Heavy-fermion superconductors are mostly associated with f-electron materials with Kondo lattices, while known d-electron heavy-fermion-like systems are often linked to orbital-selective local moments, Hund-metal physics, or a charge-density-wave mechanism. Here we report Mo4PtGa17, a noncentrosymmetric itinerant d-electron superconductor with a geometrically frustrated breathing-pyrochlore Mo lattice. Thermodynamic, transport and NMR measurements reveal heavy-fermion-like behavior superconductivity and dominant ferromagnetic spin fluctuations near a ferromagnetic instability. Theoretical calculations identify nearly flat bands, van Hove singularities and Kramers nodal lines near the Fermi energy, derived intrinsically from Mo-4d states and are robust against on-site electronic correlations. These results suggest that the geometrically frustrated lattice in Mo4PtGa17 generates an intriguing electronic structure that enhances the density of states, spin susceptibility and quasiparticle mass. Mo4PtGa17 therefore identifies a unique route to heavy-fermion-like superconductivity in d-electron materials through geometrical frustration, different from the previously reported systems.
Static and dynamical magnetic and electronic properties of the kagome metal Sc3Mn3Al7Si5 have been investigated by 27Al nuclear magnetic resonance (NMR) measurements. Two distinct 27Al-NMR signals with two different values of quadrupolar frequencies of vQ = 1.55(2) and 1.07(2) MHz are observed, which are assigned to Al(1) and Al(2), respectively. From the detailed NMR spectrum measurements under three different magnetic field directions and the density functional theory calculations, the principal axes of the electric field gradient for each Al site have been determined. The temperature dependence of Knight shift (K) shows a similar temperature dependence of the DC magnetic susceptibility chi except for the low-temperature region below '50 K where K is almost constant while chi keeps increasing, which suggests that the increase in chi at low temperatures is not intrinsic. 27Al spin-lattice relaxation rate divided by temperature (1/T1T ) is found to be constant, confirming the metallic state of Sc3Mn3Al7Si5 from a microscopic point of view. Based on a Korringa ratio analysis using the T1 and K data, ferromagnetic fluctuations are found to dominate in Sc3Mn3Al7Si5. These fluctuations are suggested to be very slow with frequencies on the order of kilohertz or lower.
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.
Static and dynamical magnetic and electronic properties of the kagome metal Sc$_3$Mn$_3$Al$_7$Si$_5$ have been investigated by $^{27}$Al nuclear magnetic resonance (NMR) measurements. The temperature dependence of Knight shift ($K$) shows a similar temperature dependence of the DC magnetic susceptibility $\chi$ except for the low-temperature region below $\sim$ 50 K where $K$ is almost constant while $\chi$ keeps increasing, which suggests that the increase in $\chi$ at low temperatures is not intrinsic. $^{27}$Al spin-lattice relaxation rate divided by temperature ($1/T_1T$) is found to be constant, confirming the metallic state of Sc$_3$Mn$_3$Al$_7$Si$_5$ from a microscopic point of view. Based on a Korringa ratio analysis using the $T_1$ and $K$ data, ferromagnetic spin fluctuations are found to dominate in Sc$_3$Mn$_3$Al$_7$Si$_5$. These fluctuations are suggested to be very slow with frequencies on the order of kilohertz or lower.
Ferrimagnets that can be driven to magnetic compensation show promise for use in spintronics as they exhibit a finite anomalous Hall effect at zero magnetic field without having a substantial magnetic moment. Compensated ferrimagnet spintronic devices with both a large anomalous Hall effect and a high coercivity would be simultaneously easy to read and difficult to erase. The kagome ferrimagnet TbMn6Sn6 has been reported to host a large intrinsic anomalous Hall effect. Here, we demonstrate that doping the Mn sites with Cr drives the system toward magnetic compensation. For nearly compensated compositions at low temperatures, giant coercive fields exceeding 14 T are observed. Additionally, Cr doping markedly enhances the intrinsic anomalous Hall effect, which can be attributed to a shift in the Fermi level. Our results extend the range of unique magnetic states observed in kagome materials, demonstrating that chemical doping is an effective strategy to tune and realize these states.
The interplay between magnetism and flat-band (FB) instability is a central theme in quantum materials research. A striking example is the emergence of magnetic order in a nominally nonmagnetic compound when a flat band is tuned near the Fermi energy ([Formula: see text]). In this study, we investigate this phenomenon in the Pauli paramagnet [Formula: see text], where an FB associated with Co [Formula: see text] orbitals lies close to [Formula: see text]. Remarkably, a minute substitution of the nonmagnetic element Pd onto the Co site ([Formula: see text]2%) induces antiferromagnetic order with a transition temperature as high as [Formula: see text] K. Temperature- and magnetic-field-dependent magnetic and transport measurements, complemented by zero-field neutron diffraction, reveal a helical magnetic order for [Formula: see text] in Sr(Co1-xPdx)2As2, transitioning to a complex ferromagnetic state at higher Pd concentrations. Spectroscopic evidence and theoretical band structure calculations demonstrate that electron doping shifts the flat band closer to [Formula: see text], significantly enhancing the Stoner parameter. This enhancement drives a strong ferromagnetic instability, leading to helical magnetic ordering dominated by in-plane ferromagnetic interactions. The emergence of robust magnetic ordering through substitution with nonmagnetic elements is a unique phenomenon that underscores the pivotal role of flat-band instability in tuning magnetism in itinerant systems.
The discovery of novel quantum materials within ternary phase spaces containing antagonistic pairs 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.
The interplay between magnetism and flat-band (FB) instability is a central theme in quantum materials research. A striking example is the emergence of magnetic order in a nominally nonmagnetic compound when a flat band is tuned near the Fermi energy ( E F ). In this study, we investigate this phenomenon in the Pauli paramagnet SrCo 2 As 2 , where an FB associated with Co e g orbitals lies close to E F . Remarkably, a minute substitution of the nonmagnetic element Pd onto the Co site ( ∼ 2%) induces antiferromagnetic order with a transition temperature as high as T N = 25 K. Temperature- and magnetic-field-dependent magnetic and transport measurements, complemented by zero-field neutron diffraction, reveal a helical magnetic order for x ≤ 0.10 in Sr(Co 1− x Pd x ) 2 As 2 , transitioning to a complex ferromagnetic state at higher Pd concentrations. Spectroscopic evidence and theoretical band structure calculations demonstrate that electron doping shifts the flat band closer to E F , significantly enhancing the Stoner parameter. This enhancement drives a strong ferromagnetic instability, leading to helical magnetic ordering dominated by in-plane ferromagnetic interactions. The emergence of robust magnetic ordering through substitution with nonmagnetic elements is a unique phenomenon that underscores the pivotal role of flat-band instability in tuning magnetism in itinerant systems.
Magnetic anisotropy is a crucial characteristic for enhancing the spintronic device performance. The synthesis of SmCrGe3 single crystals through a high-temperature solution method has led to the determination of uniaxial magnetocrystalline anisotropy. Phase verification was achieved by using scanning transmission electron microscopy (STEM), powder, and single-crystal X-ray diffraction techniques. Electrical transport and specific heat measurements indicate a Curie temperature (T C) of approximately 160 K, while magnetization measurements were utilized to determine the anisotropy fields and constants. Curie-Weiss fitting applied to magnetization data suggests the contribution of both Sm and Cr in the paramagnetic phase. Additionally, density functional theory (DFT) calculations explored the electronic structures and magnetic properties of SmCrGe3, revealing a significant easy-axis single-ion Sm magnetocrystalline anisotropy of 16 meV/fu. Based on the magnetization measurements, easy-axis magnetocrystalline anisotropy at 20 K is 13 meV/fu.
Kagome metals with the Fermi energy tuned near the van Hove singularities (vHss) have shown to host exotic phases including unconventional superconductivity and a chiral flux phase arising from a charge density wave. However, most quantum oscillations studies of the electronic structure of kagome metals focus on compounds which electronically or magnetically order, obscuring the unperturbed vHs. Here we present quantum oscillation measurements of YV$_6$Sn$_6$ which contains a pristine kagome lattice free from long range order. We discovered quantum oscillations corresponding to a large orbit ($\approx$70% of the Brillouin Zone area) with the heaviest mass ever observed in vanadium based kagome metals ($\approx3.3 m_e$), consistent with a Fermi pocket whose Fermi level is near the vHs. Comparing with first principles calculations suggests that the effective mass of this pocket is highly sensitive to the position of Fermi level. Our study establishes the enhanced density of states associated with a vHs in a kagome metal, allowing further insight into a potential driving mechanism for the unconventional electronic orderings in this class of materials.
The addition of magnetic impurities in topological insulators can drive ferromagnetic order that leads to novel quantum anomalous Hall transport well below the Curie temperature. The fragility of the quantized regime has been ascribed to the random nature of the magnetic moment distribution. Here, we refine this hypothesis by using inelastic neutron scattering and density-functional theory calculations to show that two antagonistic components define the magnetism in Mn-substituted SnTe, thereby limiting the effectiveness of dilute magnetic TIs. One component is strongly bound antiferromagnetic dimers that compete with ferromagnetic order. The other component consists of undimerized moments where ferromagnetic order develops via long-range interactions.
Charge density waves (CDWs) in kagome metals have been tied to many exotic phenomena. Here, using spectroscopic-imaging scanning tunneling microscopy and angle-resolved photoemission spectroscopy, we study the charge order in kagome metal ScV 6 Sn 6 . The similarity of electronic band structures of ScV 6 Sn 6 and TbV 6 Sn 6 (where charge ordering is absent) suggests that charge ordering in ScV 6 Sn 6 is unlikely to be primarily driven by Fermi surface nesting of the Van Hove singularities. In contrast to the CDW state of cousin kagome metals, we find no evidence supporting rotation symmetry breaking. Differential conductance d I /d V spectra show a partial gap Δ 1 CO ≈ 20 meV at the Fermi level. Interestingly, d I /d V maps reveal that charge modulations exhibit an abrupt phase shift as a function of energy at energy much higher than Δ 1 CO , which we attribute to another spectral gap. Our experiments reveal a distinctive nature of the charge order in ScV 6 Sn 6 with fundamental differences compared to other kagome metals.
The interaction between strong correlation and Berry curvature is an open territory of in the field of quantum materials. Here we report large anomalous Hall conductivity in a Kondo lattice ferromagnet USbTe which is dominated by intrinsic Berry curvature at low temperatures. However, the Berry curvature induced anomalous Hall effect does not follow the scaling relation derived from Fermi liquid theory. The onset of the Berry curvature contribution coincides with the Kondo coherent temperature. Combined with ARPES measurement and DMFT calculations, this strongly indicates that Berry curvature is hosted by the flat bands induced by Kondo hybridization at the Fermi level. Our results demonstrate that the Kondo coherence of the flat bands has a dramatic influence on the low temperature physical properties associated with the Berry curvature, calling for new theories of scaling relations of anomalous Hall effect to account for the interaction between strong correlation and Berry curvature.
[Fe(en)(tren)][FeSe2](2) (en = ethylenediamine, C2H8N2, tren = tris(2-aminoethyl)amine, C6H18N4) has been synthesized by a mixed-ligand solvothermal method. Its crystal structure contains heteroleptic [Fe(en)(tren)](2+) complexes with distorted octahedral coordination, incorporated between 1D-FeSe2 chains composed of edge-sharing FeSe4 tetrahedra. The twisted octahedral coordination environment of the Fe-amine complex leads to partial dimerization of Fe-Fe distances in the FeSe2 chains so that the FeSe4 polyhedra deviate strongly from the regular tetrahedral geometry. Fe-57 M & ouml;ssbauer spectroscopy reveals oxidation states of +3 for the Fe-chain atoms and +2 for the Fe-complex atoms. The close proximity of Fe atoms in the chains promotes ferromagnetic nearest neighbor interactions, as indicated by a positive Weiss constant, theta = +53.8(6) K, derived from the Curie-Weiss fitting. Magnetometry and heat capacity reveal two consecutive magnetic transitions below 10 K. DFT calculations suggest that the ordering observed at 4 K is due to antiferromagnetic intrachain interactions in the 1D-FeSe2 chains. The combination of two different ligands creates an asymmetric coordination environment that induces changes in the structure of the Fe-Se fragments. This synthetic strategy opens new ways to explore the effects of ligand field strength on the structure of both Fe-amine complexes and surrounding Fe-Se chains.
The intricate nature of magnetism in uranium-based Kondo lattices is a consequence of correlations between U-5f and conduction electrons. Previously, the source of magnetism has been ascribed to either Mott physics or Ruderman-Kittel-Kasuya-Yosida interaction, both of which are not fully applicable to uranium-based Kondo lattices. Using linearized quasiparticle self-consistent GW plus dynamical mean-field theory, we demonstrate a crossover from incoherent to coherent f-d Kondo cloud in the paramagnetic phase of UTe2, USbTe and USbSe. As the transition occurs, we observe an augmented f-d coherence and Pauli-like magnetic susceptibility, with a substantial frozen magnetic moment of U-5f persisting. We show that momentum dependent f-d hybridization is responsible for the magnetic moments arising from the renormalized f electrons’ van Hove singularity. Our findings provide a perspective to explain the dual nature of magnetism and the long-range magnetic ordering induced by pressure in UTe2.
Kagome metals with the Fermi energy tuned near the van Hove singularities (vHss) have shown to host exotic phases including unconventional superconductivity and a chiral flux phase arising from a charge density wave. However, most quantum oscillations studies of the electronic structure of kagome metals focus on compounds which electronically or magnetically order, obscuring the unperturbed vHs. Here we present quantum oscillation measurements of YV6Sn6 which contains a pristine kagome lattice free from long-range order. We discovered quantum oscillations corresponding to a large orbit (approximate to 70% of the Brillouin Zone area) with the heaviest mass ever observed in vanadium-based kagome metals (approximate to 3.3me), consistent with a Fermi pocket whose Fermi level is near the vHs. Comparing with first-principle calculations suggests that the effective mass of this pocket is highly sensitive to the position of Fermi level. Our study establishes the enhanced density of states associated with a vHs in a kagome metal, allowing further insight into a potential driving mechanism for the unconventional electronic orderings in this class of materials.
Magnetic defects play an important, but poorly understood, role in magnetic topological insulators (TIs). For example, topological surface transport and bulk magnetic properties are controlled by magnetic defects in Bi_2Se_3-based dilute ferromagnetic (FM) TIs and MnBi_2Te_4 (MBT)-based antiferromagnetic (AFM) TIs. Despite its nascent ferromagnetism, our inelastic neutron scattering data show that a fraction of the Mn defects in Sb_2Te_3 form strong AFM dimer singlets within a quintuple block. The AFM superexchange coupling occurs via Mn-Te-Mn linear bonds and is identical to the AFM coupling between antisite defects and the FM Mn layer in MBT, establishing common interactions in the two materials classes. We also find that the FM correlations in (Sb_1-xMn_x)_2Te_3 are likely driven by magnetic defects in adjacent quintuple blocks across the van der Waals gap. In addition to providing answers to long-standing questions about the evolution of FM order in dilute TI, these results also show that the evolution of global magnetic order from AFM to FM in Sb-substituted MBT is controlled by defect engineering of the intrablock and interblock coupling.
Intricate nature of magnetism in uranium-based Kondo lattices is a consequence of correlations between U-5$f$ and conduction electrons. Using linearized quasiparticle self-consistent GW plus dynamical mean-field theory, we demonstrate a crossover from incoherent to coherent $f$-$d$ Kondo cloud in the paramagnetic phase of UTe$_2$ with reduced volumes, USbTe and USbSe. As the transition occurs, we observe an augmented $f$-$d$ coherence and Pauli-like magnetic susceptibility, with a substantial frozen magnetic moment of U-5$f$ persisting. We show that momentum dependent $f$-$d$ hybridization is responsible for the magnetic moments arising from the renormalized $f$ electrons' van Hove singularity. Our findings provide a unique perspective to explain the dual nature of magnetism and the long-range magnetic ordering induced by pressure in UTe$_2$.
139La nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements have been performed to investigate the magnetic properties of the itinerant magnet La2Ni7 which shows a series of antiferromagnetic (AFM) phase transitions at $T_{N1}$=61 K, $T_{N2}$=56 K, and $T_{N3}$=42 K under zero magnetic field. Two distinct La NMR signals were observed due to the two crystallographically inequivalent La sites in La2Ni7 (La1 and La2 in the La2Ni4 and the LaNi5 sub-units of the La2Ni7 unit cell, respectively). From the 139La NQR spectrum in the AFM state below $T_{N3}$, the AFM state was revealed to be a commensurate state where Ni ordered moments align along the crystalline c axis. Owing to the two different La sites, we were able to estimate the average values of the Ni ordered moments ($\sim$0.09-0.10 $\mu_{B}$/Ni and $\sim$0.17$\mu_{B}$/Ni around La1 and La2, respectively) from 139La NMR spectrum measurements in the AFM state below $T_{N3}$, suggesting a non-uniform distribution of the Ni-ordered moments in the AFM state. In contrast, a more uniform distribution of the Ni-ordered moments in the saturated paramagnetic state induced by the application of high magnetic fields is observed. The temperature dependence of the sublattice magnetization measured by the internal field at the La2 site in the AFM state was reproduced by a local moment model better than the self-consistent renormalization (SCR) theory for weak itinerant antiferromagnets. Given the small Ni-ordered moments in the magnetically ordered state, our results suggest that La2Ni7 has characteristics of both itinerant and localized natures in its magnetism. With this in mind, it is noteworthy that the temperature dependence of nuclear spin-relaxation rates in the paramagnetic state above $T_{N1}$ measured at zero magnetic field can be explained qualitatively by both the SCR theory and the local-moment model.
Abstract Over the last few years, significant attention has been devoted to studying the kagome materials A V3Sb5 (A = K, Rb, Cs) due to their unconventional superconductivity and charge density wave (CDW) ordering. Recently $${{{{\rm{ScV}}}}}_{6}{{{{\rm{Sn}}}}}_{6}$$ ScV 6 Sn 6 was found to host a CDW below ≈ 90 K, and, like A V3Sb5, it contains a kagome lattice comprised only of V ions. Here we present a comprehensive magnetotransport study on $${{{{\rm{ScV}}}}}_{6}{{{{\rm{Sn}}}}}_{6}$$ ScV 6 Sn 6 . We discovered several anomalous transport phenomena above the CDW ordering temperature, including insulating behavior in interlayer resistivity, a strongly temperature-dependent Hall coefficient, and a violation of Kohler’s rule. All these anomalies can be consistently explained by a progressive decrease in carrier densities with decreasing temperature, suggesting the formation of a pseudogap. Our findings suggest that high-temperature CDW fluctuations play a significant role in determining the normal state electronic properties of $${{{{\rm{ScV}}}}}_{6}{{{{\rm{Sn}}}}}_{6}$$ ScV 6 Sn 6 .