations, provide new insights into the impact of chemical structure and their corresponding spin systems on JCS. In several instances, the JCS provided more chemical information than traditional high field NMR, demonstrating that JCS can be used for robust chemical analysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Unified Radio and Plasma wave investigation

The scientific objectives of the Ulysses Unified Radio and Plasma wave (URAP) experiment are twofold: (1) the determination of the direction, angular size, and polarization of radio sources for remote sensing of the heliosphere and the Jovian magnetosphere and (2) the detailed study of local wave phenomena, which determine the transport coefficients of the ambient plasma. A brief discussion of the scientific goals of the experiment is followed by a comprehensive description of the instrument. The URAP sensors consist of a 72.5 m electric field antenna in the spin plane, a 7.5-m electric field monopole along the spin axis of a pair of orthogonal search coil magnetic antennas. The various receivers, designed to encompass specific needs of the investigation, cover the frequency range from dc to 1 MHz. A relaxation sounder provides very accurate electron density measurements. Radio and plasma wave observations are shown to demonstrate the capabilities and limitations of the URAP instruments: radio observations include solar bursts, auroral kilometric radiation, and Jovian bursts; plasma waves include Langmuir waves, ion acousticlike noise, and whistlers.

Stone, R. G.↗

Studies of superconducting materials with muon spin rotation

The muon spin rotation/relaxation technique was found to be an exceptionally effective means of measuring the magnetic properties of superconductors, including the new high temperature superconductor materials, at the microscopic level. The technique directly measures the magnetic penetration depth (type II superconductors (SC's)) and detects the presence of magnetic ordering (antiferromagnetism or spin-glass ordering were observed in some high temperature superconductor (HTSC's) and in many closely related compounds). Extensive studies of HTSC materials were conducted by the Virginia State University - College of William and Mary - Columbia University collaboration at Brookhaven National Laboratory and TRIUMF (Vancouver). A survey of LaSrCuO and YBaCaCuO systems shows an essentially linear relationship between the transition temperature T(sub c) and the relaxation rate. This appears to be a manifestation of the proportionality between T(sub c) and the Fermi energy, which suggests a high energy scale for the SC coupling, and which is not consistent with the weak coupling of phonon-mediated SC. Studies of LaCuO and YBaCuO parent compounds show clear evidence of antiferromagnetism. YBa2Cu(3-x)CO(x)O7 shows the simultaneous presence of spin-glass magnetic ordering and superconductivity. Three-dimensional SC, (Ba, K) BiO3, unlike the layered CuO-based compounds, shows no suggestion of magnetic ordering. Experimental techniques and theoretical implications are discussed.

Davis, Michael R.↗

Bias Momentum Sizing for Hovering Dual-Spin Platforms

An atmospheric flight vehicle in hover is typically controlled by varying its thrust vector. Achieving both levitation and control with the propulsion system places considerable demands on it for agility and precision, particularly if the vehicle is statically unstable, or nearly so. These demands can be relaxed by introducing an appropriately sized angular momentum bias about the vehicle's yaw axis, thus providing an additional margin of attitude stability about the roll and pitch axes. This paper describes an approach for specifying the appropriate size of such angular momentum bias, based on the vehicle s physical parameters and its disturbance environment. It also describes several simplifications that provide a more physical and intuitive understanding of the dynamics. This will enhance the possibility of practically applying this technology to a flying vehicle.

Lim, K. B.↗

Magnetic order in nanogranular iron germanium (Fe 0.53 Ge 0.47 ) films

We study the effect of strain on the magnetic properties and magnetization configurations in nanogranular Fe x Ge 1-x films (x = 0.53 ± 0.05) with and without B20 FeGe nanocrystals surrounded by an amorphous structure. Relaxed films on amorphous silicon nitride membranes reveal a disordered skyrmion phase while films near and on top of a rigid substrate favor ferromagnetism and an anisotropic hybridization of Fe d levels and spin-polarized Ge sp band states. The weakly coupled topological states emerge at room temperature and become more abundant at cryogenic temperatures without showing indications of pinning at defects or confinement to individual grains. These results demonstrate the possibility to control magnetic exchange and topological magnetism by strain and inform magnetoelasticity-mediated voltage control of topological phases in amorphous quantum materials.

36 MATERIALS SCIENCE↗

Valley phonons and exciton complexes in a monolayer semiconductor

The coupling between spin, charge, and lattice degrees of freedom plays an important role in a wide range of fundamental phenomena. Monolayer semiconducting transitional metal dichalcogenides have emerged as an outstanding platform for studying these coupling effects. Here, we report the observation of multiple valley phonons – phonons with momentum vectors pointing to the corners of the hexagonal Brillouin zone – and the resulting exciton complexes in the monolayer semiconductor WSe2. We find that these valley phonons lead to efficient intervalley scattering of quasi particles in both exciton formation and relaxation. This leads to a series of photoluminescence peaks as valley phonon replicas of dark trions. Using identified valley phonons, we also uncover an intervalley exciton near charge neutrality. Our work not only identifies a number of previously unknown 2D excitonic species, but also shows that monolayer WSe 2 is a prime candidate for studying interactions between spin, pseudospin, and zone-edge phonons.

36 MATERIALS SCIENCE↗

Circuit Quantum Electrodynamics in Hyperbolic Space: From Photon Bound States to Frustrated Spin Models

Circuit quantum electrodynamics is one of the most promising platforms for efficient quantum simulation and computation. In recent groundbreaking experiments, the immense flexibility of superconducting microwave resonators was utilized to realize hyperbolic lattices that emulate quantum physics in negatively curved space. Here we investigate experimentally feasible settings in which a few superconducting qubits are coupled to a bath of photons evolving on the hyperbolic lattice. We compare our numerical results for finite lattices with analytical results for continuous hyperbolic space on the Poincaré disk. We find good agreement between the two descriptions in the long-wavelength regime. We show that photon-qubit bound states have a curvature-limited size. We propose to use a qubit as a local probe of the hyperbolic bath, for example, by measuring the relaxation dynamics of the qubit. We find that, although the boundary effects strongly impact the photonic density of states, the spectral density is well described by the continuum theory. We show that interactions between qubits are mediated by photons propagating along geodesics. We demonstrate that the photonic bath can give rise to geometrically frustrated hyperbolic quantum spin models with finite-range or exponentially decaying interaction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗