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Scott B. Lee

Publications and source records attributed to Scott B. Lee.

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Electron-affinity difference distributions as an organizing principle for superconductivity, enabling the discovery of PtPb$_3$Bi

Predicting the superconducting transition temperature ($T_c$) from crystal structure and composition remains a central challenge in condensed-matter physics, reflecting the absence of a broadly predictive framework connecting microscopic bonding to macroscopic quantum behavior. Here, we introduce $\mathcal{GP}$-$T_c$, an interpretable, structure- and chemistry-aware Gaussian process model that enables uncertainty-quantified $T_c$ prediction from experimentally accessible inputs. By encoding local bonding environments as graphlet histograms, we find that the predictive space collapses to a compact set of descriptors: the distribution of electron-affinity (EA) differences between neighboring atoms, together with interatomic distances and simple elemental features, suffices to predict $T_c$ across disparate superconducting families---identifying an overlooked chemical control parameter that underscores the essential role of local structure beyond composition-only approaches. Our results demonstrate that the EA differences serves as an accessible window into electronic structure providing a mechanism-agnostic physical basis that captures $T_c$ across conventional and unconventional families, including doped charge transfer insulators. $\mathcal{GP}$-$T_c$ reproduces the experimentally reported $T_c$ range of the infinite-layer nickelate Nd$_{0.8}$Sr$_{0.2}$NiO$_2$, and we predict and experimentally confirm superconductivity in stoichiometric PtPb$_3$Bi ($T_c \approx 3$~K). To facilitate broad community use, $\mathcal{GP}$-$T_c$ is made available through a web interface for crystal-structure-based prediction, and the same framework identifies additional high-priority superconducting candidates---including SrNiO$_2$ and K(PRh)$_2$---that provide concrete targets for ongoing and future experimental exploration.

cond-mat.supr-con

New Superconductors in the PtPb$_3$Bi Structure Type

The quest for new superconductors is of both fundamental and technological importance. Recently, an artificial intelligence method correctly predicted PtPb$_3$Bi to be a superconductor. In this work, we find superconductivity in the newly synthesized $M$Pb$_{4-x}$Bi$_x$ ($M$ = Au, Pd, and Rh), of which PtPb$_3$Bi is a member. When $M$ = Ni, whose radius is considerably smaller, the structure instead collapses into the different, Pb-substituted NiBi$_3$ type. Interestingly, the stoichiometric parameter $x$ shifts across the three compounds to keep the total valence electron count close to 20 per formula unit. The superconducting transitions occur at 4.9, 4.2, and 3.4 K, for $M$ = Au, Pd, and Rh, respectively. Using electrical resistivity, magnetization, and specific heat measurements, we establish the bulk nature of the superconducting state and determine the critical fields, characteristic length scales, and anisotropy ratios. All three compounds are moderately anisotropic type-II superconductors, with modest upper critical field anisotropies of $H_{c2}^{\parallel c}/H_{c2}^{\perp c} \approx 1.2$ to $1.5$. These results establish $M$Pb$_{4-x}$Bi$_x$ as a family of anisotropic superconductors and a platform for studying how site disorder and Pb-Bi mixing govern superconductivity in heavy-element intermetallics.

cond-mat.supr-con

New Crystal Structures Hide in Plain Sight: A Stress Test for AI-Guided Materials Discovery

New types of crystal structures are discovered only rarely, and the artificial intelligence (AI) models now reshaping materials discovery have so far produced new chemical compositions within known structural families rather than genuinely new structures. We report GdNiSn4 and LuNiSn4, intermetallics that adopt a previously unreported structure type, found not by computation but by exploratory synthesis. Single-crystal diffraction shows that the structure is an intergrowth of two known structural units. We then use this system as a benchmark for two leading generative models, MatterGen and DiffCSP++. For DiffCSP++, the benchmark is performed in its crystallographically constrained setting, using the required space-group and Wyckoff-position inputs. Under our sampling budget, neither model recovers the experimentally reported monoclinic structure within the structural-matching tolerance. The generated structures are evaluated without further structural relaxation using the nonmagnetic analog LuNiSn4, where we rule out 4f magnetism as the cause. Because the new structure is built from familiar building blocks, it should be derivable. We argue that encoding chemical reasoning, such as the stacking of known motifs, is a concrete path toward AI that can discover structurally novel materials.

cond-mat.mtrl-sci

Measuring the Hall effect in hysteretic materials

Measurement of the Hall effect is a ubiquitous probe for materials discovery, characterization, and metrology. Inherent to the Hall measurement geometry, the measured signal is often contaminated by unwanted contributions, so the data must be processed to isolate the Hall response. The standard approach invokes Onsager-Casimir reciprocity and antisymmetrizes the raw signal about zero applied magnetic field. In hysteretic materials this becomes nontrivial, since Onsager-Casimir relations apply only to microscopically reversible states. Incorrect antisymmetrization can lead to artifacts that mimic anomalous or topological Hall signatures. The situation is especially subtle when hysteresis loops are not centered at zero applied field, as in exchange-biased systems. A practical reference for generically extracting the Hall response in hysteretic materials is lacking. Here, using Co$_3$Sn$_2$S$_2$ as a bulk single-crystal model that can be prepared with or without exchange-biased hysteresis, we demonstrate two procedures that can be used to extract the Hall effect: (1) reverse-magnetic-field reciprocity and (2) antisymmetrization with respect to applied field. We then measure the Hall effect on CeCoGe$_3$, a noncentrosymmetric antiferromagnet which can be prepared to have asymmetric magnetization and magnetoresistance, and demonstrate how improper processing can generate artificial anomalous Hall signals. These methods are generic and can be applied to any conductor.

cond-mat.str-el

Tunable magnetotransport through kinetically hindered first-order phase transitions in an antiferromagnetic metal

Controllable multilevel resistance states are of interest for memory technologies like neuromorphic computing, but robust materials platforms toward such behavior remain limited. Here, we show that the non-centrosymmetric antiferromagnetic metal CeCoGe$_3$ suggests one such route through a kinetically hindered first-order magnetic transition. Cooling through the kinetically hindered first-order transition in an applied magnetic field produces a magnetic glass state in which high- and low-temperature magnetic phases coexist. The relative fraction of these phases can be controlled by the applied field in which the sample is cooled, and the electrical resistance is directly sensitive to that fraction. As a result, it is demonstrated that CeCoGe$_3$ supports stable multilevel resistive states. These results identify kinetically hindered first-order phase transitions as a promising route towards controllable multilevel magnetoresistive states.

cond-mat.str-el

Stripping Symmetry: Electrochemical Oxidation to a Superconducting Polar Metal in Au2Pb0.914P2

Polar metals and noncentrosymmetric superconductors are exceptionally rare, yet their broken inversion symmetry can give rise to emergent electronic phenomena including mixed singlet-triplet superconducting pairing. As only a few such materials have been found among known compounds, accessing new examples requires synthetic strategies that go beyond conventional crystal growth. Here, we use electrochemical topotactic deintercalation to remove Pb from the centrosymmetric parent compound Au$_2$PbP$_2$, producing the polar metal Au$_2$Pb$_{0.914}$P$_2$. Unlike conventional chemical doping, this transformation actively drives structural symmetry-breaking: the partial removal of Pb triggers a cooperative electronic and geometric rearrangement, mediated by a second-order Jahn-Teller effect and stereochemically active lone pairs, that locks the product into a polar, noncentrosymmetric superspace group Ama2(01g)ss0. We solve the complete (3+1)D modulated structure by synchrotron single-crystal X-ray diffraction and confirm the polar assignment through nonlinear electronic transport. Below T$_c$ = 1.52 K, Au$_2$Pb$_{0.914}$P$_2$ becomes a type-II superconductor whose heat capacity and AC susceptibility both exhibit power-law behavior, suggestive of a gap structure governed by the broken inversion symmetry of the host lattice. This work establishes electrochemical oxidation as a rational route to metastable noncentrosymmetric superconductors through chemically directed symmetry-breaking.

cond-mat.supr-con

Directionally Locked Heteroepitaxy with a Structurally Modulated van der Waals Material

Precise orientation of symmetry-mismatched epilayers on van der Waals (vdW) substrates via heteroepitaxy has commonly been achieved through surface treatment processes to accommodate weak interlayer registry and bonding strength, thereby limiting the range of material combinations for heterostructure design. In this study, we investigate the influence of lattice instabilities in a structurally modulated vdW TaCo2Te2 substrate on the growth and alignment of a symmetry-mismatched bulk CoxTey epilayer using in situ heating in a transmission electron microscope (TEM). We show that a Peierls-like lattice instability occurs in TaCo2Te2 at a transition temperature of ~523 K, which was corroborated by phonon calculations. Post-heat-treated samples reveal a thermally induced surface diffusion process and the dominant lateral growth of the CoxTey epilayer on the TaCo2Te2 vdW layers, as observed in cross-sectional TEM images. Temperature-dependent selected area electron diffraction (SAED) patterns reveal that the quasi-vdW CoxTey/TaCo2Te2 heterointerface acquires directional locking by aligning larger interlayer lattice mismatch along the lattice instability axis of TaCo2Te2, while preserving a strong lattice matching along the orthogonal direction. This heterostructure exhibits precise interlayer registry with one-dimensional lattice incommensuration along the lattice instability axis, resulting from structural distortion to accommodate lattice-mismatch strain. Moreover, the interfacial reconstruction of TaCo2Te2 back to the distorted phase stabilizes the lattice-locking of the quasi-vdW heterointerface at elevated temperatures. These findings encourage the expansion of material diversity for designing and predicting novel multi-dimensional heterostructures by leveraging lattice instabilities to guide epitaxy.

cond-mat.mtrl-sci

Collinear spin density wave state in distorted square-lattice GdNiSn$_4$

We characterize the magnetic ground state of the newly synthesized lanthanide intermetallic GdNiSn$_4$ via resonant elastic x-ray scattering measurements. This compound forms distorted square nets of Gd that initially order magnetically below 23 K followed by a lower temperature transition at 16 K. Our scattering data identify the ground state order as a single-$q$ incommensurate, collinear order that slides towards a commensurate wave vector above the 16 K transition. Magnetic symmetry analysis combined with azimuthal dependence resolves the ground state magnetic structure as a moment-modulated spin density wave state with Gd moments oriented parallel to the in-plane a-axis. We discuss connections between the observed magnetic order and electronic properties in this square-net compound.

cond-mat.str-el

Bonding Interactions Can Drive Topological Phase Transitions in a Zintl Antiferromagnetic Insulator

While $\sim$30% of materials are reported to be topological, topological insulators are rare. Magnetic topological insulators (MTI) are even harder to find. Identifying crystallographic features that can host the coexistence of a topological insulating phase with magnetic order is vital for finding intrinsic MTI materials. Thus far, most materials that are investigated for the determination of an MTI are some combination of known topological insulators with a magnetic ion such as MnBi$_2$Te$_4$. Motivated by the recent success of EuIn$_{2}$As$_{2}$, we investigate the role of chemical pressure on topologically trivial insulator, Eu$_5$In$_2$Sb$_6$ via Ga substitution. Eu$_5$Ga$_2$Sb$_6$ is predicted to be topological but is synthetically difficult to stabilize. We look into the intermediate compositions between Eu$_5$In$_2$Sb$_6$ and Eu$_5$Ga$_2$Sb$_6$ through theoretical works to explore a topological phase transition and band inversion mechanism. We attribute the band inversion mechanism to changes in Eu-Sb hybridization as Ga is substituted for In due to chemical pressure. We also synthesize Eu$_{5}$In$_{4/3}$Ga$_{2/3}$Sb$_{6}$, the highest Ga concentration in Eu$_{5}$In$_{2-x}$Ga$_{x}$Sb$_{6}$, and report the thermodynamic, magnetic, transport, and Hall properties. Overall, our work paints a picture of a possible MTI via band engineering and explains why Eu-based Zintl compounds are suitable for the co-existence of magnetism and topology.

cond-mat.mtrl-sci

Pb$_9$Cu(PO4)$_6$(OH)$_2$: Phonon bands, Localized Flat Band Magnetism, Models, and Chemical Analysis

In a series of recent reports, doped lead apatite (LK-99) has been proposed as a candidate ambient temperature and pressure superconductor. However, from both an experimental and theoretical perspective, these claims are largely unsubstantiated. To this end, our synthesis and subsequent analysis of an LK-99 sample reveals a multiphase material that does not exhibit high-temperature superconductivity. We study the structure of this phase with single-crystal X-ray diffraction (SXRD) and find a structure consistent with doped $\text{Pb}_{10}(\text{PO}_4)_6(\text{OH})_2$. However, the material is transparent which rules out a superconducting nature. From ab initio defect formation energy calculations, we find that the material likely hosts $\text{OH}^-$ anions, rather than divalent $\text{O}^{2-}$ anions, within the hexagonal channels and that Cu substitution is highly thermodynamically disfavored. Phonon spectra on the equilibrium structures reveal numerous unstable phonon modes. Together, these calculations suggest it is doubtful that Cu enters the structure in meaningful concentrations, despite initial attempts to model LK-99 in this way. However for the sake of completeness, we perform ab initio calculations of the topology, quantum geometry, and Wannier function localization in the Cu-dominated flat bands of four separate doped structures. In all cases, we find they are atomically localized by irreps, Wilson loops, and the Fubini-Study metric. It is unlikely that such bands can support strong superfluidity, and instead are susceptible to ferromagnetism (or out-of-plane antiferromagnetism) at low temperatures, which we find in ab initio studies. In sum, $\text{Pb}_{9}\text{Cu}(\text{PO}_4)_6(\text{OH})_2$ could more likely be a magnet, rather than an ambient temperature and pressure superconductor.

cond-mat.supr-con