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Sean M. Thomas

Publications and source records attributed to Sean M. Thomas.

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High-quality single crystals of the kagome metals Ni$_3$In and Ni$_3$Sn grown from Pb flux

The bilayer kagome metal Ni$_3$In has recently attracted attention due to the presence of a flat band located near the Fermi level, which has been associated with unconventional thermodynamic and electronic transport properties [Ye et al., Nat. Phys. 20, 610-614 (2024)]. However, further investigation of the intrinsic properties of this system has been hindered by the lack of large, high-quality single crystals. Here, we report the successful growth of Ni$_3$(In, Sn) single crystals using a Pb-flux technique. By optimizing the growth conditions, competing binary phases can be effectively suppressed, enabling the synthesis of single crystals with dimensions reaching several millimeters. We compare the physical properties of our Pb-flux-grown crystals to previously reported samples prepared by iodine-assisted chemical vapor transport and molecular beam epitaxy as well as to first-principles resistivity calculations. We find a significantly lower electrical resistivity in our crystals, in excellent agreement with calculations of resistivity from electron-phonon scattering, a sizeable non-saturating magnetoresistance, and a reduced Sommerfeld coefficient and magnetic susceptibility compared to previous experimental findings, which are likely related to differences in the Fermi level position. Our results establish Pb-flux growth as a reliable route for obtaining large single crystals of the bilayer kagome metals Ni$_3$(In, Sn) that are suitable for further thermodynamic and spectroscopic investigations of their intrinsic electronic and magnetic properties.

cond-mat.mtrl-sci

Directional Manipulation of a Staggered Charge Density Wave and Kondo Resonance in UTe2

UTe2 is a rare example of a correlated quantum material in which unconventional density wave orders, Kondo physics, spin-triplet pairing, and reentrant superconductivity coexist within the same electronic system. Its superconducting state develops out of a strongly correlated normal phase. The identification and control of competing or intertwined normal-state orders are thus central to elucidating the electronic landscape from which its superconductivity arises. Here, using scanning tunnelling microscopy (STM) in a vector magnetic field, we uncover a previously unreported staggered charge-density-wave (CDW) in high-quality UTe2 crystals and demonstrate its strong directional response to an external magnetic field: the staggered CDW is completely quenched by a modest 1.7 T field aligned with the quasi-one-dimensional uranium chain direction (a-axis), while remaining robust against fields along other crystallographic directions. This pronounced anisotropy is consistent with an orbital-driven mechanism that leads to a field-tuned quantum phase transition. Strikingly and counterintuitively, the same field orientation and strength concomitantly alter the hybridization gap and suppress the 5f Kondo resonance. Modelling indicates that this correlated evolution arises from a switch of the dominant hybridization channel from Te 5p- U 5f to U 6d- U 5f coupling, suggesting an intimate interplay between CDW and the Kondo effect. Our work establishes an effective tuning knob for the intertwined orders in UTe2 and provides evidence for orbital-selective Kondo hybridization, shedding light on its correlated normal state.

cond-mat.str-el

Random singlet physics in exchange disordered 2D triangular YbCu$_{1.14}$Se$_2$

Quantum spin liquid (QSL) phases exist in theory, but real candidate QSL materials are often extraordinarily sensitive to structural defects which disrupt the ground state. Here, we investigate candidate triangular QSL material YbCu$_{1.14}$Se$_2$ and discover the absence of magnetic order, but also no compelling evidence of a QSL ground state due to significant structural disorder. We instead look at the results through a lens of a 2-dimensional (2D) random singlet phase. We are able to match thermodynamic measurements using a phenomenological model of a distribution of singlet formation. YbCu$_{1.14}$Se$_2$ behaves strikingly similar to other disordered triangular lattice materials, suggesting universal behavior of random singlet formation in 2D frustrated systems.

cond-mat.str-el

Fabrication of microstructured devices of the unconventional superconductor CeCoIn5 for investigations of isolated grain boundaries

Grain boundaries are critical for determining the functionality of polycrystalline materials. Here we present on the structural $\&$ transport properties of grain boundaries in the unconventional superconductor CeCoIn$_5$. We provide a detailed recipe for the fabrication of isolated grain boundary devices from of as-grown polycrystalline samples of CeCoIn$_5$. Electron backscattered diffraction imaging of polycrystalline CeCoIn$_5$ samples reveals an abundance of $90^\circ$ misorientation grain boundaries suggesting a preferential nucleation of CeCoIn$_5$ grains with 90$^\circ$ misorientation over a random distribution of grain orientations. Transport measurements across grain boundary devices establish coherence of superconductivity and allows us to establish a lower bound on the critical current density for the grain boundaries. Our work opens new possibilities for fabrication of quantum devices such as Josephson-junctions out of bulk unconventional superconducting materials.

cond-mat.supr-con

Exploring the apparent violation of the Mott relation in a noncentrosymmetric kagome ferromagnet

In magnetic topological materials, time-reversal symmetry breaking gives rise to topological point and line nodes with distinctive signatures in the anomalous Hall and anomalous Nernst conductivity that satisfy the well-known Mott relation. However, this relationship can fail for doping-dependent transport measurements of materials with complex magnetism, topology, and electronic correlations. In this work, we present transport measurements of the correlated topological metal UCoAl doped with Ru, which appear to violate the Mott relation. We develop a model that captures the evolution of Stoner magnetism and topological Weyl points as a function of doping. Using this model, we show how the correlated flat band in this material pins the Weyl points to the Fermi energy, and demonstrate how this explains the unusual doping-dependent behavior of the anomalous Hall and anomalous Nernst conductivities in this material, while the Mott relation is in fact satisfied at each doping level.

cond-mat.str-el

Tracking flat bands via phonon-mediated interband scattering

Flat-band (FB) materials have emerged as promising platforms for exploring exotic quantum phases. While numerous candidates have recently been identified through spectroscopic techniques such as angle-resolved photoemission spectroscopy, central challenges remain on how to tune FBs towards the Fermi level $E_F$ and to understand their impact on low-energy excitations probed in electronic transport experiments. Here, we show that, by attributing the temperature dependence of the electrical resistivity at elevated temperatures to electron-phonon interband scattering, one can infer the position of FBs near $E_F$ across diverse material classes. As charge carriers scatter off phonons, interband transitions into FB states lead to distinctive sub- or superlinear resistivity at elevated temperatures, governed by the proximity of the FB to $E_F$. Our phenomenological model captures these universal transport behaviors observed across several recently studied FB compounds and offers a simple, broadly applicable method for detecting flat bands.

cond-mat.str-el

Putative excitonic insulating state in narrow-gap semiconductor La$_3$Cd$_2$As$_6$

Excitonic insulators are electronically-driven phases of matter characterized by the spontaneous condensation of electron-hole pairs. Here we show that La$_3$Cd$_2$As$_6$ undergoes a transition at $T_{0}=278$ K to a highly insulating state with no accompanying structural transition. We observe quasi-two-dimensional electrical transport and charge fluctuations consistent with an electronic transition enabled by enhanced Coulomb interactions. Density functional theory calculations are unable to replicate the insulating ground state. Our results support the opening of a gap by excitonic effects at $T_{0}$, placing La$_3$Cd$_2$As$_6$ as a rare example of a bulk excitonic insulator.

cond-mat.str-el

Hydrostatic pressure studies on non-superconducting UTe2

We report the temperature-pressure phase diagram of a UTe$_2$ single crystal that does not undergo a bulk superconducting transition but shows filamentary superconductivity with a critical transition temperature of 1 K at ambient pressure. Electrical-resistivity measurements reveal that the evolution of the filamentary superconducting state under pressure resembles the behavior observed in previous reports on bulk superconducting samples. AC calorimetry, however, does not show evidence for either bulk superconductivity or magnetism for pressures up to 1.6 GPa. Our results highlight the role of inhomogeneity in chemical-vapor-transport-grown UTe$_2$ samples and serve as a cautionary tale when probing electrical resistivity alone.

cond-mat.str-el

Magnetic polaron formation in EuZn$_2$P$_2$

Colossal magnetoresistance (CMR) has been observed across many Eu$^{2+}$-based materials; however, its origin is not completely understood. Here we investigate the antiferromagnetic insulator EuZn$_2$P$_2$ through single crystal x-ray diffraction, transmission electron microscopy, electrical transport, magnetization, dilatometry, and electron spin resonance measurements complemented by density functional theory calculations. Our electrical resistivity data reveal a large negative magnetoresistance, $MR = [R(H)-R(0)]/R(0)$, that reaches $MR = -99.7\%$ at 9~T near the antiferromagnetic ordering temperature $T_N=23\ \text{K}$. Dilatometry measurements show an accompanying field-induced lattice strain. Additionally, Eu$^{2+}$ electron spin resonance reveals a strong ferromagnetic exchange interaction between Eu$^{2+}$ and conduction electrons. Our experimental results in EuZn$_2$P$_2$ are consistent with a magnetic polaron scenario and suggest magnetic polaron formation as a prevailing explanation of CMR in Eu$^{2+}$-based compounds.

cond-mat.str-el

Local aging effects in PuB$_{4}$: Growing inhomogeneity and slow dynamics of local-field fluctuations probed by $^{239}$Pu NMR

The effect of self-irradiation damage can influence many properties of a radioactive material. Actinide materials involving the decay through alpha radiation have been frequently studied using techniques such as transport, thermodynamics, and x-ray diffraction. The use of nuclear magnetic resonance (NMR) spectroscopy to study such effects, however, has seen relatively little attention. Here, we use $^{239}$Pu NMR to study the local influence of self-damage in a single crystal of the candidate topological insulator plutonium tetraboride (PuB$_{4}$). We first characterize the anisotropy of the $^{239}$Pu resonance in a single crystal and confirm the local axial site symmetry inferred from previous polycrystalline measurements. Aging effects are then evaluated over the timeframe of six years. We find that, though the static NMR spectra may show a slight modulation in their shape, their field-rotation pattern reveals no change in Pu local site symmetry over time, suggesting that aging has a surprisingly small impact on the spatial distribution of the static hyperfine field. By contrast, aging has a prominent impact on the NMR relaxation processes and signal intensity. Specifically, aging-induced damage manifests itself as an increase in the spin-lattice relaxation time $T_{1}$, an increased distribution of $T_{1}$, and a signal intensity that decreases linearly by 20 % per year. The spin-spin relaxation time $T_{2}$ in the aged sample shows a strong variation across the spectrum as well as a drastic shortening towards lower temperature, suggesting growth of slow fluctuations of the hyperfine field that are linked to radiation-damage-induced inhomogeneity and could be responsible for the signal wipeout that develops over time.

cond-mat.mtrl-sci

Electronic and magnetic phase diagrams of Kitaev quantum spin liquid candidate Na$_2$Co$_2$TeO$_6$

The 3$d^7$ Co$^{2+}$-based insulating magnet \NCTO{} has recently been reported to have strong Kitaev interactions on a honeycomb lattice, and is thus being considered as a Kitaev quantum spin liquid candidate. However, due to the existence of other types of interactions, a spontaneous long-range magnetic order occurs. This order is suppressed by applied magnetic fields leading to a succession of phases and ultimately saturation of the magnetic moments. The precise phase diagram, the nature of the phases, and the possibility that one of the field-induced phases is a Kitaev quantum spin liquid phase are still a matter of debate. Here we measured an extensive set of physical properties to build the complete temperature-field phase diagrams to magnetic saturation at 10 T for magnetic fields along the $a$- and $a^*$-axes, and a partial phase diagram up to 60 T along $c$. We probe the phases using magnetization, specific heat, magnetocaloric effect, magnetostriction, dielectric constant, and electric polarization, which is a symmetry-sensitive probe. With these measurements we identify all the previously incomplete phase boundaries and find new high-field phase boundaries. We find strong magnetoelectric coupling in the dielectric constant and moderate magnetostrictive coupling at several phase boundaries. Furthermore, we detect the symmetry of the magnetic order using electrical polarization measurements under magnetic fields. Based on our analysis, the absence of electric polarization under zero or finite magnetic field in any of the phases or after...

cond-mat.str-el

Sudden adiabaticity entering field-induced state in UTe2

There has been a recent surge of interest in UTe$_2$ due to its unconventional magnetic field (H) reinforced spin-triplet superconducting phases persisting at fields far above the simple Pauli limit for H $\parallel$ [010]. Magnetic fields in excess of 35 T then induce a field-polarized magnetic state via a first-order-like phase transition. More controversially, for field orientations close to H $\parallel$ [011] and above 40 T, electrical resistivity measurements suggest that a further superconducting state may exist. However, no Meissner effect or thermodynamic evidence exists to date for this phase making it difficult to exclude a simple low-resistance metallic state. In this paper, we describe a study using thermal, electrical, and magnetic probes in magnetic fields of up to 55 T applied between the [010] ($b$) and [001] ($c$) directions. Our MHz conductivity data reveal the field-induced state of low or vanishing electrical resistance; simultaneous magnetocaloric effect measurements (i.e. changes in sample temperature due to changing magnetic field), show the first definitive evidence for adiabaticity and thermal behavior characteristic of bulk field-induced superconductivity.

cond-mat.supr-con

Thermal Equation of State of U$_6$Fe from Experiments and Calculations

Actinide-bearing intermetallics display unusual electronic, magnetic, and physical properties which arise from the complex behavior of their 5$f$ electron orbitals. Temperature ($T$) effects on actinide intermetallics are well studied, but high pressure ($P$) properties and phase stabilities are known for only a handful of compositions. Furthermore, almost no data exist for simultaneous high $P$ and high $T$. We performed ambient-$T$ diamond anvil cell X-ray diffraction experiments to study the behavior of the intermetallic U$_6$Fe upon compression up to 82 GPa. U$_6$Fe remains stable in the tetragonal $I4/mcm$ structure over this pressure range. We also performed ambient $P$, low-$T$ diffraction and heat capacity measurements to constrain U$_6$Fe's thermal behavior. These data were combined with calculations and fitted to a Mie-Gruneisen/Birch-Murnaghan thermal equation of state with the following parameter values at ambient $P$: bulk modulus $B_0$ = 124.0 GPa, pressure derivative $B'_0$ = 5.6, Gruneisen parameter $Γ_0$ = 2.028, volume exponent $q$ = 0.934, Debye temperature $θ_0$ = 175 K, and unit cell volume $V_0$ = 554.4 angstrom$^3$. We report $T$-dependent thermal expansion coefficients and bond lengths of U$_6$Fe, which demonstrate the anisotropic compressibility and negative thermal expansion of the crystallographic $c$ axis. Additionally, density-functional theory calculations indicate increased delocalization of U$_6$Fe bonds at high $P$.

cond-mat.mtrl-sci

Superconductivity by alloying the topological insulator SnBi2Te4

Alloying indium into the topological insulator Sn1-xInxBi2Te4 induces bulk superconductivity with critical temperatures Tc up to 1.85 K and upper critical fields up to about 14 kOe. This is confirmed by electrical resistivity, heat capacity, and magnetic susceptibility measurements. The heat capacity shows a discontinuity at Tc and temperature dependence below Tc consistent with weak coupling BCS theory, and suggests a superconducting gap near 0.25 meV. The superconductivity is type-II and the topological surface states have been verified by photoemission. A simple picture suggests analogies with the isostructural magnetic topological insulator MnBi2Te4, in which a natural heterostructure hosts complementary properties on different sublattices, and motivates new interest in this large family of compounds. The existence of both topological surface states and superconductivity in Sn1-xInxBi2Te4 identifies these materials as promising candidates for the study of topological superconductivity.

cond-mat.supr-con

Interwoven atypical quantum states in CeLiBi$_2$

We report the discovery of CeLiBi$_2$, the first example of a material in the tetragonal Ce$TX_2$ ($T$ = transition metal; $X$ = pnictogen) family wherein an alkali cation replaces the typical transition metal. Magnetic susceptibility and neutron powder diffraction measurements are consistent with a crystal-field $Γ_6$ ground state Kramers doublet that orders antiferromagnetically below $T_N = 3.4$ K with an incommensurate propagation wave vector ${\bf{k}} = (0, 0.0724(4), 0.5)$ that generates a nanometric modulation of the magnetic structure. The best model of the ordered state is an elliptical cycloid with Ce moments primarily residing in the $ab$ plane. This is highly unusual, as all other $Γ_6$ Ce$TX_2$ members order ferromagnetically. Further, we observe an atypical hard-axis metamagnetic transition at $2$ T in magnetostriction, magnetization, and resistivity measurements. CeLiBi$_2$ is a rare example of a highly conductive material with dominant skew scattering leading to a large anomalous Hall effect. Quantum oscillations with five frequencies arise in magnetostriction and magnetic susceptibility data to $T = 30$ K and $μ_0H = 55$ T, which indicate small Fermi pockets of light carriers with effective masses as low as 0.07$m_e$. Density functional theory calculations indicate that square-net Dirac-like Bi$-p$ bands are responsible for these ultralight carriers. Together, our results show that CeLiBi$_2$ enables multiple atypical magnetic and electronic properties in a single clean material.

cond-mat.str-el

Predicting electrical conductivity in Cu/Nb composites: a combined model-experiment study

The generation of high magnetic fields requires materials with high electric conductivity and good strength properties. Cu/Nb composites are considered to be good candidates for this purpose. In this work we aim to predict, from theory, the dependence of electric conductivity on the microstructure, most notably on the layer thickness and grain sizes. We also conducted experiments to calibrate and validate our simulations. Bimetal interfaces and grain boundaries are confirmed to have the largest impact on conductivity in this composite material. In this approach, a distribution of the layer thickness is accounted for in order to better model the experimentally observed microstructure. Because layer thicknesses below the mean free path of Cu significantly degrade the conductivity, an average layer thickness larger than expected may be needed to meet conductivity requirements in order to minimize these smaller layers in the distribution. We also investigate the effect of variations in volume fraction of Nb and temperature on the material's conductivity.

cond-mat.mtrl-sci

Thermodynamic and electrical transport properties of UTe$_2$ under uniaxial stress

Despite intense experimental efforts, the nature of the unconventional superconducting order parameter of UTe$_2$ remains elusive. This puzzle stems from different reported numbers of superconducting transitions at ambient pressure, as well as a complex pressure-temperature phase diagram. To bring new insights into the superconducting properties of UTe$_2$, we measured the heat capacity and electrical resistivity of single crystals under compressive uniaxial stress $σ$ applied along different crystallographic directions. We find that the critical temperature $T_{\rm c}$ of the single observed bulk superconducting transition decreases with $σ$ along $[100]$ and $[110]$ but increases with $σ$ along $[001]$. Aside from its effect on $T_{\rm c}$, we notice that $c$-axis stress leads to a significant piezoresistivity, which we associate with the shift of the zero-pressure resistivity peak at $T^\star \approx 15\, \rm K$ to lower temperatures under stress. Finally, we show that an in-plane shear stress $σ_{xy}$ does not induce any observable splitting of the superconducting transition over a stress range of $σ_{xy}\approx 0.17 \, \rm GPa$. This result suggests that the superconducting order parameter of UTe$_2$ may be single-component at ambient pressure.

cond-mat.supr-con

Robust narrow-gap semiconducting behavior in square-net La$_{3}$Cd$_{2}$As$_{6}$

ABSTRACT: Narrow-gap semiconductors are sought-after materials due to their potential for long-wavelength detectors, thermoelectrics, and more recently non-trivial topology. Here we report the synthesis and characterization of a new family of narrow-gap semiconductors, $R$$_{3}$Cd$_{2}$As$_{6}$ ($R=$ La, Ce). Single crystal x-ray diffraction at room temperature reveals that the As square nets distort and Cd vacancies order in a monoclinic superstructure. A putative charge-density ordered state sets in at 279~K in La$_{3}$Cd$_{2}$As$_{6}$ and at 136~K in Ce$_{3}$Cd$_{2}$As$_{6}$ and is accompanied by a substantial increase in the electrical resistivity in both compounds. The resistivity of the La member increases by thirteen orders of magnitude on cooling, which points to a remarkably clean semiconducting ground state. Our results suggest that light square net materials within a $I4/mmm$ parent structure are promising clean narrow-gap semiconductors.

cond-mat.mtrl-sci