arXiv subjects

Paul C. Canfield

Publications and source records attributed to Paul C. Canfield.

At least 37 records · Page 2Linked to original sources

arXiv2026

Suppression of the valence transition in solution-grown single crystals of Eu$_2$Pt$_6$Al$_{15}$

The study of Eu intermetallic compounds has allowed the exploration of valence fluctuations and transitions in 4f electron systems. Recently, a Eu$_2$Pt$_6$Al$_{15}$ phase synthesized by arc-melting followed by a thermal treatment was reported [M. Radzieowski \textit{et al.}, J Am Chem Soc 140(28), 8950-8957 (2018)], which undergoes a transition upon cooling below 45~K that was interpreted as a valence transition from Eu$^{2+}$ to Eu$^{3+}$. In this paper, we present the discovery of another polymorph of Eu$_2$Pt$_6$Al$_{15}$ obtained by high temperature solution growth, which presents different physical properties than the arc-melted polycrystalline sample. Despite the similarities in crystal structure and chemical composition, the Eu valence transition is almost fully suppressed in the solution-grown crystals, allowing the moments associated with the Eu$^{2+}$ state to order antiferromagnetically at around 14~K. A detailed analysis of the crystal structure using single crystal X-ray diffraction reveals that, although the solution grown crystals are built from the same constituent layers as the arc-melted samples, these layers present a different stacking. The effect of different thermal treatments is also studied. Different anneal procedures did not result in significant changes in the intrinsic properties, and only by arc-melting and quenching the crystals we were able to convert them into the previously reported polymorph.

cond-mat.mtrl-sci↗

arXiv2026

Quantum critical point followed by Kondo-like behavior due to Cu substitution in itinerant, antiferromagnet ${\text{La}_{2}\text{(Cu}_{x}\text {Ni}_{1-x})_7}$

$\text{La}_2 \text{Ni}_7$ is an itinerant magnetic system with a small ordered moment of $\sim$ 0.1 $μ_{B}/\text{Ni}$ and a series of antiferromagnetic (AFM) transitions at $T_1$ = 61.0 K, $T_2$ = 56.5 K and $T_3$ = 42.2 K. $M(H)$, and $ρ(H)$ isotherms as well as constant field $M(T)$ and $ρ(T)$ measurements on single crystalline samples manifest a complex, anisotropic $H-T$ phase diagram with multiple phase lines. Here we present the growth and characterization of single crystals of the ${\text{La}_{2}\text{(Cu}_{x}\text {Ni}_{1-x})_7}$ series for 0 $\leq x \leq$ 0.181. We measured powder x-ray diffraction, and composition, as well as anisotropic $R(H,T)$, $M(H,T)$, and $C_p(T)$ on these single crystals. Using the measured data, we infer a $(T-x)$ phase diagram to study the evolution of the AFM ordering upon Cu substitution. For ${0 \leq x \leq 0.097}$, the system remains magnetically ordered at base temperature with $x \leq$ 0.012, showing signs of multiple AFM ordering temperatures. For the higher substitution levels, ${0.125 \leq x \leq 0.181}$, there are no signatures of magnetic ordering, but anomalous features in $R(T)$ and $C_p(T)$ data are observed which are consistent with the Kondo effect in this system. The intermediate $x$ = 0.105 sample lies between the magnetic ordered and the Kondo regime and is in the vicinity of the AFM-quantum critical point (QCP). Thus, ${\text{La}_{2}\text{(Cu}_{x}\text {Ni}_{1-x})_7}$ is an example of a small moment system that can be tuned through a QCP. Given these data combined with the fact that the $\text{La}_2 \text{Ni}_7$ structure has kagome-like, Ni-sublattices running perpendicular to the crystallographic $c$ axis, and a predicted $3d$-electron flat band that contributes to the density of states near the Fermi energy, ${\text{La}_{2}\text{(Cu}_{x}\text {Ni}_{1-x})_7}$ becomes a promising system to host and study exotic physics.

cond-mat.str-el↗

arXiv2025

Structural phase transitions in the van der Waals ferromagnets Fe$_x$Pd$_{y}$Te$_2$

Here, we provide a detailed study of the crystal structure and physical properties of the recently discovered vdW ferromagnet FePd$_2$Te$_2$. We find this compound has a relatively wide width of formation, and grow single crystals with compositions Fe$_x$Pd$_{y}$Te$_2$ where $x$ ranges from 0.9 to 1.1 and $y$ from 1.8 to 2.5, respectively. Temperature-dependent X-ray diffraction and transport measurements reveal that a first-order structural transition occurs in the range of $T$ = 360-420 K. Above the transition, the compounds with Pd fraction $y>2$ adopt a disordered derivative of the tetragonal FeTe structure, with the Fe layer showing mixed Fe/Pd occupancy and the extra Pd atoms partially occupying interstitial sites. Below 370 K, the structure is incommensurately modulated. For $y<2$, the composition Fe$_{1.1}$Pd$_{1.8}$Te$_2$ has monoclinic symmetry at room temperature that is consistent with the reported structure of FePd$_2$Te$_2$. This phase undergoes a structural transition at 420 K for which the high temperature structure is yet to be determined; however, based on the similarities with the $y > 2$ compounds, we speculate that this composition also adopts a tetragonal structure above 420\,K. All compounds investigated in the Fe$_x$Pd$_{y}$Te$_2$ series show metallic behavior, with magnetic characterization indicating that they are easy-plane, hard, ferromagnets with $T_C$ spanning 98--180 K. Both the critical temperature for the structural transition and the Curie temperature are moderately suppressed with increasing Pd fraction $y$ and corresponding decreasing Fe fraction $x$, indicating that synthetic control over $x$ and $y$ paves way for the further exploration of these compounds.

cond-mat.str-el↗

arXiv2025

Hidden symmetry-breaking in a kagome Ising ferromagnet

Kagome metals can host unconventional electronic phenomena that emerge from their frustrated lattice geometry and associated band topology. Correlated electronic orders, such as charge-density waves and superconductivity, are observed to intertwine with subtle time-reversal symmetry breaking whose microscopic origin is not currently understood. Here, we provide evidence for such time-reversal symmetry breaking in the kagome metal TbV$_6$Sn$_6$ arising from staggered magnetic moments within the kagome layers. TbV$_6$Sn$_6$ consists of metallic V kagome layers separated by Tb triangular layers that host Ising ferromagnetic order. Deep in the ferromagnetic state, the Tb Ising doublet ground state should display a single, dispersionless spin-flip excitation. Instead, inelastic neutron scattering reveals two sharp excitations associated with inequivalent Tb sites, demonstrating that a symmetry-broken phase coexists with Ising ferromagnetism. No additional structural or magnetic phase transitions are detected, and first-principles calculations rule out lattice distortions as the origin of the splitting. We attribute this effect to time-reversal symmetry breaking encoded by small V moments that couple to the Tb sublattice and leave a measurable spectral fingerprint. Our results establish rare-earth local moment spectroscopy as a sensitive probe of subtle broken symmetries and highlight an unexpected interplay between kagome magnetism and rare-earth local moment magnetism.

cond-mat.str-el↗

arXiv2025

Nature of quantum criticality in the Ising ferromagnet TbV$_6$Sn$_6$

TbV$_6$Sn$_6$ is a topological metal where ferromagnetic Tb ions with strong uniaxial magnetic anisotropy interact with V kagome layers. Inelastic neutron scattering (INS) measurements show that the Tb ions adopt an Ising doublet ground state. Here, we consider whether a transverse magnetic field can drive TbV$_6$Sn$_6$ toward a quantum critical point, providing a rare example of transverse-field Ising criticality in a metallic compound. High-field magnetization measurements reveal a first-order-like spin-reorientation transition at 25.6 T. Our INS-based magnetic model finds that this is caused by an avoided crossing of an excited-state singlet with the ground-state doublet. Surprisingly, our model predicts that quantum critical and tricritical points are accessible within the range of experimentally determined model parameters and may be reached by varying the direction of an applied magnetic field.

cond-mat.str-el↗

arXiv2025

Competing Magnetic Phases in Li-Fe-Ge Kagome Systems

Competing interlayer magnetic interactions in kagome magnets can lead to diverse magnetic phases, which enable various promising topological or quantum material properties. Here, the electronic structure and magnetic properties have been studied using first-principles calculations for the LiFe$_6$Ge$_6$, LiFe$_6$Ge$_4$, and LiFe$_6$Ge$_5$ compounds sharing the kagome Fe$_3$Ge layer motif but with different interlayer arrangements. For LiFe$_6$Ge$_4$ and LiFe$_6$Ge$_5$, the predicted magnetic ground states are collinear antiferromagnetic (AFM) states involving a mix of ferromagnetic (FM) and AFM interlayer orientations. Whereas for LiFe$_6$Ge$_6$, an incommensurate cycloidal spin spiral is stabilized as a ground state, being close to a collinear A-type AFM state. The analysis of magnetic RKKY exchange coupling confirms the results of electronic structure calculations. The values of atomic magnetic moments are in good agreement with existing experimental estimations. Our experiments on LiFe$_6$Ge$_6$ single crystals have observed AFM ordering at ~540 K and transition to another magnetic phase, with a small FM component (possibly with spin canting), below ~270 K. Thus, our theory and experiment suggest the existence and sequence of collinear and noncollinear magnetic states in kagome LiFe$_6$Ge$_6$. Our findings provide a platform for exploring various novel magnetic phases and associated unconventional or topological magnetism.

cond-mat.mtrl-sci↗

arXiv2025

Electronic band structure from quasiparticle interference and Landau quantization in WTe$_2$

WTe$_2$ stands out as a semimetal presenting Fermi level quantum oscillations in most measured quantities under magnetic fields. However, the electronic band structure above and below the Fermi level has not been explored completely. Here we study the electronic band structure of WTe$_2$ by quasiparticle interference with Scanning Tunneling Microscopy (STM) and observe, with the support of Density Functional Theory (DFT), the electron and hole bands around the Fermi level. We also report on the observation of Landau quantization in atomically resolved measurements and discuss the possible connection with band structure calculations.

cond-mat.mes-hall↗

arXiv2025

Intrinsic Layer-Dependent Surface Energy and Exfoliation Energy of van der Waals Materials

Stacking and twisting 2D van der Waals (vdW) layers have become versatile platforms to tune electron correlation. These platforms rely on exfoliating vdW materials down to a single and few vdW layers. We calculate the intrinsic layer-dependent surface and exfoliation energies of typical vdW materials such as, graphite, h-BN, black P, MX$_2$ (M=Mo and W, X=S, Se and Te), MX (M=Ga and In, X=S, Se and Te), Bi$_2$Te$_3$ and MnBi$_2$Te$_4$ using density functional theory. For exchange-correlation functionals with explicit vdW interaction, a single vdW layer always has the smallest surface energy, giving a surface energy reduction when compared to thicker vdW layers. However, the magnitude of this surface energy reduction quickly decreases with increasing number of atomic layers inside the single vdW layer for different vdW materials. Such atomic-layer-dependence in surface energy reduction helps explain the different effectiveness of exfoliation for different vdW materials down to a single vdW layer.

cond-mat.mtrl-sci↗

arXiv2025

Physical properties of $R$Co$_{2}$Al$_{8}$ ($R=$ La, Ce, Pr, Nd and Sm) single crystals: An emerging structure-type for anisotropic Kondo lattice studies

Systematic investigations of rare-earth ($R$) based intermetallic materials are a leading strategy to reveal the underlying mechanisms governing a range of physical phenomena, such as the formation of a Kondo lattice and competing electronic and magnetic anisotropies. In this work, the magnetic, thermal and transport properties of $R$Co$_{2}$Al$_{8}$ ($R=$ La, Ce, Pr, Nd and Sm) single crystals are presented. LaCo$_{2}$Al$_{8}$ is characterized as a Pauli paramagnet and transport measurements, with the current along and perpendicular to the orthorhombic $c$-axis ($ρ_{c}$ and $ρ_{ab}$, respectively), reveal a clear electronic anisotropy, with $ρ_{ab }\approx(4-7)ρ_{c }$ at $300$ K. We show that CeCo$_{2}$Al$_{8}$ is a Kondo-lattice for which the Kondo coherence temperature $T_{\text{K}}^{*}$, deduced from broad maximums in $ρ_{c}$ and $ρ_{ab}$ at $\approx$ 68 and 46 K, respectively, is also anisotropic. This finding is related to a possible underlying anisotropy of the Kondo coupling in CeCo$_{2}$Al$_{8}$. The Pr- and Nd-based materials present strong easy-axis anisotropy ($c$-axis) and antiferromagnetic (AFM) orders below $T=4.84$ K and $T=8.1$ K, respectively. Metamagnetic transitions from this AFM to a spin-polarized paramagnetic phase state are investigated by isothermal magnetization measurements. The Sm-based compound is also an easy-axis AFM with a transition at $T=21.6$ K.

cond-mat.str-el↗

arXiv2025

Superconducting density of states of PtPb4

PtPb$_4$ is a type II superconductor with a bulk critical temperature $T_{c}\approx 3 $K and an upper critical field of $H_{c2}=0.36 $T. PtPb$_4$ is related to non-superconducting PtSn$_4$, which presents nodal arc states at the surface. Here we measure the superconducting density of states of PtPb$_4$ using millikelvin Scanning Tunneling Microscopy (STM). We observe a fully opened superconducting gap of $Δ=0.48$\ meV similar to expectations from Bardeen Cooper and Schrieffer (BCS) theory ($Δ_0=1.76k_BT_{c}=0.49 $meV). Measurements under magnetic fields applied perpendicular to the surface show a spatially inhomogeneous gap structure, presenting superconducting signatures at fields as high as 1.5 T, significantly above $H_{c2}=0.36 $T. On some locations we find that the superconducting density of states does not vanish above $T_{c}$. We can find signatures of a superconducting gap up to 5K. We discuss possible reasons for the observation of superconducting properties above $T_{c}$ and $H_{c2}$, emphasizing the role played by structural defects.

cond-mat.supr-con↗

arXiv2025

Role of Nematic Fluctuations on Superconductivity in FeSe$_{0.47}$Te$_{0.53}$ Revealed by NMR under Pressure

The relationship between antiferromagnetic (AFM) spin fluctuations (SF), nematic fluctuations, and superconductivity (SC) has been central to understanding the pairing mechanism in iron-based superconductors (IBSCs). Iron chalcogenides, which hold the simplest crystal structure in IBSCs, provide a good platform to investigate the relationship. Here, we report $^{77}$Se and $^{125}$Te nuclear magnetic resonance studies of FeSe$_{0.47}$Te$_{0.53}$, which is located close to a nematic quantum critical point (QCP), under pressures up to 1.35 GPa. Both the superconducting critical temperature and AFMSF were found to be enhanced under pressure, which suggests a correlation between SC and AFMSF in FeSe$_{0.47}$Te$_{0.53}$. However, the contribution of AFMSF to SC in FeSe$_{0.47}$Te$_{0.53}$ was found to be much less compared to that in FeSe$_{1-x}$S$_{x}$, suggesting that nematic fluctuations play a dominant role in the SC in FeSe$_{1-x}$Te$_{x}$ around the nematic QCP.

cond-mat.supr-con↗

arXiv2025

Superconducting dome and structural changes in LaRu$_3$Si$_2$ under pressure

LaRu$_3$Si$_2$ is of current research interest as a kagome metal with a superconducting transition temperature, $T_c\sim$7 K and higher temperature charge density wave (CDW) orders. Here we report electrical transport and X-ray diffraction measurements on LaRu$_3$Si$_2$ under pressure up to 65 GPa and 35 GPa respectively. The superconducting transition temperature $T_c$ first gets slightly enhanced and reaches a maximum $\sim$8.7 K at $\sim$8.5 GPa. With further applied pressure, $T_c$ is initially gradually suppressed, then more rapidly suppressed, followed by gradual suppression, revealing a superconducting dome. Two possible pressure-induced structural phase transitions are also observed at room temperature, from original hexagonal phase to another hexagonal structure above $\sim$11.5 GPa, and further to a structure with lower symmetry above $\sim$23.5 GPa. These transition pressures roughly correlate with features found in our pressure dependent transport data.

cond-mat.supr-con↗

arXiv2025

Use of frit-disc crucible sets to make solution growth more quantitative and versatile

The recent availability of step-edge, frit-disc crucible sets (generally sold as Canfield Crucible Sets or CCS) has led to multiple innovations associated with our group's use of solution growth. Use of CCS allows for the clean separation of liquid from solid phases during the growth process. This clean separation enables the reuse of the decanted liquid, either allowing for simple, economic, savings associated with recycling expensive precursor elements or allowing for the fractionation of a growth into multiple, small steps, revealing the progression of multiple solidifications. Clean separation of liquid from solid phases also allows for the determination of the liquidus line (or surface) and the creation, or correction, of composition-temperature phase diagrams. The reuse of clean decanted liquid has also allowed us to prepare liquids ideally suited for the growth of large single crystals of specific phases by tuning the composition of the melt to the optimal composition for growth of the desired phase, often with reduced nucleation sites. Finally, we discuss how solution growth and CCS use can be harnessed to provide a plethora of composition-temperature data points defining liquidus lines or surfaces with differing degrees of precision to either test or anchor artificial intelligence and/or machine learning based attempts to augment and extend the limited experimentally determined data base.

cond-mat.mtrl-sci↗

arXiv2025

Topography of Fermi Arcs in t-PtBi$_2$ Using High Resolution Angle-resolved Photoemission Spectroscopy

We use high resolution angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) to investigate the electronic structure of trigonal phase ${\rm PtBi_2}$ (t-${\rm PtBi_2}$), a proposed Weyl semimetal that is expected to exhibit topological Fermi Arcs. Our ARPES data elucidates the topography of these objects and confirms their Fermi arc character. The arcs are formed by surface bands that have fairly flat bottom located very close to the chemical potential $\sim$ 6-8 meV, before they merge with bulk bands at higher binding energy. Comparison of the ARPES data with DFT calculations shows good agreement about their location and topography. Data acquired at low temperatures does not show any signatures of superconductivity down to 3 K in terms of expected changes in dispersion due to formation of Bogoliubov quasiparticles or superconducting gap in form of reliable shifts of peaks in energy distribution curves.

cond-mat.mes-hall↗

arXiv2025

Design and Predict Tetragonal van der Waals Layered Quantum Materials of MPd$_5$I$_2$ (M=Ga, In and 3$d$ Transition Metals)

Quantum materials with stacked van der Waals (vdW) layers hosting non-trivial band structure topology and magnetism have shown many interesting properties. Using high throughput density functional theory calculations, we design and predict tetragonal vdW-layered quantum materials in the MPd$_5$I$_2$ structure (M=Ga, In and 3d transition metals). We show that besides the known AlPd$_5$I$_2$, the -MPd$_5$- structural motif of three-atomic-layer slabs separated by two I layers can accommodate a variety of metal atoms giving arise to topologically non-trivial features and highly tunable magnetic properties in both bulk and single layer 2D structures. Among them, TiPd$_5$I$_2$ and InPd$_5$I$_2$ host a pair of Dirac points and likely an additional strong topological insulator state for the band manifolds just above and below the top valence band, respectively, with their single layers hosting or near quantum spin Hall states. CrPd$_5$I$_2$ is a ferromagnet with a large out-of-plane magneto-anisotropy energy, desirable for rare-earth-free permanent magnets.

cond-mat.mtrl-sci↗

arXiv2025

Machine learning accelerated prediction of Ce-based ternary compounds involving antagonistic pairs

The discovery of novel quantum materials within ternary phase spaces containing antagonistic pair such as Fe with Bi, Pb, In, and Ag, presents significant challenges yet holds great potential. In this work, we investigate the stabilization of these immiscible pairs through the integration of Cerium (Ce), an abundant rare-earth and cost-effective element. By employing a machine learning (ML)-guided framework, particularly crystal graph convolutional neural networks (CGCNN), combined with first-principles calculations, we efficiently explore the composition/structure space and predict 9 stable and 37 metastable Ce-Fe-X (X=Bi, Pb, In and Ag) ternary compounds. Our findings include the identification of multiple new stable and metastable phases, which are evaluated for their structural and energetic properties. These discoveries not only contribute to the advancement of quantum materials but also offer viable alternatives to critical rare earth elements, underscoring the importance of Ce-based intermetallic compounds in technological applications.

cond-mat.mtrl-sci↗

arXiv2025

Effects of Co substitution on the structural and magnetic properties of Sr(Ni$_{1-x}$Co$_x$)$_2$P$_2$

Although SrNi$_2$P$_2$ adopts the common ThCr$_2$Si$_2$ structure for $T\geq 325$ K, being in an uncollapsed tetragonal state, on cooling below 325 K it adopts a one-third collapsed orthorhombic phase where one out of every three P rows bond across the Sr layers. On the other hand, SrCo$_2$P$_2$ only exhibits the uncollapsed ThCr$_2$Si$_2$ structure from room temperature down to 1.8 K. Neither SrNi$_2$P$_2$ nor SrCo$_2$P$_2$ manifests magnetic transitions down to 50 mK and 2 K, respectively. In this work we report the effects of Co substitution in Sr(Ni$_{1-x}$Co$_x$)$_2$P$_2$, which allows for tuning the transition between the one-third collapsed and the uncollapsed structure. We find a rapid decrease of the one-third collapsed structural transition temperature with increasing Co fraction, until reaching full suppression for $x \geq 0.1$. Substitution levels in the range $0.11\leq x\leq 0.58$ show no signs of any transition down to 1.8 K in the magnetization or resistance measurements in the range $1.8\ \text{K}\leq T\leq 300\ \text{K}$. However, different magnetically ordered states emerge for $x\geq 0.65$, and disappear for $x\geq 0.99$, recovering the known paramagnetic properties of the parent compound SrCo$_2$P$_2$. These results are summarized in a phase diagram, built upon the characterization done on single crystals with different Co fraction. Both the magnetic and structural properties are compared to other systems with ThCr$_2$Si$_2$ structure that exhibit magnetic ordering and collapsed tetragonal transitions. The magnetic ordering and moment formation are well described by Takahashi's spin fluctuation theory of itinerant electron magnetism.

cond-mat.str-el↗

arXiv2025

Tuning the structure and superconductivity of SrNi$_2$P$_2$ by Rh substitution

SrNi$_2$P$_2$ is unique among the ThCr$_2$Si$_2$ class since it exhibits a temperature induced transition upon cooling from an uncollapsed tetragonal (ucT) state to a one-third-collapsed orthorhombic (tcO) state where one out of every three P-rows bond across the Sr layers. This compound is also known for exhibiting bulk superconductivity below 1.4 K at ambient pressure. In this work, we report on the effects of Rh substitution in Sr(Ni$_{1-x}$Rh$_x$)$_2$P$_2$ on the structural and superconducting properties. We studied the variation of the nearest P-P distances as a function of the Rh fraction at room temperature, as well as its temperature dependence for selected compositions. We find that increasing the Rh fraction leads to a decrease in the transition temperature between the ucT and tcO states, until a full suppression of the tcO state for $x\geq 0.166$. The superconducting transition first remains nearly insensitive to the Rh fraction, and then it increases to 2.3 K after the tcO state is fully suppressed. These results are summarized in a phase diagram, built upon the characterization by energy dispersive x-ray spectroscopy, x-ray diffraction, resistance, magnetization and specific heat measurements done on crystalline samples with varying Rh content. The relationship between band structure, crystal structure and superconductivity is discussed based on previously reported band structure calculations on SrRh$_2$P$_2$. Moreover, the effect of Rh fraction on the stress-induced structural transitions is also addressed by means of strain-stress studies done by uniaxial compression of single-crystalline micropillars of Sr(Ni$_{1-x}$Rh$_x$)$_2$P$_2$.

cond-mat.supr-con↗