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Kagome lattice $A$V$_3$Sb$_5$ ($A$ = K, Rb, and Cs) superconductors without magnetism from vanadium $d$-electrons are intriguing because they have a novel charge density wave (CDW) order around 90 K and display superconductivity at $\sim$3 K that competes with the CDW order. Recently, CsCr$_3$Sb$_5$, isostructural to $A$V$_3$Sb$_5$, was found to have concurrent structural and magnetic phase transition at $T^{\ast}\approx$ 55 K that can be suppressed by pressure to induce superconductivity [Liu \textit{et al.}, \href{https://doi.org/10.1038/s41586-024-07761-x}{Nature \textbf{632}, 1032 (2024)}]. Here, we use elastic and inelastic X-ray scattering to study the microscopic origin of the structural transition in CsCr$_3$Sb$_5$. Although our elastic measurements confirm the 4$\times$1$\times$1 superlattice order below $T^{\ast}$, its underlying correlation is rather short-ranged. Moreover, our inelastic measurements at the superlattice wavevectors around (3, 0, 0) find no evidence of a significant acoustic phonon anomaly below $T^{\ast}$, similar to the case of $A$V$_3$Sb$_5$. The absence of acoustic phonon anomaly indicates a weak electron-phonon coupling in CsCr$_3$Sb$_5$, suggesting that the structural transition is likely associated with an unconventional CDW order., Comment: Six pages, four figures

Two-dimensional (2D) kagome lattice metals are interesting because they display flat electronic bands, Dirac points, Van Hove singularities, and can have interplay between charge density wave (CDW), magnetic order, and superconductivity. In kagome lattice antiferromagnet FeGe, a short-range CDW order was found deep within an antiferromagnetically ordered state, interacting with the magnetic order. Surprisingly, post-growth annealing of FeGe at 560$^{\circ}$C can suppress the CDW order while annealing at 320$^{\circ}$C induces a long-range CDW order, with the ability to cycle between the states repeatedly by annealing. Here we perform transport, neutron scattering, scanning transmission electron microscopy (STEM), and muon spin rotation ($\mu$SR) experiments to unveil the microscopic mechanism of the annealing process and its impact on magneto-transport, CDW, and magnetic properties of FeGe. We find that 560$^{\circ}$C annealing creates germanium vacancies uniformly distributed throughout the FeGe kagome lattice, which prevent the formation of Ge-Ge dimers necessary for the CDW order. Upon annealing at 320$^{\circ}$C, the system segregates into stoichiometric FeGe regions with long-range CDW order and regions with stacking faults that act as nucleation sites for the CDW. The presence or absence of CDW order greatly affects the anomalous Hall effect, incommensurate magnetic order, and spin-lattice coupling in FeGe, thus placing FeGe as the only known kagome lattice material with a tunable CDW and magnetic order, potentially useful for sensing and information transmission.

Magnetic kagome materials provide a fascinating playground for exploring the interplay of magnetism, correlation and topology. Many magnetic kagome systems have been reported including the binary FemXn (X=Sn, Ge; m:n = 3:1, 3:2, 1:1) family and the rare earth RMn6Sn6 (R = rare earth) family, where their kagome flat bands are calculated to be near the Fermi level in the paramagnetic phase. While partially filling a kagome flat band is predicted to give rise to a Stoner-type ferromagnetism, experimental visualization of the magnetic splitting across the ordering temperature has not been reported for any of these systems due to the high ordering temperatures, hence leaving the nature of magnetism in kagome magnets an open question. Here, we probe the electronic structure with angle-resolved photoemission spectroscopy in a kagome magnet thin film FeSn synthesized using molecular beam epitaxy. We identify the exchange-split kagome flat bands, whose splitting persists above the magnetic ordering temperature, indicative of a local moment picture. Such local moments in the presence of the topological flat band are consistent with the compact molecular orbitals predicted in theory. We further observe a large spin-orbital selective band renormalization in the Fe d_xy+d_(x^2-y^2 ) spin majority channel reminiscent of the orbital selective correlation effects in the iron-based superconductors. Our discovery of the coexistence of local moments with topological flat bands in a kagome system echoes similar findings in magic-angle twisted bilayer graphene, and provides a basis for theoretical effort towards modeling correlation effects in magnetic flat band systems.

In magnetically ordered insulators, elementary quasiparticles manifest as spin waves - collective motions of localized magnetic moments propagating through the lattice - observed via inelastic neutron scattering. In effective spin-1/2 systems where geometric frustrations suppress static magnetic order, spin excitation continua can emerge, either from degenerate classical spin ground states or from entangled quantum spins characterized by emergent gauge fields and deconfined fractionalized excitations. Comparing the spin Hamiltonian with theoretical models can unveil the microscopic origins of these zero-field spin excitation continua. Here, we use neutron scattering to study spin excitations of the two-dimensional (2D) triangular-lattice effective spin-1/2 antiferromagnet CeMgAl11O19. Analyzing the spin waves in the field-polarized ferromagnetic state, we find that the spin Hamiltonian is close to an exactly solvable 2D triangular-lattice XXZ model, where degenerate 120$^\circ$ ordered ground states - umbrella states - develop in the zero temperature limit. We then find that the observed zero-field spin excitation continuum matches the calculated ensemble of spin waves from the umbrella state manifold, and thus conclude that CeMgAl11O19 is the first example of an exactly solvable spin liquid on a triangular lattice where the spin excitation continuum arises from the ground state degeneracy., Comment: 11 pages, 5 figures

Superconductivity and magnetism are antagonistic quantum matter, while their intertwining has long been considered in frustrated-lattice systems1-3. In this work, we utilize scanning tunneling microscopy and muon spin resonance to discover time-reversal symmetry-breaking superconductivity in kagome metal Cs(V,Ta)3Sb5, where the Cooper pairing exhibits magnetism and is modulated by it. In the magnetic channel, we observe spontaneous internal magnetism in a full-gap superconducting state. Under perturbations of inverse magnetic fields, we detect a time-reversal asymmetrical interference of Bogoliubov quasi-particles at a circular vector. At this vector, the pairing gap spontaneously modulates, which is distinct from pair density waves occurring at a point vector and consistent with the theoretical proposal of unusual interference effect under time-reversal symmetry-breaking. The correlation between internal magnetism, Bogoliubov quasi-particles, and pairing modulation provides a chain of experimental clues for time-reversal symmetry-breaking kagome superconductivity., Comment: To appear in Nature Materials (2024)

As many Kagome metals, the topological superconductor AV$_3$Sb$_5$ with (A = K,Rb,Cs) hosts a charge density wave . A related chiral flux phase that breaks the time-reversal symmetry has been further theoretically predicted in these materials. The flux phase is associated with loop currents that produce ordered orbital magnetic moments, which would occur at the momentum points, $\bf M$, characterizing the charge-density wave state. Polarized neutron-diffraction experiments have been performed on an assembly of single crystals of ${\rm CsV_3Sb_5}$ to search for such orbital magnetic moments. No evidence for the existence of a three-dimensionally ordered moment is found at any temperature at the first ${\bf M_1}$=(1/2,0,0) point in the Brillouin zone within an excellent experimental uncertainty, ${\it i.e.}$ ${\bf m}=0 \pm 0.01\mu_B$ per vanadium atom. However, a hint to a magnetic orbital moment is found in the second Brillouin zone at {\bf M$_2$}=(1/2,1/2,0) at the detection limit of the experiment. Some loop currents patterns flowing ${\it only}$ on vanadium triangles are able to account for this finding suggesting an ordered orbital magnetic moment of, at most, $\sim 0.02 \pm 0.01\mu_B$ per vanadium triangle., Comment: 11 figures

In the quest for novel quantum states driven by topology and correlation, kagome lattice materials have garnered significant interest due to their distinctive electronic band structures, featuring flat bands (FBs) arising from the quantum destructive interference of the electronic wave function. The tuning of the FBs to the chemical potential would lead to the possibility of liberating electronic instabilities that lead to emergent electronic orders. Despite extensive studies, direct evidence of FBs tuned to the chemical potential and their participation in emergent electronic orders have been lacking in bulk quantum materials. Here using a combination of Angle-Resolved Photoemission Spectroscopy (ARPES) and Density Functional Theory (DFT), we reveal that the low-energy electronic structure of the recently discovered Cr-based kagome metal superconductor CsCr3Sb5 is dominated by a pervasive FB in close proximity to, and below the Fermi level. A comparative analysis with orbital-projected DFT and polarization dependence measurement uncovers that an orbital-selective renormalization mechanism is needed to reconcile the discrepancy with the DFT calculations, which predict the FB to appear 200 meV above the Fermi level. Furthermore, we observe the FB to shift away from the Fermi level by 20 meV in the low-temperature density wave-ordered phase, highlighting the role of the FB in the emergent electronic order. Our results reveal CsCr3Sb5 to stand out as a promising platform for further exploration into the effects of FBs near the Fermi level on kagome lattices, and their role in emergent orders in bulk quantum materials.

Hexagonal boron nitride (h-BN) is brittle, however, its atomic-scale structural engineering can lead to unprecedented physical properties. Here we report the bulk synthesis of high-density crystalline h-BN solids by using high-temperature spark plasma sintering (SPS) of micron size h-BN powders. In addition to the high mechanical strength and ductile response of such materials, we have obtained anomalous values of dielectric constant beyond theoretical limits, high thermal conductivity, and exceptional neutron radiation shielding capability. Through exhaustive characterizations we reveal that SPS induces non-basal plane crystallinity, twisting of layers, and facilitates inter-grain fusion with a high degree of in-plane alignment across macroscale dimensions, resulting in near-theoretical density and anomalous properties. Our findings highlight the importance of material design, via new approaches such as twisting and interconnections between atomically thin layers, to create novel ceramics with properties that could go beyond their intrinsic theoretical predictions., Comment: Authors revised version, 46 pages, 4 figures

Understanding spin and lattice excitations in a metallic magnetic ordered system form the basis to unveil the magnetic and lattice exchange couplings and their interactions with itinerant electrons. Kagome lattice antiferromagnet FeGe is interesting because it displays rare charge density wave (CDW) deep inside the antiferromagnetic ordered phase that interacts with the magnetic order. We use neutron scattering to study the evolution of spin and lattice excitations across the CDW transition $T_{\rm CDW}$ in FeGe. While spin excitations below $\sim$100 meV can be well described by spin waves of a spin-1 Heisenberg Hamiltonian, spin excitations at higher energies are centered around the Brillouin zone boundary and extend up to $\sim180$ meV consistent with quasiparticle excitations across spin-polarized electron-hole Fermi surfaces. Furthermore, $c$-axis spin wave dispersion and Fe-Ge optical phonon modes show a clear hardening below $T_{\rm CDW}$ due to spin-charge-lattice coupling but with no evidence for a phonon Kohn anomaly. By comparing our experimental results with density functional theory calculations in absolute units, we conclude that FeGe is a Hund's metal in the intermediate correlated regime where magnetism has contributions from both itinerant and localized electrons arising from spin polarized electronic bands near the Fermi level.

A quantum spin liquid (QSL) arises from a highly entangled superposition of many degenerate classical ground states in a frustrated magnet, and is characterized by emergent gauge fields and deconfined fractionalized excitations (spinons). Because such a novel phase of matter is relevant to high-transition-temperature superconductivity and quantum computation, the microscopic understanding of QSL states is a long-sought goal in condensed matter physics. The 3D pyrochlore lattice of corner-sharing tetrahedra can host a QSL with U(1) gauge fields called quantum spin ice (QSI), which is a quantum (with effective $S=1/2$) analog of the classical (with large effective moment) spin ice. A key difference between QSI and classical spin ice is the predicted presence of the linearly dispersing collective excitations near zero energy, dubbed the "photons", arising from emergent quantum electrodynamics, in addition to the spinons at higher energies. Recently, 3D pyrochlore systems Ce2M2O7 (M = Sn, Zr, Hf) have been suggested as effective $S=1/2$ QSI candidates, but there has been no evidence of quasielastic magnetic scattering signals from photons, a key signature for a QSI. Here, we use polarized neutron scattering experiments on single crystals of Ce2Zr2O7 to conclusively demonstrate the presence of magnetic excitations near zero energy at 50 mK in addition to signatures of spinons at higher energies. By comparing the energy (E), wave vector (Q), and polarization dependence of the magnetic excitations with theoretical calculations, we conclude that Ce2Zr2O7 is the first example of a dipolar-octupolar $\pi$ flux QSI with dominant dipolar Ising interactions, therefore identifying a microscopic Hamiltonian responsible for a QSL.

The discovery of the charge density wave order (CDW) within a magnetically ordered phase in the kagome lattice FeGe has provided a promising platform to investigate intertwined degrees of freedom in kagome lattices. Recently, a method based on post-annealing has been suggested to manipulate the CDW order in kagome FeGe towards either long-range or suppressed orders. Here, we provide a comprehensive comparison of the experimentally measured electronic structures of FeGe crystals that have undergone different post-annealing procedures and demonstrate the remarkable effectiveness on tuning the CDW gap without strong perturbation on the underlying electronic structure. Moreover, we observe an additional low temperature transition that only appears in crystals with a long-range CDW order, which we associate with a lattice-spin coupled order. Our work indicates a likely strong sensitivity of the CDW order to disorder in FeGe, and provides evidence for strong coupling between the electronic, lattice, and spin degrees of freedom in this kagome magnet.

We report on the charge dynamics of kagome FeGe, an antiferromagnet with a charge density wave (CDW) transition at $T_{\mathrm{CDW}} \simeq 105$ K, using polarized infrared spectroscopy and band structure calculations. We reveal a pronounced optical anisotropy, various excitations associated with flat bands and van Hove singularities (VHSs), and a moderate level of electronic correlations. Notably, there are two types of remarkable spectral weight (SW) redistributions for above and below $T_{\mathrm{CDW}}$. The former involves a transfer between incoherent and coherent excitations driven by the magnetic splitting-induced elevation of flat bands. The latter manifests itself as a sudden change of SW from low to high energies for both $a$ and $c$ directions, suggesting a first-order transition and the three-dimensional nature of CDW. These anomalies in SW significantly differ from those observed in other kagome metals like CsV$_3$Sb$_5$, where the nesting of VHSs results in a pronounced CDW gap feature. Instead, our findings can be accounted for by the jump of VHSs relative to the Fermi energy via a first-order structural transition involving large partial Ge1-dimerization. Our study thus unveils a complex interplay among structure, magnetism, electronic correlations, and charge order in FeGe, offering valuable insights for a comprehensive understanding of CDW order in kagome systems., Comment: 7 pages, 3 figures

A hallmark of unconventional superconductors is their complex electronic phase diagrams where "intertwined orders" of charge-spin-lattice degrees of freedom compete and coexist as in copper oxides and iron pnictides. While the electronic phase diagram of kagome lattice superconductor such as CsV3Sb5 also exhibits complex behavior involving coexisting and competing charge density wave order and superconductivity, much is unclear about the microscopic origin of superconductivity. Here, we study the vortex lattice (VL) in superconducting state of Cs(V0.86Ta0.14)3Sb5, where the Ta-doping suppresses charge order and enhances superconductivity. Using small-angle neutron scattering, a strictly bulk probe, we show that the VL exhibits a strikingly conventional behavior. This includes a triangular VL with a period consistent with 2e-pairing, a field dependent scattering intensity that follows a London model, and a temperature dependence consistent with a uniform superconducting gap expected for s-wave pairing. These results suggest that optimal bulk superconductivity in Cs(V1-xTax)3Sb5 arises from a conventional Bardeen-Cooper-Schrieffer electron-lattice coupling, different from spin fluctuation mediated unconventional copper and iron based superconductors., Comment: Multiple revisions

We use elastic and inelastic neutron scattering (INS) to study the antiferromagnetic (AF) phase transitions and spin excitations in the two-dimensional (2D) zig-zag antiferromagnet FePSe$_3$. By determining the magnetic order parameter across the AF phase transition, we conclude that the AF phase transition in FePSe$_3$ is first-order in nature. In addition, our INS measurements reveal that the spin waves in the AF ordered state have a large easy-axis magnetic anisotropy gap, consistent with an Ising Hamiltonian, and possible biquadratic magnetic exchange interactions. On warming across $T_N$, we find that dispersive spin excitations associated with three-fold rotational symmetric AF fluctuations change into FM spin fluctuations above $T_N$. These results suggest that the first-order AF phase transition in FePSe$_3$ may arise from the competition between $C_3$ symmetric AF and $C_1$ symmetric FM spin fluctuations around $T_N$, in place of a conventional second-order AF phase transition.

Understanding the magnetoresistance (MR) of a magnetic material forms the basis for uncovering the orbital mechanisms and charge-spin interactions in the system. Although the parent state of iron-based high-temperature superconductors, including $BaFe_2As_2$, exhibits unusual electron transport properties resulting from spin and charge correlations, there is still valuable insight to be gained by understanding the in-plane MR effect due to twin domains in the orthorhombic antiferromagnetic (AF) ordered state. Here, we study the in-plane magnetoresistance anisotropy in detwinned $BaFe_2As_2$ and compare the results to the non-magnetic Ni-doped sample. We find that in the antiferromagnetically ordered state, $BaFe_2As_2$ exhibits anisotropic MR that becomes large at low temperatures and high fields. Both transverse and longitudinal MRs are highly anisotropic and dependent on the field and current orientations. These results cannot be fully explained by calculations considering only the anisotropic Fermi surface. Instead, the spin orientation of the ordered moment also affects the MR effect, suggesting the presence of a large charge-spin interaction in $BaFe_2As_2$ that is not present in the Ni-doped material.

The unusual quantum-disordered magnetic ground state intertwined with superconductivity and electronic nematicity in FeSe has been a research focus in iron-based superconductors. However, the intrinsic spin excitations across the entire Brillouin zone in detwinned FeSe, which forms the basis for a microscopic understanding of the magnetic state and superconductivity, remain to be determined. Here, we use inelastic neutron scattering to map out the spin excitations of FeSe dewtinned with a uniaxial-strain device. We find that the stripe spin excitations (Q=(1, 0)/(0, 1)) exhibit the $C_2$ symmetry up to $E\approx120$ meV, while the N{\'e}el spin excitations (Q=(1, 1)) retain their $C_4$ symmetry in the nematic state. The temperature dependence of the difference in the spin excitations at Q=(1, 0) and (0, 1) for temperatures above the structural phase transition unambiguously shows the establishment of the nematic quantum disordered state. The similarity of the N\'eel excitations in FeSe and NaFeAs suggests that the N\'eel excitations are driven by the enhanced electron correlations in the $3d_{xy}$ orbital. By determining the key features of the stripe excitations and fitting their dispersions using a Heisenberg Hamiltonian with biquadratic interaction ($J_1$-$K$-$J_2$), we establish a spin-interaction phase diagram and conclude that FeSe is close to a crossover region between the antiferroquadrupolar, N\'eel, and stripe ordering regimes. The results provide an experimental basis for establishing a microscopic theoretical model to describe the origin and intertwining of the emergent orders in iron-based superconductors., Comment: 9 pages, 5 figures

The recently discovered (Ba,Sr)Ni$_2$As$_2$ family provides an ideal platform for investigating the interaction between electronic nematicity and superconductivity. Here we report the muon spin relaxation ($\mu$SR) measurements on BaNi$_2$As$_2$. Transverse-field $\mu$SR experiments indicate that the temperature dependence of superfluid density is best fitted with a single-band $s$-wave model. On the other hand, the magnetic penetration depth $\lambda$ shows magnetic field dependence, which contradicts with the single-band fully-gapped scenario. Zero-field $\mu$SR experiments indicate the absence of spontaneous magnetic field in the superconducting state, showing the preservation of time-reversal symmetry in the superconducting state. Our $\mu$SR experiments suggest that BaNi$_2$As$_2$ is a fully-gapped multiband superconductor. The superconducting gap amplitudes of each band are nearly the same while different bands exhibit different coherence lengths. The present work helps to elucidate the controversial superconducting property of this parent compound, paving the way for further research on doping the system with Sr to enhance superconductivity., Comment: Accepted by Phys. Rev. B

The two-dimensional (2D) material Cr$_2$Ge$_2$Te$_6$ is a member of the class of insulating van der Waals magnets. Here, using high resolution angle-resolved photoemission spectroscopy in a detailed temperature dependence study, we identify a clear response of the electronic structure to a dimensional crossover in the form of two distinct temperature scales marking onsets of modifications in the electronic structure. Specifically, we observe Te $p$-orbital-dominated bands to undergo changes at the Curie transition temperature T$_C$ while the Cr $d$-orbital-dominated bands begin evolving at a higher temperature scale. Combined with neutron scattering, density functional theory calculations, and Monte Carlo simulations, we find that the electronic system can be consistently understood to respond sequentially to the distinct temperatures at which in-plane and out-of-plane spin correlations exceed a characteristic length scale. Our findings reveal the sensitivity of the orbital-selective electronic structure for probing the dynamical evolution of local moment correlations in vdW insulating magnets., Comment: PRB, in press

We use transport measurements to determine the in-plane anisotropy of the upper critical field Hc2 in detwinned superconducting Ba(Fe1-xMx)2As2 (M = Co, Ni) single crystals. In previous measurements on twinned single crystals, the charge carrier doping dependence (x) of the upper critical field anisotropy for fields along the inter-planar (c-axis) and in-plane field directions was found to increase in the overdoped regime. For underdoped samples, which exhibit a spin nematic phase below the tetragonal to orthorhombic structural transition temperature Ts , we find that Hc2 along the a-axis is considerably lower than that along the b-axis. The upper critical field anisotropy disappears in the over-doped regime when the system becomes tetragonal. By combining these results with inelastic neutron scattering studies of spin excitations, and angle-resolved photoemission spectroscopy, we conclude that superconductivity in under-doped iron pnictides is orbital selective - with a dominant contribution from electrons with the dyz orbital character and being intimately associated with spin excitations.

Electronic correlation effects are manifested in quantum materials when either the onsite Coulomb repulsion is large or the electron kinetic energy is small. The former is the dominant effect in the cuprate superconductors or heavy fermion systems while the latter in twisted bilayer graphene or geometrically frustrated metals. However, the simultaneous cooperation of both effects in the same quantum material--the design principle to produce a correlated topological flat bands pinned at the Fermi level--remains rare. Here, using angle-resolved photoemission spectroscopy, we report the observation of a flat band at the Fermi level in a 3$d$ pyrochlore metal CuV$_2$S$_4$. From a combination of first-principles calculations and slave-spin calculations, we understand the origin of this band to be a destructive quantum-interference effect associated with the V pyrochlore sublattice and further renormalization to the Fermi level by electron interactions in the partially filled V $t_{2g}$ orbitals. As a result, we find transport behavior that indicates a deviation from Fermi-liquid behavior as well as a large Sommerfeld coefficient. Our work demonstrates the pathway into correlated topology by constructing and pinning correlated flat bands near the Fermi level out of a pure $d$-electron system by the combined cooperation of local Coulomb interactions and geometric frustration in a pyrochlore lattice system., Comment: 23 pages, 4 figures, to appear in Nature Physics

Ever since the discovery of the charge density wave (CDW) transition in the kagome metal CsV$_3$Sb$_5$, the nature of its symmetry breaking is under intense debate. While evidence suggests that the rotational symmetry is already broken at the CDW transition temperature ($T_{\rm CDW}$), an additional electronic nematic instability well below $T_{\rm CDW}$ has been reported based on the diverging elastoresistivity coefficient in the anisotropic channel ($m_{E_{2g}}$). Verifying the existence of a nematic transition below $T_{\rm CDW}$ is not only critical for establishing the correct description of the CDW order parameter, but also important for understanding low-temperature superconductivity. Here, we report elastoresistivity measurements of CsV$_3$Sb$_5$ using three different techniques probing both isotropic and anisotropic symmetry channels. Contrary to previous reports, we find the anisotropic elastoresistivity coefficient $m_{E_{2g}}$ is temperature-independent, except for a step jump at $T_{\rm CDW}$. The absence of nematic fluctuations is further substantiated by measurements of the elastocaloric effect, which show no enhancement associated with nematic susceptibility. On the other hand, the symmetric elastoresistivity coefficient $m_{A_{1g}}$ increases below $T_{\rm CDW}$, reaching a peak value of 90 at $T^* = 20$ K. Our results strongly indicate that the phase transition at $T^*$ is not nematic in nature and the previously reported diverging elastoresistivity is due to the contamination from the $A_{1g}$ channel., Comment: 11 pages, 5 figures, to appear in Physical Review X

Spontaneous symmetry breaking-the phenomenon where an infinitesimal perturbation can cause the system to break the underlying symmetry-is a cornerstone concept in the understanding of interacting solid-state systems. In a typical series of temperature-driven phase transitions, higher temperature phases are more symmetric due to the stabilizing effect of entropy that becomes dominant as the temperature is increased. However, the opposite is rare but possible when there are multiple degrees of freedom in the system. Here, we present such an example of a symmetry-ascending phenomenon in a magnetic kagome metal FeGe by utilizing neutron Larmor diffraction and Raman spectroscopy. In the paramagnetic state at 460K, we confirm that the crystal structure is indeed hexagonal kagome lattice. On cooling to TN, the crystal structure changes from hexagonal to monoclinic with in-plane lattice distortions on the order of 10^(-4) and the associated splitting of the double degenerate phonon mode of the pristine kagome lattice. Upon further cooling to TCDW, the kagome lattice shows a small negative thermal expansion, and the crystal structure becomes more symmetric gradually upon further cooling. Increasing the crystalline symmetry upon cooling is unusual, it originates from an extremely weak structural instability that coexists and competes with the CDW and magnetic orders. These observations are against the expectations for a simple model with a single order parameter, hence can only be explained by a Landau free energy expansion that takes into account multiple lattice, charge, and spin degrees of freedom. Thus, the determination of the crystalline lattice symmetry as well as the unusual spin-lattice coupling is a first step towards understanding the rich electronic and magnetic properties of the system and sheds new light on intertwined orders where the lattice degree of freedom is no longer dominant., Comment: 20 pages with 10 figures, replaced with journal version

A spin-1/2 triangular-lattice antiferromagnet is a prototypical frustrated quantum magnet, which exhibits remarkable quantum many-body effects that arise from the synergy between geometric spin frustration and quantum fluctuations. It can host quantum frustrated magnetic topological phenomena like quantum spin liquid (QSL) states, highlighted by the presence of fractionalized quasiparticles within a continuum of magnetic excitations. In this work, we use neutron scattering to study CoZnMo$_3$O$_8$, which has a triangular lattice of Jeff = 1/2 Co2+ ions with octahedral coordination. We found a wave-vector-dependent excitation continuum at low energy that disappears with increasing temperature. Although these excitations are reminiscent of a spin excitation continuum in a QSL state, their presence in CoZnMo$_3$O$_8$ originates from magnetic intersite disorder-induced dynamic spin states with peculiar excitations. Our results, therefore, give direct experimental evidence for the presence of a disorder-induced spin excitation continuum.

Two-dimensional kagome metals consisting of corner-sharing triangles offer a unique platform for studying strong electron correlations and band topology due to its geometrically frustrated lattice structure. The similar energy scales between spin, lattice, and electronic degrees of freedom in these systems give rise to competing quantum phases such as charge density wave (CDW), magnetic order, and superconductivity. For example, kagome metal FeGe first exhibits A-type collinear antiferromagnetic (AFM) order at T_N ~ 400 K, then establishes a CDW phase coupled with AFM ordered moment below T_CDW ~ 100 K, and finally forms a $c$-axis double cone AFM structure around T_Canting ~ 60 K. Here we use neutron scattering to demonstrate the presence of gapless incommensurate spin excitations associated with the double cone AFM structure at temperatures well above T_Canting and T_CDW that merge into gapped commensurate spin waves from the A-type AFM order. While commensurate spin waves follow the Bose population factor and can be well described by a local moment Heisenberg Hamiltonian, the incommensurate spin excitations first appear below T_N where AFM order is commensurate, start to deviate from the Bose population factor around T_CDW, and peaks at T_Canting, consistent with a critical scattering of a second order magnetic phase transition, as a function of decreasing temperature. By comparing these results with density functional theory calculations, we conclude that the incommensurate magnetic structure arises from the nested Fermi surfaces of itinerant electrons and the formation of a spin density wave order. The temperature dependence of the incommensurate spin excitations suggests a coupling between spin density wave and CDW order, likely due to flat electronic bands near the Fermi level around T_N and associated electron correlation effects., Comment: Submitted for publication in April 2023

The ability to reversibly toggle between two distinct states in a non-volatile method is important for information storage applications. Such devices have been realized for phase-change materials, which utilizes local heating methods to toggle between a crystalline and an amorphous state with distinct electrical properties. To expand such kind of switching between two topologically distinct phases requires non-volatile switching between two crystalline phases with distinct symmetries. Here we report the observation of reversible and non-volatile switching between two stable and closely-related crystal structures with remarkably distinct electronic structures in the near room temperature van der Waals ferromagnet Fe$_{5-\delta}$GeTe$_2$. From a combination of characterization techniques we show that the switching is enabled by the ordering and disordering of an Fe site vacancy that results in distinct crystalline symmetries of the two phases that can be controlled by a thermal annealing and quenching method. Furthermore, from symmetry analysis as well as first principle calculations, we provide understanding of the key distinction in the observed electronic structures of the two phases: topological nodal lines compatible with the preserved global inversion symmetry in the site-disordered phase, and flat bands resulting from quantum destructive interference on a bipartite crystaline lattice formed by the presence of the site order as well as the lifting of the topological degeneracy due to the broken inversion symmetry in the site-ordered phase. Our work not only reveals a rich variety of quantum phases emergent in the metallic van der Waals ferromagnets due to the presence of site ordering, but also demonstrates the potential of these highly tunable two-dimensional magnets for memory and spintronics applications.

Magnetism in two-dimensional (2D) materials has attracted considerable attention recently for both fundamental understanding of magnetism and their tunability towards device applications. The isostructural Fe$_3$GeTe$_2$ and Fe$_3$GaTe$_2$ are two members of the Fe-based van der Waals (vdW) ferromagnet family, but exhibit very different Curie temperatures (T$_C$) of 210 K and 360 K, respectively. Here, by using angle-resolved photoemission spectroscopy and density functional theory, we systematically compare the electronic structures of the two compounds. Qualitative similarities in the Fermi surface can be found between the two compounds, with expanded hole pockets in Fe$_3$GaTe$_2$ suggesting additional hole carriers compared to Fe$_3$GeTe$_2$. Interestingly, we observe no band shift in Fe$_3$GaTe$_2$ across its T$_C$ of 360 K, compared to a small shift in Fe$_3$GeTe$_2$ across its T$_C$ of 210 K. The weak temperature-dependent evolution strongly deviates from the expectations of an itinerant Stoner mechanism. Our results suggest that itinerant electrons have minimal contributions to the enhancement of T$_C$ in Fe$_3$GaTe$_2$ compared to Fe$_3$GeTe$_2$, and that the nature of ferromagnetism in these Fe-based vdW ferromagnets must be understood with considerations of the electron correlations.

An experimental determination of electronic phase diagrams of high-transition temperature (high-$T_c$) superconductors forms the basis for a microscopic understanding of unconventional superconductivity. For most high-$T_c$ superconductors, the electronic phase diagrams are established through partial chemical substitution, which also induces lattice disorder. Here we show that symmetry-specific uniaxial strain can be used to study electronic phases in iron-based superconductors, composed of two-dimensional nearly square iron lattice planed separated by other elements. By applying tunable uniaxial strain along different high symmetry directions and carrying out transport measurements, we establish strain-tuning dependent electronic nematicity, antiferromagnetic (AF) order, and superconductivity of BaFe$_2$(As$_{1-x}$P$_{x}$)$_2$ superconductor. We find that uniaxial strain along the nearest Fe-Fe direction can dramatically tune the AF order and superconductivity, producing an electronic phase diagram clearly different from the chemical substitution-induced one. Our results thus establish strain tuning as a way to study the intertwined orders in correlated electron materials without using chemical substitution.

Emergent phases often appear when the electronic kinetic energy is comparable to the Coulomb interactions. One approach to seek material systems as hosts of such emergent phases is to realize localization of electronic wavefunctions due to the geometric frustration inherent in the crystal structure, resulting in flat electronic bands. Recently, such efforts have found a wide range of exotic phases in the two-dimensional kagome lattice, including magnetic order, time-reversal symmetry breaking charge order, nematicity, and superconductivity. However, the interlayer coupling of the kagome layers disrupts the destructive interference needed to completely quench the kinetic energy. Here we demonstrate that an interwoven kagome network-a pyrochlore lattice-can host a three dimensional (3D) localization of electron wavefunctions. Meanwhile, the nonsymmorphic symmetry of the pyrochlore lattice guarantees all band crossings at the Brillouin zone X point to be 3D gapless Dirac points, which was predicted theoretically but never yet observed experimentally. Through a combination of angle-resolved photoemission spectroscopy, fundamental lattice model and density functional theory calculations, we investigate the novel electronic structure of a Laves phase superconductor with a pyrochlore sublattice, CeRu$_2$. We observe flat bands originating from both the Ce 4$f$ orbitals as well as from the 3D destructive interference of the Ru 4$d$ orbitals. We further observe the nonsymmorphic symmetry-protected 3D gapless Dirac cones at the X point. Our work establishes the pyrochlore structure as a promising lattice platform to realize and tune novel emergent phases intertwining topology and many-body interactions., Comment: 27 pages, 4 figures

Boron nitride (BN) is an exceptional material and among its polymorphs, two-dimensional (2D) hexagonal and three-dimensional (3D) cubic BN (h-BN and c-BN) phases are most common. The phase stability regimes of these BN phases are still under debate and phase transformations of h-BN/c-BN remain a topic of interest. Here, we investigate the phase stability of 2D/3D h-BN/c-BN nanocomposites and show that the co-existence of two phases can lead to strong non-linear optical properties and low thermal conductivity at room temperature. Furthermore, spark-plasma sintering of the nanocomposite shows complete phase transformation to 2D h-BN with improved crystalline quality, where 3D c-BN grain sizes governs the nucleation and growth kinetics. Our demonstration might be insightful in phase engineering of BN polymorphs based nanocomposites with desirable properties for optoelectronics and thermal energy management applications., Comment: 29 pages, 5 figures

Magnetic order in most materials occurs when magnetic ions with finite moments in a crystalline lattice arrange in a particular pattern below the ordering temperature determined by exchange interactions between the ions. However, when the crystal electric field (CEF) effect results in a spin-singlet ground state on individual magnetic sites, the collective ground state of the system can either remain non-magnetic, or more intriguingly, the exchange interactions between neighboring ions, provided they are sufficiently strong, can admix the excited CEF levels, resulting in a magnetically ordered ground state. The collective magnetic excitations in such a state are so-called spin excitons that describe the CEF transitions propagating through the lattice. In most cases, spin excitons originating from CEF levels of a localized single ion are dispersion-less in momentum (reciprocal) space and well-defined in both the magnetically ordered and paramagnetic states. Here we use thermodynamic and neutron scattering experiments to study stoichiometric Ni2Mo3O8 without site disorder, where Ni2+ ions form a bipartite honeycomb lattice comprised of two triangular lattices, with ions subject to the tetrahedral and octahedral crystalline environment, respectively. We find that in both types of ions, the CEF excitations have nonmagnetic singlet ground states, yet the material has long-range magnetic order. Furthermore, CEF spin excitons from the triangular-lattice arrangement of tetrahedral sites form, in both the antiferromagnetic and paramagnetic states, a dispersive diffusive pattern around the Brillouin zone boundary in reciprocal space. The present work thus demonstrates that spin excitons in an ideal triangular lattice magnet can have dispersive excitations, irrespective of the existence of static magnetic order, and this phenomenon is most likely due to spin entanglement and geometric frustrations.

The Dicke model describes the cooperative interaction of an ensemble of two-level atoms with a single-mode photonic field and exhibits a quantum phase transition as a function of light--matter coupling strength. Extending this model by incorporating short-range atom--atom interactions makes the problem intractable but is expected to produce new phases. Here, we simulate such an extended Dicke model using a crystal of ErFeO$_3$, where the role of atoms (photons) is played by Er$^{3+}$ spins (Fe$^{3+}$ magnons). Through magnetocaloric effect and terahertz magnetospectroscopy measurements, we demonstrated the existence of a novel atomically ordered phase in addition to the superradiant and normal phases that are expected from the standard Dicke model. Further, we elucidated the nature of the phase boundaries in the temperature--magnetic-field phase diagram, identifying both first-order and second-order phase transitions. These results lay the foundation for studying multiatomic quantum optics models using well-characterized many-body condensed matter systems.

Kagome lattices host flat bands due to their frustrated lattice geometry, which leads to destructive quantum interference of electron wave functions. Here, we report imaging of the kagome flat band localization in real-space using scanning tunneling microscopy. We identify both the Fe3Sn kagome lattice layer and the Sn2 honeycomb layer with atomic resolution in kagome antiferromagnet FeSn. On the Fe3Sn lattice, at the flat band energy determined by the angle resolved photoemission spectroscopy, tunneling spectroscopy detects an unusual state localized uniquely at the Fe kagome lattice network. We further show that the vectorial in-plane magnetic field manipulates the spatial anisotropy of the localization state within each kagome unit cell. Our results are consistent with the real-space flat band localization in the magnetic kagome lattice. We further discuss the magnetic tuning of flat band localization under the spin-orbit coupled magnetic kagome lattice model., Comment: To appear in Communications Materials

One main theme in current condensed matter physics is the search of quantum spin liquid (QSL), an exotic magnetic state with strongly-fluctuating and highly-entangled spins down to zero temperature without static order. However, there is no consensus on the existence of a QSL ground state in any real material so far. The disorders and competing exchange interactions may prevent the formation of an ideal QSL state on frustrated spin lattices. Here we report systematic heat transport measurements on a honeycomb-lattice compound BaCo2(AsO4)2, which manifests magnetic order in zero field. In a narrow field range after the magnetic order is nearly suppressed by an in-plane field, in both perpendicular and parallel to the zigzag direction, a finite residual linear term of thermal conductivity is clearly observed, which is attributed to the mobile fractionalized spinon excitations. This provides smoking-gun evidence for a gapless QSL state in BaCo2(AsO4)2. We discuss the underlying physics to form this exotic gapless QSL state in Co2+ honeycomb lattice.

The anomalous Hall effect (AHE), typically observed in ferromagnetic (FM) metals with broken time-reversal symmetry, depends on electronic and magnetic properties. In Co$_{3}$Sn$_{2-x}$In$_{x}$S$_{2}$, a giant AHE has been attributed to Berry curvature associated with the FM Weyl semimetal phase, yet recent studies report complicated magnetism. We use neutron scattering to determine the spin dynamics and structures as a function of $x$ and provide a microscopic understanding of the AHE and magnetism interplay. Spin gap and stiffness indicate a contribution from Weyl fermions consistent with the AHE. The magnetic structure evolves from $c$-axis ferromagnetism at $x$ = 0 to a canted antiferromagnetic (AFM) structure with reduced $c$-axis moment and in-plane AFM order at $x$ = 0.12 and further reduced $c$-axis FM moment at $x$ = 0.3. Since noncollinear spins can induce non-zero Berry curvature in real space acting as a fictitious magnetic field, our results revealed another AHE contribution, establishing the impact of magnetism on transport.

Electron correlations often lead to emergent orders in quantum materials. Kagome lattice materials are emerging as an exciting platform for realizing quantum topology in the presence of electron correlations. This proposal stems from the key signatures of electronic structures associated with its lattice geometry: flat band induced by destructive interference of the electronic wavefunctions, topological Dirac crossing, and a pair of van Hove singularities (vHSs). A plethora of correlated electronic phases have been discovered amongst kagome lattice materials, including magnetism, charge density wave (CDW), nematicity, and superconductivity. These materials can be largely organized into two types: those that host magnetism and those that host CDW order. Recently, a CDW order has been discovered in the magnetic kagome FeGe, providing a new platform for understanding the interplay between CDW and magnetism. Here, utilizing angle-resolved photoemission spectroscopy, we observe all three types of electronic signatures of the kagome lattice: flat bands, Dirac crossings, and vHSs. From both the observation of a temperature-dependent shift of the vHSs towards the Fermi level as well as guidance via first-principle calculations, we identify the presence of the vHSs near the Fermi level (EF) to be driven by the development of underlying magnetic exchange splitting. Furthermore, we show spectral evidence for the CDW order as gaps that open on the near-EF vHS bands, as well as evidence of electron-phonon coupling from a kink on the vHS band together with phonon hardening observed by inelastic neutron scattering. Our observation points to the magnetic interaction-driven band modification resulting in the formation of the CDW order, indicating an intertwined connection between the emergent magnetism and vHS charge order in this moderately-correlated kagome metal., Comment: submitted on April 22, 2022

Quantum spin liquid (QSL) is a disordered state of quantum-mechanically entangled spins commonly arising from frustrated magnetic dipolar interactions. However, QSL in some pyrochlore magnets can also come from frustrated magnetic octupolar interactions. Although the key signature for both dipolar and octupolar interaction-driven QSL is the presence of a spin excitation continuum (spinons) arising from the spin quantum number fractionalization, an external magnetic field-induced ferromagnetic order will transform the spinons into conventional spin waves in a dipolar QSL. By contrast, in an octupole QSL, the spin waves carry octupole moments that do not couple, in the leading order, to the external magnetic field or to neutron moments but will contribute to the field dependence of the heat capacity. Here we use neutron scattering to show that the application of a large external magnetic field to Ce2Zr2O7, an octupolar QSL candidate, induces an Anderson-Higgs transition by condensing the spinons into a static ferromagnetic ordered state with octupolar spin waves invisible to neutrons but contributing to the heat capacity. Our theoretical calculations also provide a microscopic, qualitative understanding for the presence of octupole scattering at large wavevectors in Ce2Sn2O7 pyrochlore, and its absence in Ce2Zr2O7. Therefore, our results identify Ce2Zr2O7 as a strong candidate for an octupolar U (1) QSL, establishing that frustrated magnetic octupolar interactions are responsible for QSL properties in Ce-based pyrochlore magnets.

Spin and lattice are two fundamental degrees of freedom in a solid, and their fluctuations about the equilibrium values in a magnetic ordered crystalline lattice form quasiparticles termed magnons (spin waves) and phonons (lattice waves), respectively. In most materials with strong spin-lattice coupling (SLC), the interaction of spin and lattice induces energy gaps in the spin wave dispersion at the nominal intersections of magnon and phonon modes. Here we use neutron scattering to show that in the two-dimensional (2D) van der Waals honeycomb lattice ferromagnetic CrGeTe3, spin waves propagating within the 2D plane exhibit an anomalous dispersion, damping, and break-down of quasiparticle conservation, while magnons along the c axis behave as expected for a local moment ferromagnet. These results indicate the presence of dynamical SLC arising from the zero-temperature quantum fluctuations in CrGeTe3, suggesting that the observed in-plane spin waves are mixed spin and lattice quasiparticles fundamentally different from pure magnons and phonons., Comment: 12 pages, 4 figures; Nature Communication in press

We present the ultralow-temperature specific heat and thermal conductivity measurements on single crystals of triangular-lattice antiferromagnet Na$_2$BaCo(PO$_4$)$_2$, which was recently argued to host itinerant fermionic excitations, like a quantum spin liquid, above its antiferromagnetic phase transition temperature $T_{\rm N}$ = 0.148 K. In specific heat measurements, we confirm the peaks due to antiferromagnetic ordering when magnetic field $\mu_0 H \leq$ 1 T, roughly consistent with previous work [N. Li $et$ $al.$, Nat. Commun. 11, 4216 (2020)]. However, in thermal conductivity measurements, we observe negligible residual linear term in zero and finite magnetic fields, in sharp contrast to previous report [N. Li $et$ $al.$, Nat. Commun. 11, 4216 (2020)]. At 0.35 K, the thermal conductivity increases with field up to 3 T then saturates, similar to that of another triangular-lattice compound YbMgGaO$_4$, which further shows that the heat is conducted only by phonons with scattering from spins and boundary. Our results clearly demonstrate the absence of itinerant fermionic excitations in the disordered state above $T_{\rm N}$ in this frustrated antiferromagnet Na$_2$BaCo(PO$_4$)$_2$, thus such a state is not as exotic as previously reported., Comment: 6 pages, 4 figures

We report high pressure studies on the C-type antiferromagnetic semiconductor EuTe2 up to 36.0 GPa. A structural transition from the I4/mcm to C2/m space group is identified at ~16 GPa. Superconductivity is discovered above ~5 GPa in both the I4/mcm and C2/m space groups. In the low-pressure phase (< 16 GPa), the antiferromagnetic transition temperature is enhanced with increasing pressure due to the enhanced magnetic exchange interactions. Magnetoresistance measurements indicate an interplay between the local moments of Eu2+ and the conduction electrons of Te 5p orbits. The upper critical field of the superconductivity is well above the Pauli limit. Across the structural transition to the high-pressure phase (> 16 GPa), EuTe2 becomes nonmagnetic and the superconducting transition temperature evolves smoothly with the upper critical field below the Pauli limit. Therefore, the high upper critical field of EuTe2 in the low-pressure phase is due to the exchange field compensation effect of the Eu magnetic order and the superconductivity in both structures may arise in the framework of the BCS theory., Comment: 11 pages,5 figures with 8 pages supplementary

The emergence of unconventional superconductivity in proximity to intertwined electronic orders is especially relevant in the case of iron-based superconductors. Such order consists of an electronic nematic order and a spin density wave in these systems. BaNi$_2$As$_2$, like its well-known iron-based analog BaFe$_2$As$_2$, also hosts a symmetry-breaking structural transition that is coupled to a unidirectional charge density wave (CDW), providing a novel platform to study intertwined orders. Here, through a systematic angle-resolved photoemission spectroscopy study combined with a detwinning $B_1g$ uniaxial strain, we identify distinct spectral evidence of band evolution due to the structural transition as well as CDW-induced band folding. In contrast to the nematicity and spin density wave in BaFe$_2$As$_2$, the structural and CDW order parameters in BaNi$_2$As$_2$ are observed to be strongly coupled and do not separate in the presence of uniaxial strain. Our measurements point to a likely lattice origin of the CDW in BaNi$_2$As$_2$., Comment: 6 pages, 4 figures

We report the synthesis and characterization of RbNi$_2$Se$_2$, an analog of the iron chalcogenide superconductor Rb$_x$Fe$_2$Se$_2$, via transport, angle resolved photoemission spectroscopy, and density functional theory calculations. A superconducting transition at $T_{c}$ = 1.20 K is identified. In normal state, RbNi$_2$Se$_2$ shows paramagnetic and Fermi liquid behaviors. A large Sommerfeld coefficient yields a heavy effective electron mass of $m^{*}\approx6m_{e}$. In the superconducting state, zero-field electronic specific-heat data $C_{es}$ can be described by a two-gap BCS model, indicating that RbNi$_2$Se$_2$ is a multi-gap superconductor. Our density functional theory calculations and angle resolved photoemission spectroscopy measurements demonstrate that RbNi$_2$Se$_2$ exhibits relatively weak correlations and multi-band characteristics, consistent with the multi-gap superconductivity., Comment: 7 pages, 4 figures