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Kagome metals with van Hove singularities (VHSs) near the Fermi level can host intriguing quantum phenomena, including chiral loop currents, electronic nematicity, and unconventional superconductivity. However, unconventional magnetic states driven by VHSs, such as spin-density waves (SDWs), have yet to be observed experimentally in kagome metals. Here, we present a comprehensive investigation of the magnetic and electronic structure of the layered kagome metal CeTi3Bi4, where the Ti kagome electronic structure interacts with a magnetic sublattice of Ce3+ Jeff = 1/2 moments. Our neutron diffraction measurements reveal an incommensurate SDW ground state of the Ce3+ Jeff = 1/2 moments, which notably coexists with commensurate antiferromagnetic order across most of the temperature-field phase diagram. The commensurate component is preferentially suppressed by both thermal fluctuations and external magnetic fields, resulting in a rich phase diagram that includes an intermediate single-Q SDW phase. First-principles calculations and angle-resolved photoemission spectroscopy (ARPES) measurements identify VHSs near the Fermi level, with the observed magnetic propagation vectors connecting their high density of states, strongly suggesting a VHS-assisted SDW in CeTi3Bi4. These findings establish the rare-earth Kagome metals LnTi3Bi4 as a model platform where characteristic electronic structure of the kagome lattice plays a pivotal role in magnetic order., Comment: 20 pages, 4 figures, SI not included more...

The kagome motif is a versatile platform for condensed matter physics, hosting rich interactions between magnetic, electronic, and structural degrees of freedom. In recent years, the discovery of a charge density wave (CDW) in the AV$_3$Sb$_5$ superconductors and structurally-derived bond density waves in FeGe and ScV$_6$Sn$_6$ have stoked the search for new kagome platforms broadly exhibiting density wave (DW) transitions. In this work, we evaluate the known AM$_6$X$_6$ chemistries and construct a stability diagram that summarizes the structural relationships between the $\approx$125 member family. Subsequently we introduce our discovery of the broader LnNb$_6$Sn$_6$ (Ln:Ce-Nd,Sm,Gd-Tm,Lu,Y) family of kagome metals and an analogous DW transition in LuNb$_6$Sn$_6$. Our X-ray scattering measurements clearly indicate a (1/3, 1/3, 1/3) ordering wave vector ($\sqrt{3}\times\sqrt{3}\times3$ superlattice) and diffuse scattering on half-integer $L$-planes. Our analysis of the structural data supports the ``rattling mode'' DW model proposed for ScV$_6$Sn$_6$ and paints a detailed picture of the steric interactions between the rare-earth filler element and the host Nb-Sn kagome scaffolding. We also provide a broad survey of the magnetic properties within the HfFe$_6$Ge$_6$-type LnNb$_6$Sn$_6$ members, revealing a number of complex antiferromagnetic and metamagnetic transitions throughout the family. This work integrates our new LnNb$_6$Sn$_6$ series of compounds into the broader AM$_6$X$_6$ family, providing new material platforms and forging a new route forward at the frontier of kagome metal research. more...

In this work, we investigate the electrical conductivity of carbon nanotubes (CNTs), with a particular focus on the effects of doping. Using a first-principles approach, we study the electronic structure, phonon dispersion, and electron-phonon scattering to understand the finite-temperature electrical transport properties in CNTs. Our study covers both prototypical metallic and semiconducting CNTs, with special emphasis on the influence of typical defects such as vacancies and the incorporation of copper or nitrogen, such as pyridinic N, pyrrolic N, graphitic N, and oxidized N. Our theoretical study shows significant improvements in the electrical conduction properties of copper-CNT composites, especially when semiconducting CNTs are functionalized with nitrogen. Doping is found to cause significant changes in the electronic density of states near the Fermi level, which affects the electrical conductivity. Calculations show that certain types of functional groups, such as N-pyrrolic, result in a ~30-fold increase in the conductivity of semiconducting CNTs compared to Cu-incorporated CNTs alone. For metallic CNTs, the conductivity is in agreement with existing experimental data, and our prediction of significant increases in conductivity with N-pyrrolic functional group is consistent with recent experimental results, demonstrating the effectiveness of doping in modifying conductivity. Our study provides valuable insight into the electronic properties of doped CNTs and contributes to the development of ultra-high conductivity CNT composites., Comment: 16 pages, 4 figures, 39 references more...

Here we present the discovery and characterization of the kagome metal TbTi$_3$Bi$_4$ in tandem with a new series of compounds, the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ (Ln: Tb-Lu) shurikagome metals. We previously reported on the growth of the LnTi$_3$Bi$_4$ (Ln: La-Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$) family, a chemically diverse and exfoliable series of kagome metals with complex and highly anisotropic magnetism. However, unlike the La-Gd analogs, TbTi$_3$Bi$_4$ cannot be synthesized by our previous methodology due to phase competition with Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ (x$\sim$1.7-1.2). Here we discuss the phase competition between the LnTi$_3$Bi$_4$ and Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ families, helping to frame the difficulty in synthesizing LnTi$_3$Bi$_4$ compounds with small Ln species and providing a strategy to circumvent formation of Ln$_{2-x}$Ti$_{6+x}$Bi$_9$. Detailed characterization of the magnetic and electronic transport properties on single crystals of TbTi$_3$Bi$_4$ reveals a highly complex landscape of magnetic phases arising from an antiferromagnetic ground state. A series of metamagnetic transitions creates at least 5 unique magnetic phase pockets, including a 1/3 and 2/3 magnetization plateau. Further, the system exhibits an intimate connection between the magnetism and magnetotransport, exhibiting sharp switching from positive (+40%) to negative magnetoresistance (-50%). Like the LnTi$_3$Bi$_4$ kagome metals, the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ family exhibits quasi-2D networks of titanium and chains of rare-earth. We present the structures and some basic magnetic properties of the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ family alongside our characterization of the newly discovered TbTi$_3$Bi$_4$. more...

Here we present the family of titanium-based kagome metals of the form LnTi$_3$Bi$_4$ (Ln: La...Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$). Single crystal growth methods are presented alongside detailed magnetic and thermodynamic measurements. The orthorhombic (Fmmm) LnTi$_3$Bi$_4$ family of compounds exhibit slightly distorted titanium-based kagome nets interwoven with zig-zag lanthanide-based (Ln) chains. Crystals are easily exfoliated parallel to the kagome sheets and angular resolved photoemission (ARPES) measurements highlight the intricacy of the electronic structure in these compounds, with Dirac points existing at the Fermi level. The magnetic properties and the associated anisotropy emerge from the quasi-1D zig-zag chains of Ln, and impart a wide array of magnetic ground states ranging from anisotropic ferromagnetism to complex antiferromagnetism with a cascade of metamagnetic transitions. Kagome metals continue to provide a rich direction for the exploration of magnetic, topologic, and highly correlated behavior. Our work here introduces the LnTi$_3$Bi$_4$ compounds to augment the continuously expanding suite of complex and interesting kagome materials. more...

Machine learning force fields (MLFFs) are an increasingly popular choice for atomistic simulations due to their high fidelity and improvable nature. Here, we propose a hybrid small-cell approach that combines attributes of both offline and active learning to systematically expand a quantum mechanical (QM) database while constructing MLFFs with increasing model complexity. Our MLFFs employ the moment tensor potential formalism. During this process, we quantitatively assessed structural properties, elastic properties, dimer potential energies, melting temperatures, phase stability, point defect formation energies, point defect migration energies, free surface energies, and generalized stacking fault (GSF) energies of Zr as predicted by our MLFFs. Unsurprisingly, model complexity has a positive correlation with prediction accuracy. We also find that the MLFFs wee able to predict the properties of out-of-sample configurations without directly including these specific configurations in the training dataset. Additionally, we generated 100 MLFFs of high complexity (1513 parameters each) that reached different local optima during training. Their predictions cluster around the benchmark DFT values, but subtle physical features such as the location of local minima on the GSFE surface are washed out by statistical noise. more...

The kagome lattice is a fertile platform to explore topological excitations with both Fermi-Dirac and Bose-Einstein statistics. While relativistic Dirac Fermions and flat-bands have been discovered in the electronic structure of kagome metals, the spin excitations have received less attention. Here we report inelastic neutron scattering studies of the prototypical kagome magnetic metal FeSn. The spectra display well-defined spin waves extending up to 120 meV. Above this energy, the spin waves become progressively broadened, reflecting interactions with the Stoner continuum. Using linear spin wave theory, we determine an effective spin Hamiltonian that reproduces the measured dispersion. This analysis indicates that the Dirac magnon at the K-point remarkably occurs on the brink of a region where well-defined spin waves become unobservable. Our results emphasize the influential role of itinerant carriers on the topological spin excitations of metallic kagome magnets., Comment: 6 pages, 4 figures more...

Understanding the magnetism and its possible correlations to the topological properties has emerged as a forefront and difficult topic in studying magnetic Weyl semimetals. Co$_{3}$Sn$_{2}$S$_{2}$ is a newly discovered magnetic Weyl semimetal with a kagome lattice of cobalt ions and has triggered intense interest for rich fantastic phenomena. Here, we report the magnetic exchange couplings of Co$_{3}$Sn$_{2}$S$_{2}$ using inelastic neutron scattering and two density functional theory (DFT) based methods: constrained magnetism and multiple-scattering Green's function methods. Co$_{3}$Sn$_{2}$S$_{2}$ exhibits highly anisotropic magnon dispersions and linewidths below $T_{C}$, and paramagnetic excitations above $T_{C}$. The spin-wave spectra in the ferromagnetic ground state is well described by the dominant third-neighbor "across-hexagon" $J_{d}$ model. Our density functional theory calculations reveal that both the symmetry-allowed 120$^\circ$ antiferromagnetic orders support Weyl points in the intermediate temperature region, with distinct numbers and the locations of Weyl points. Our study highlights the important role Co$_{3}$Sn$_{2}$S$_{2}$ can play in advancing our understanding of kagome physics and exploring the interplay between magnetism and band topology., Comment: 5 pages, 4 figures, plus one supplementary material more...

Charge density waves (CDW) are modulations of the electron density and the atomic lattice that develop in some crystalline materials at low temperature. We report an unusual example of a CDW in BaFe$_2$Al$_9$ below 100 K. In contrast to the canonical CDW phase transition, temperature dependent physical properties of single crystals reveal a first-order phase transition. This is accompanied by a discontinuous change in the size of the crystal lattice. In fact, this large strain has catastrophic consequences for the crystals causing them to physically shatter. Single crystal x-ray diffraction reveals super-lattice peaks in the low-temperature phase signaling the development of a CDW lattice modulation. No similar low-temperature transitions are observed in BaCo$_2$Al$_9$. Electronic structure calculations provide one hint to the different behavior of these two compounds; the d-orbital states in the Fe compound are not completely filled. Iron compounds are renowned for their magnetism and partly filled d-states play a key role. It is therefore surprising that BaFe$_2$Al$_9$ develops a structural modulation instead at low temperature instead of magnetic order., Comment: 34 pages, 8 figures Edits to text as well as figures 2 and 5. Added neutron diffraction (Fig. 6) more...

Quantum interference on the kagome lattice generates electronic bands with narrow bandwidth, called flat bands. Crystal structures incorporating this lattice can host strong electron correlations with non-standard ingredients, but only if these bands lie at the Fermi level. In the six compounds with the CoSn structure type (FeGe, FeSn, CoSn, NiIn, RhPb, and PtTl) the transition metals form a kagome lattice. The two iron variants are robust antiferromagnets so we focus on the latter four and investigate their thermodynamic and transport properties. We consider these results and calculated band structures to locate and characterize the flat bands in these materials. We propose that CoSn and RhPb deserve the community's attention for exploring flat band physics., Comment: 12pg 11fig more...

We show that the Fermi surface can survive the presence of extreme compositional disorder in the equiatomic alloy Ni$_{0.25}$Fe$_{0.25}$Co$_{0.25}$Cr$_{0.25}$. Our high-resolution Compton scattering experiments reveal a Fermi surface which is smeared across a significant fraction of the Brillouin zone (up to 40\% of $\frac{2\pi}{a}$). The extent of this smearing and its variation on and between different sheets of the Fermi surface has been determined, and estimates of the electron mean-free-path and residual resistivity have been made by connecting this smearing with the coherence length of the quasiparticle states. more...

Quantum critical behavior has been associated with some of the most exotic emergent states of matter including high-temperature superconductivity. Much of the research into quantum critical point (QCP) physics has been hampered by the lack of model systems simple enough to be analyzed by theory. Here, we show that the concentrated solid solution fcc alloys, including the so-called high-entropy alloys, are ideal model systems to study the effects of chemical disorder on emergent properties near a quantum critical region. The face centered cubic (fcc) alloy NiCoCrx with x near 1 is found to be close to the Cr concentration where the ferromagnetic transition temperature, Tc, goes to 0. Near this composition these alloys exhibit a resistivity linear in temperature to 2 K, a linear magnetoresistance, an excess -TlnT contribution to the low temperature heat capacity and excess low temperature entropy. All of the low temperature electrical, magnetic and thermodynamic properties of the alloys with compositions near x near 1 are not typical of a Fermi liquid and suggest strong magnetic fluctuations associated with a quantum critical region. The limit of extreme chemical disorder in these simple fcc materials thus provides a novel and unique platform to study quantum critical behavior in a highly tunable system. more...

The magnetic phase diagrams of models for quasi one-dimensional compounds belonging to the iron-based superconductors family are presented. The five-orbital Hubbard model and the real-space Hartree-Fock approximation are employed, supplemented by density functional theory to obtain the hopping amplitudes. Phase diagrams are constructed varying the Hubbard $U$ and Hund $J$ couplings and at zero temperature. The study is carried out at electronic density (electrons per iron) $n = 5.0$, which is of relevance for the already known material TlFeSe$_2$, and also at $n = 6.0$, where representative compounds still need to be synthesized. At $n = 5.0$ there is a clear dominance of staggered spin order along the chain direction. At $n = 6.0$ and the realistic Hund coupling $J/U = 0.25$, the phase diagram is far richer including a variety of ``block'' states involving ferromagnetic clusters that are antiferromagnetically coupled, in qualitative agreement with recent Density Matrix Renormalization Group calculations for the three-orbital Hubbard model in a different context. These block states arise from the competition between ferromagnetic order (induced by double exchange, and prevailing at large $J/U$) and antiferromagnetic order (dominating at small $J/U$). The density of states and orbital compositions of the many phases are also provided., Comment: 12 pages, 11 figures more...

Recent neutron scattering experiments addressing the magnetic state of the two-leg ladder selenide compound BaFe$_2$Se$_3$ have unveiled a dominant spin arrangement involving ferromagnetically ordered 2$\times$2 iron-superblocks, that are antiferromagnetically coupled among them (the "block-AFM" state). Using the electronic five-orbital Hubbard model, first principles techniques to calculate the electronic hopping amplitudes between irons, and the real-space Hartree-Fock approximation to handle the many-body effects, here it is shown that the exotic block-AFM state is indeed stable at realistic electronic densities close to $n \sim 6.0$. Another state (the "CX" state) with parallel spins along the rungs and antiparallel along the legs of the ladders is close in energy. This state becomes stable in other portions of the phase diagrams, such as with hole doping, as also found experimentally via neutron scattering applied to KFe$_2$Se$_3$. In addition, the present study unveils other competing magnetic phases that could be experimentally stabilized varying either $n$ chemically or the electronic bandwidth by pressure. Similar results were obtained using two-orbital models, studied here via Lanczos and DMRG techniques. A comparison of the results obtained with the realistic selenides hoppings amplitudes for BaFe$_2$Se$_3$ against those found using the hopping amplitudes for pnictides reveals several qualitative similarities, particularly at intermediate and large Hubbard couplings., Comment: 10 pages, 6 figures more...

The anisotropic physical properties of single crystals of orthorhombic PtSn4 are reported for magnetic fields up to 140 kOe, applied parallel and perpendicular to the crystallographic b-axis. The magnetic susceptibility has an approximately temperature independent behavior and reveals an anisotropy between ac-plane and b-axis. Clear de Haas-van Alphen oscillations in fields as low as 5 kOe and at temperatures as high as 30 K were detected in magnetization isotherms. The thermoelectric power and resistivity of PtSn4 show the strong temperature and magnetic field dependencies. A change of the thermoelectric power at H = 140 kOe is observed as high as ~ 50 mu-V/K. Single crystals of PtSn4 exhibit very large transverse magnetoresistance of ~ 5x10^5% for the ac-plane and of ~ 1.4x10^5% for the b-axis resistivity at 1.8 K and 140 kOe, as well as pronounced Shubnikov-de Haas oscillations. The magnetoresistance of PtSn4 appears to obey Kohler's rule in the temperature and field range measured. The Hall resistivity shows a linear temperature dependence at high temperatures followed by a sign reversal around 25 K which is consistent with thermoelectric power measurements. The observed quantum oscillations and band structure calculations indicate that PtSn4 has three dimensional Fermi surfaces., Comment: accepted to PRB more...

We present detailed thermodynamic and transport measurements on single crystals of the recently discovered binary intermetallic superconductor, SrSn4. We find this material to be a slightly anisotropic three-dimensional, strongly-coupled, possibly multi-band, superconductor. Hydrostatic pressure causes a decrease in the superconducting transition temperature at the rate of -0.068 K/kbar. Band structure calculations are consistent with experimental data on Sommerfeld coefficient and upper superconducting critical field anisotropy and suggest complex, multi-sheet Fermi surface formed by four bands., Comment: Figure 11 corrected more...

We determine the anisotropy of the spin fluctuation induced pairing gap on the Fermi surface of the FeAs based superconductors as function of the exchange and Hund's coupling $J_{H}$. We find that for sufficiently large $J_{H}$, nearly commensurate magnetic fluctuations yield a fully gapped $s^{\pm}$-pairing state with small anisotropy of the gap amplitude on each Fermi surface sheet, but significant variations of the gap amplitude for different sheets of the Fermi surface. In particular, we obtain the large variation of the gap amplitude on different Fermi surface sheets, as seen in ARPES experiments. For smaller values of Hund's coupling incommensurate magnetic fluctuations yield an $s^{\pm}$-pairing state with line nodes. Such a state is also possible once the anisotropy of the material is reduced and three dimensional effects come into play., Comment: Revised and substantially extended version, accepted for publication in Phys. Rev. B; 9 pages, 6 figures more...

Shubnikov - de Haas oscillations were measured in single crystals of highly metallic antiferromagnetic SmAgSb$_{2}$ and ferromagnetic CeAgSb$_{2}$ using a tunnel diode resonator. Resistivity oscillations as a function of applied magnetic field were observed via measurements of skin depth variation. The effective resolution of $\Delta\rho\simeq20$ p$\Omega$ allows a detailed study of the SdH spectra as a function of temperature. The effects of the Sm long - range magnetic ordering as well as its electronic structure ($4f$-electrons) on the Fermi surface topology is discussed. more...

Density-functional studies of the electronic structures and exchange interaction parameters have been performed for a series of ferromagnetic full Heusler alloys of general formula Co$_2$MnZ (Z = Ga, Si, Ge, Sn), Rh$_2$MnZ (Z = Ge, Sn, Pb), Ni$_2$MnSn, Cu$_2$MnSn and Pd$_2$MnSn, and the connection between the electronic spectra and the magnetic interactions have been studied. Different mechanisms contributing to the exchange coupling are revealed. The band dependence of the exchange parameters, their dependence on volume and valence electron concentration have been thoroughly analyzed within the Green function technique., Comment: 9 figures, 6 tables more...