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Caitlin S. Kengle

Publications and source records attributed to Caitlin S. Kengle.

9 recordsLinked to original sources

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.

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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.

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Measurement of the dynamic charge susceptibility near the charge density wave transition in ErTe$_3$

A charge density wave (CDW) is a phase of matter characterized by a periodic modulation of the valence electron density accompanied by a distortion of the lattice structure. The microscopic details of CDW formation are closely tied to the dynamic charge susceptibility, $χ(q,ω)$, which describes the behavior of electronic collective modes. Despite decades of extensive study, the behavior of $χ(q,ω)$ in the vicinity of a CDW transition has never been measured with high energy resolution ($\sim$meV). Here, we investigate the canonical CDW transition in ErTe$_3$ using momentum-resolved electron energy loss spectroscopy (M-EELS), a technique uniquely sensitive to valence band charge excitations. Unlike phonons in these materials, which undergo conventional softening due to the Kohn anomaly at the CDW wavevector, the electronic excitations display purely relaxational dynamics that are well described by a diffusive model. The diffusivity peaks around 250 K, just below the critical temperature. Additionally, we report, for the first time, a divergence in the real part of $χ(q,ω)$ in the static limit ($ω\rightarrow 0$), a phenomenon predicted to characterize CDWs since the 1970s. These results highlight the importance of energy- and momentum-resolved measurements of electronic susceptibility and demonstrate the power of M-EELS as a versatile probe of charge dynamics in materials.

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Evidence for incommensurate antiferromagnetism in nonsymmorphic UPd$_{0.65}$Bi$_2$

The intersection between nonsymmorphic symmetry and electronic correlations has emerged as a platform for topological Kondo semimetallic states and unconventional spin textures. Here we report the synthesis of nonsymmorphic UPd$_{0.65}$Bi$_2$ single crystals and their structural, electronic, magnetic, and thermodynamic properties. UPd$_{0.65}$Bi$_2$ orders antiferromagnetically (AFM) below $T_N\simeq$ 161 K as evidenced by a sharp cusp in magnetic susceptibility, a second-order phase transition in specific heat, and an upturn in electrical resistivity, which suggests an incommensurate AFM structure that deviates from the A-type magnetism typically observed in this class of materials. Across $T_N$, Hall effect measurements reveal a change from electron-dominated to hole-dominated transport, which points to a sharp reconstruction in the electronic structure at $T_N$. Upon further cooling, a first-order transition is observed at $T_1 \simeq 30 $K in magnetic susceptibility and heat capacity but not in electrical resistivity or Hall measurements, which indicates a small change in the AFM structure that does not affect the electronic structure. Our specific heat data reveal a small Sommerfeld coefficient ($γ\simeq$13 mJmol$^{-1}$K$^{-2}$), consistent with localized 5$f$ electrons. Our results indicate that UPd$_{0.65}$Bi$_2$ hosts weak electronic correlations and is likely away from a Kondo semimetallic state. Low-temperature magnetization measurements show that the AFM structure is remarkably stable to 160 kOe and does not undergo any field-induced transitions. Neutron diffraction and magnetization experiments at higher fields would be valuable to probe the presence of unconventional spin textures.

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Conformally invariant charge fluctuations in a strange metal

The strange metal is a peculiar phase of matter in which the electron scattering rate, $τ^{-1} \sim k_B T/\hbar$, which determines the electrical resistance, is universal across a wide family of materials and determined only by fundamental constants. In 1989, theorists hypothesized that this universality would manifest as scale-invariant behavior in the dynamic charge susceptibility, $χ''(q,ω)$. Here, we present momentum-resolved inelastic electron scattering measurements of the strange metal Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ showing that the susceptibility has the scale-invariant form $χ''(q,ω) = T^{-ν} f(ω/T)$, with exponent $ν= 0.93$. We find the response is consistent with conformal invariance, meaning the dynamics may be thought of as occurring on a circle of radius $1/T$ in imaginary time, characterized by conformal dimension $Δ= 0.05$. Our study indicates that the strange metal is a universal phenomenon whose properties are not determined by microscopic properties of a particular material.

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Absence of a bulk charge density wave signature in x-ray measurements of UTe$_2$

The long-sought pair density wave (PDW) is an exotic phase of matter in which charge density wave (CDW) order is intertwined with the amplitude or phase of coexisting, superconducting order \cite{Berg2009,Berg2009b}. Originally predicted to exist in copper-oxides, circumstantial evidence for PDW order now exists in a variety of materials. Recently, scanning tunneling microscopy (STM) studies have reported evidence for a three-component charge density wave (CDW) at the surface of the heavy-fermion superconductor, UTe$_2$, persisting below its superconducting transition temperature. Here, we use hard x-ray diffraction measurements on crystals of UTe$_2$ at $T = 1.9$ K and $12$ K to search for a bulk signature of this CDW. Using STM measurements as a constraint, we calculate the expected locations of CDW superlattice peaks, and sweep a large volume of reciprocal space in search of a signature. We failed to find any evidence for a CDW near any of the expected superlattice positions in many Brillouin zones. We estimate an upper bound on the CDW lattice distortion of $u_{max} \lesssim 4 \times 10^{-3} \mathrmÅ$. Our results suggest that the CDW observed in STM is either purely electronic, somehow lacking a signature in the structural lattice, or is restricted to the material surface.

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Absence of bulk charge density wave order in the normal state of UTe$_2$

A spatially modulated superconducting state, known as pair density wave (PDW), is a tantalizing state of matter with unique properties. Recent scanning tunneling microscopy (STM) studies revealed that spin-triplet superconductor UTe$_2$ hosts an unprecedented spin-triplet, multi-component PDW whose three wavevectors are indistinguishable from a preceding charge-density wave (CDW) order that survives to temperatures well above the superconducting critical temperature, $T_{c}$. Whether the PDW is the mother or a subordinate order remains unsettled. Here, based on a systematic search for bulk charge order above $T_{c}$ using resonant elastic X-ray scattering (REXS), we show that the structure factor of charge order previously identified by STM is absent in the bulk within the sensitivity of REXS. Our results invite two scenarios: either the density-wave orders condense simultaneously at $T_{c}$ in the bulk, in which case PDW order is likely the mother phase, or the charge modulations are restricted to the surface.

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Anharmonic multiphonon origin of the valence plasmon in SrTi1-xNbxO3

Doped SrTi1-xNbxO3 exhibits superconductivity and a mid-infrared optical response reminiscent of copper-oxide superconductors. Strangely, its plasma frequency, omega_p, increases by a factor of ~3 when cooling from 300 K to 20 K, without any accepted explanation. Here, we present momentum-resolved electron energy loss spectroscopy (M-EELS) measurements of SrTi1-xNbxO3 at nonzero momentum, q. We find that the infrared feature previously identified as a plasmon is present at large q in insulating SrTiO3, where it exhibits the same temperature dependence and may be identified as an anharmonic, multiphonon background. Doping with Nb increases its peak energy and total spectral weight, drawing this background to lower q where it becomes visible in IR optics experiments. We conclude that the "plasmon" in doped SrTi1-xNbxO3 is not a free-carrier mode, but a composite excitation that inherits its unusual properties from the lattice anharmonicity of the insulator.

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Incommensurate magnetic orders and topological Hall effect in the square-net centrosymmetric EuGa$_2$Al$_2$ system

Neutron diffraction on the centrosymmetric square-net magnet EuGa$_2$Al$_2$ reveals multiple incommensurate magnetic states (AFM1,2,3) in zero field. In applied field, a new magnetic phase (A) is identified from magnetization and transport measurements, bounded by two of the $μ_0H$~=~0 incommensurate magnetic phases (AFM1,helical and AFM3, cycloidal) with different moment orientations. Moreover, magneto-transport measurements indicate the presence of a topological Hall effect, with maximum values centered in the A phase. Together, these results render EuGa$_2$Al$_2$ a material with non-coplanar or topological spin texture in applied field. X-ray diffraction reveals an out-of-plane (OOP) charge density wave (CDW) below $T_{CDW} \sim$ 50 K while the magnetic propagation vector lies in plane below $T_N$ = 19.5 K. Together these data point to a new route to realizing in-plane non-collinear spin textures through an OOP CDW. In turn, these non-collinear spin textures may be unstable against the formation of topological spin textures in an applied field.

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