arXiv subjects

William Ratcliff II

Publications and source records attributed to William Ratcliff II.

12 recordsLinked to original sources

arXiv2026

Computed materials proposals depart from the structural memory of experimental discovery

Generative AI and high-throughput DFT pipelines propose millions of inorganic crystal structures, but lack a calibrated reference frame against experimentally realized chemistry. Here we embed 167,500 Inorganic Crystal Structure Database entries in a continuous structural-similarity space, partition it into graph communities, and replay them in time. Experimental discovery shows strong structural memory: 82.9% of new formulas enter pre-existing communities; new-community formation falls from 40.2% (1930s) to 2.6% (2010s). The communities are chemically meaningful, positively identifying nine textbook field-defining renaissances, including cuprates, colossal-magnetoresistance manganites, MAX phases, and Li-ion battery cathodes. Projecting GNoME, MatterGen-public, Materials Project, JARVIS-DFT, and Alexandria-PBE into frozen historical maps yields a cutoff-robust ordering: held-out ICSD > MatterGen > {GNoME ~ MP-theoretical} > JARVIS > Alexandria. Structural departure from experimental basins is not specific to generative AI but general across the tested computed sets. Combining structural proximity with reduced-formula precedent defines a historical synthesizability prior for triaging computed materials.

cond-mat.mtrl-sci↗

arXiv2026

Accelerating Quantum Materials Characterization: Hybrid Active Learning for Autonomous Spin Wave Spectroscopy

Autonomous neutron spectroscopy must solve three distinct tasks: detection (where is the signal?), inference (which Hamiltonian governs it?), and refinement (what are the parameters?). No single controller solves all three equally well. We present TAS-AI, a hybrid agnostic-to-physics-informed framework for autonomous triple-axis spin-wave spectroscopy that separates these tasks explicitly. In blind reconstruction benchmarks, model-agnostic methods such as random sampling, coarse grids, and Gaussian-process mappers reach a global error threshold more reliably and with fewer measurements than physics-informed planning, supporting the claim that discovery and inference are distinct tasks requiring distinct controllers. Once signal structure is localized, the physics-informed stage performs in-loop Hamiltonian discrimination and parameter refinement: in a controlled square-lattice test between nearest-neighbor-only and J1-J2 Hamiltonians, TAS-AI reaches a decisive AIC-derived evidence ratio (>100) in fewer than 10 measurements, while motion-aware scheduling cuts wall-clock time by 32% at a fixed measurement budget. We also identify a failure mode of posterior-weighted design, algorithmic myopia, in which the planner over-refines the current leading model while under-sampling low-intensity falsification probes. A constrained falsification channel sharply reduces time spent committed to the wrong model and accelerates correct model selection without modifying the Bayesian inference engine. In controlled two-model ablations, both a deterministic top-two max-disagreement rule and an LLM-based audit committee achieve this gain under identical constraints. We demonstrate the full workflow in silico using a high-fidelity digital twin and provide an open-source Python implementation.

cond-mat.mtrl-sci↗

arXiv2019

Ferromagnetic van der Waals compound MnSb$_{1.8}$Bi$_{0.2}$Te$_4$

The intersection of topology and magnetism represents a new playground to discover novel quantum phenomena and device concepts. In this work, we show that a van der Waals compound MnSb$_{1.8}$Bi$_{0.2}$Te$_4$ exhibits a ferromagnetic ground state with a Curie temperature of 26 K, in contrast to the antiferromagnetic order previously found for other members of the Mn(Sb, Bi)$_2$Te$_4$ family. We employ magneto-transport, bulk magnetization and neutron scattering studies to illustrate the magnetic and electrical properties of MnSb$_{1.8}$Bi$_{0.2}$Te$_4$ and report on the observation of an unusual anomalous Hall effect. Our results are an important step in the synthesis and understanding of ferromagnetic topological insulators.

cond-mat.mes-hall↗

arXiv2019

Quantum oscillations from networked topological interfaces in a Weyl semimetal

Layered transition metal chalcogenides are promising hosts of electronic Weyl nodes and topological superconductivity. MoTe$_2$ is a striking example that harbors both noncentrosymmetric T$_d$ and centrosymmetric T' phases, both of which have been identified as topologically nontrivial. Applied pressure tunes the structural transition separating these phases to zero temperature, stabilizing a mixed T$_d$-T' matrix that entails a unique network of interfaces between the two non-trivial topological phases. Here, we show that this critical pressure range is characterized by unique coherent quantum oscillations, indicating that the change in topology between two phases give rise to a new topological interface state. A rare combination of topologically nontrivial electronic structures and locked-in transformation barriers leads to this counterintuitive situation wherein quantum oscillations can be observed in a structurally inhomogeneous material. These results open the possibility of stabilizing multiple topological superconducting phases, which are important for solving the decoherence problem in quantum computers.

cond-mat.mtrl-sci↗

arXiv2018

Mechanical control of crystal symmetry and superconductivity in Weyl semimetal MoTe$_2$

The non-centrosymmetric Weyl semimetal candidate, MoTe$_2$ was investigated through neutron diffraction and transport measurements at pressures up to 1.5 GPa and at temperatures down to 40 mK. Centrosymmetric and non-centrosymmetric structural phases were found to coexist in the superconducting state. Density Functional Theory (DFT) calculations reveal that the strength of the electron-phonon coupling is similar for both crystal structures. Furthermore, it was found that by controlling non-hydrostatic components of stress, it is possible to mechanically control the ground state crystal structure. This allows for the tuning of crystal symmetry in the superconducting phase from centrosymmetric to non-centrosymmetric. DFT calculations support this strain control of crystal structure. This mechanical control of crystal symmetry gives a route to tuning the band topology of MoTe$_2$ and possibly the topology of the superconducting state.

cond-mat.str-el↗

arXiv2018

reductus: a stateless Python data-reduction service with a browser frontend

The online data reduction service reductus transforms measurements in experimental science from laboratory coordinates into physically meaningful quantities with accurate estimation of uncertainties based on instrumental settings and properties. This reduction process is based on a few well-known transformations, but flexibility in the application of the transforms and algorithms supports flexibility in experiment design, supporting a broader range of measurements than a rigid reduction scheme for data. The user interface allows easy construction of arbitrary pipelines from well-known data transforms using a visual dataflow diagram. Source data is drawn from a networked, open data repository. The Python backend uses intelligent caching to store intermediate results of calculations for a highly responsive user experience. The reference implementation allows immediate reduction of measurements as they are recorded for the three neutron reflectometry instruments at the NIST Center for Neutron Research (NCNR), without the need for visiting scientists to install additional software on their own computers.

physics.data-an↗

arXiv2017

Successive field-induced transitions in BiFeO$_{3}$ around room temperature

The effects of high magnetic fields applied perpendicular to the spontaneous ferroelectric polarization on single crystals of BiFeO$_3$ were investigated through magnetization, magnetostriction, and neutron diffraction measurements. The magnetostriction measurements revealed lattice distortion of $2\times 10^{-5}$, during the reorientation process of the cycloidal spin order by applied magnetic fields. Furthermore, anomalous changes in magnetostriction and electric polarization at a larger field demonstrate an intermediate phase between cycloidal and canted antiferromagnetic states, where a large magnetoelectric effect was observed. Neutron diffraction measurements clarified that incommensurate spin modulation along [110] direction in the cycloidal phase becomes commensurate in the intermediate phase. Theoretical calculations based on the standard spin Hamiltonian of this material suggest an antiferromagnetic cone-type spin order in the intermediate phase.

cond-mat.mtrl-sci↗

arXiv2016

Tailoring Exchange Couplings in Magnetic Topological Insulator/Antiferromagnet Heterostructures

Magnetic topological insulators such as Cr-doped (Bi,Sb)2Te3 provide a platform for the realization of versatile time-reversal symmetry-breaking physics. By constructing heterostructures with Néel order in an antiferromagnetic CrSb and magnetic topological order in Cr-doped (Bi,Sb)2Te3, we realize emergent interfacial magnetic phenomena which can be tailored through artificial structural engineering. Through deliberate geometrical design of heterostructures and superlattices, we demonstrate the use of antiferromagnetic exchange coupling in manipulating the magnetic properties of the topological surface massive Dirac fermions. This work provides a new framework on integrating topological insulators with antiferromagnetic materials and unveils new avenues towards dissipationless topological antiferromagnetic spintronics.

cond-mat.mtrl-sci↗

arXiv2014

Magnetic Structure of Hexagonal Mn-doped LuFeO$_{3}$

Neutron scattering techniques are used to investigate the crystalline and magnetic structure of LuFe$_{0.75}$Mn$_{0.25}$O$_{3}$ in bulk polycrystalline form. We find that the crystalline structure is described by the hexagonal P6$_{3}$cm space group similar to that of thin-film LuFeO$_{3}$, and that the system orders antiferromagnetically below T$_{N}$ = 134 K. Inelastic neutron scattering reveals nearest-neighbor superexchange parameters that are enhanced relative to LuMnO$_{3}$. The observation of significant diffuse scattering above T$_{N}$ demonstrates the frustrated nature of the system; comparisons with similar materials suggest the ground state magnetic configuration is sensitive to local crystallographic distortions.

cond-mat.mtrl-sci↗

arXiv2014

Complex structures of different CaFe$_{2}$As$_{2}$ samples

The interplay between magnetism and crystal structures in three CaFe$_{2}$As$_{2}$ samples is studied. For the nonmagnetic quenched crystals, different crystalline domains with varying lattice parameters are found, and three phases (orthorhombic, tetragonal, and collapsed tetragonal) coexist between T$_{S}$ = 95 K and 45 K. Annealing of the quenched crystals at 350°C leads to a strain relief through a large (~1.3 %) expansion of the c-parameter and a small (~0.2 %) contraction of the a-parameter, and to local ~0.2 Å displacements at the atomic-level. This annealing procedure results in the most homogeneous crystals for which the antiferromagnetic and orthorhombic phase transitions occur at T$_{N}$/T$_{S}$ = 168(1) K. In the 700°C-annealed crystal, an intermediate strain regime takes place, with tetragonal and orthorhombic structural phases coexisting between 80 to 120 K. The origin of such strong shifts in the transition temperatures are tied to structural parameters. Importantly, with annealing, an increase in the Fe-As length leads to more localized Fe electrons and higher local magnetic moments on Fe ions. Synergistic contribution of other structural parameters, including a decrease in the Fe-Fe distance, and a dramatic increase of the c-parameter, which enhances the Fermi surface nesting in CaFe$_{2}$As$_{2}$, are also discussed.

cond-mat.supr-con↗

arXiv2011

Nitrogen Contamination in Elastic Neutron Scattering

Nitrogen gas accidentally sealed in a sample container produces various spurious effects in elastic neutron scattering measurements. These effects are systematically investigated and the details of the spurious scattering are presented.

cond-mat.mtrl-sci↗

arXiv2009

Evolution of the bulk properties, structure, magnetic order, and superconductivity with Ni doping in CaFe2-xNixAs2

Magnetization, susceptibility, specific heat, resistivity, neutron and x-ray diffraction have been used to characterize the properties of single crystalline CaFe2-xNixAs2 as a function of Ni doping for x varying from 0 to 0.1. The combined first-order structural and magnetic phase transitions occur together in the undoped system at 172 K, with a small decrease in the area of the a-b plane along with an abrupt increase in the length of the c-axis in the orthorhombic phase. With increasing x the ordered moment and transition temperature decrease, but the transition remains sharp at modest doping while the area of the a-b plane quickly decreases and then saturates. Warming and cooling data in the resistivity and neutron diffraction indicate hysteresis of ~2 K. At larger doping the transition is more rounded, and decreases to zero for x=0.06. The susceptibility is anisotropic for all values of x. Electrical resistivity for x = 0.053 and 0.06 shows a superconducting transition with an onset of nearly 15 K which is further corroborated by substantial diamagnetic susceptibility. For the fully superconducting sample there is no long range magnetic order and the structure remains tetragonal at all temperature, but there is an anomalous increase in the area of the a-b plane in going to low T. Heat capacity data show that the density of states at the Fermi level increases for x > 0.053 as inferred from the value of Sommerfeld coefficient. The regime of superconductivity is quite restrictive, with a maximum TC of 15 K and an upper critical field Hc2=14 T. Superconductivity disappears in the overdoped region.

cond-mat.supr-con↗