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Anisotropy in strongly correlated materials is a central parameter in determining the electronic ground state and is tuned through the local crystalline electric field. This is notably the case in the CeCo$_{x}$Rh$_{1-x}$In$_{5}$ system where the ground-state wave function can provide the basis for antiferromagnetism and/or unconventional superconductivity. We develop a methodology to understand the local magnetic anisotropy and experimentally investigate with neutron spectroscopy applied to antiferromagnetic ($T_{N}$=3.8 K) CeRhIn$_{5}$ which is isostructural to $d$-wave superconducting ($T_{c}$=2.3 K) CeCoIn$_{5}$. Through diagonalizing the local crystal field Hamiltonian with discrete tetragonal $\mathrm{C}_{4}$ point group symmetry and coupling these states with the Random Phase Approximation (RPA), we find two distinct modes polarized along the crystallographic $c$ and $a-b$ planes, agreeing with experiment. The anisotropy and bandwidth, underlying the energy scale of these modes, are tuneable with a magnetic field which we use experimentally to separate in energy single and multiparticle excitations thereby demonstrating the instability of excitations polarized within the crystallographic $a-b$ plane in CeRhIn$_{5}$. We compare this approach to a $S_{eff}={1\over 2}$ parameterizations and argue for the need to extend conventional SU(2) theories of magnetic excitations to utilize the multi-level nature of the underlying crystal-field basis states constrained by the local point-group $\mathrm{C}_{4}$ symmetry., Comment: (17 pages, 8 figures, to be published in Physical Review B)

The vibrational properties of 2H-TaSe$_{2-x}$S$_x$ ($0 \le x \le 2$) single crystals were probed using Raman spectroscopy and density functional theory calculations. The end members revealed two out of four symmetry-predicted Raman active modes, together with the pronounced two-phonon structure, attributable to the enhanced electron-phonon coupling. Additional peaks become observable due to crystallographic disorder for the doped samples. The evolution of the E$_{2g}^2$ mode Fano parameter reveals that the disorder has weak impact on electron-phonon coupling, which is also supported by the persistence of two-phonon structure in doped samples. As such, this research provides thorough insights into the lattice properties, the effects of crystallographic disorder on Raman spectra, and the interplay of this disorder with the electron-phonon coupling in 2H-TaSe$_{2-x}$S$_x$ compounds.

Topological superconductors have long been sought for their potential use in quantum computing. The type-II Weyl semimetal MoTe$_{2}$ is an obvious candidate, exhibiting a superconducting state below 500 mK at ambient pressure, but the question remains whether the pairing is conventional $s^{++}$ or topological $s^{+-}$. The application of external pressure favors the superconducting state in MoTe$_{2}$ and suppresses the structural transition from $1T'$ to $T_{d}$. The competition between the two structures leads to a mixed phase that strongly enhances the disorder present in the system, remarkably without affecting the superconducting transition temperature, in contrast to the expectation of $s^{+-}$ pairing superconductivity. Our thorough analysis of the electrical and Hall resistivities as a function of pressure yields the most accurate temperature-pressure phase diagram available to date for MoTe$_{2}$ and a detailed view of the relationship between disorder and superconductivity, supporting a conventional $s^{++}$ pairing symmetry.

We utilize ultrafast photoexcitation to drive coherent lattice oscillations in the layered ferrimagnetic crystal Mn3Si2Te6, which significantly stiffen below the magnetic ordering temperature. We suggest that this is due to an exchange-mediated contraction of the lattice, stemming from strong magneto-structural coupling in this material. Additionally, simulations of the transient incoherent dynamics reveal the importance of spin relaxation channels mediated by optical and acoustic phonon scattering. Our findings highlight the importance of spin-lattice coupling in van der Waals magnets and a promising route for their dynamic optical control through their intertwined electronic, lattice, and spin degrees of freedom.

We report a study of selenospinel Cu$_{6-x}$Fe$_{4+x}$Sn$_{12}$Se$_{32}$ ($x$ = 0, 1, 2) single crystals, which crystalize in a cubic structure with the $Fd\overline{3}m$ space group, and show typical semiconducting behavior. The large discrepancy between the activation energy for electrical conductivity $E_\rho$ (32.3 $\sim$ 69.8 meV), and for thermopower $E_\textrm{S}$ (3.2 $\sim$ 11.5 meV), indicates a polaronic transport mechanism between 350 and 50 K. With decreasing temperature, it evolves into variable-range hopping conduction. Furthermore, the heat capacity shows a hump around 25(5) K and diverges from the Debye $T^3$ law at low temperatures, indicating the observation of structural glassy features in these crystalline solids., Comment: arXiv admin note: text overlap with arXiv:2210.16447

The discovery of long-range magnetic ordering in atomically thin materials catapulted the van der Waals (vdW) family of compounds into an unprecedented popularity. In particular, with a current push in space exploration, it is beneficial to study how the properties of such materials evolve under proton irradiation. Owing to their robust intra-layer stability and sensitivity to external perturbations, these materials provide excellent opportunities for studying proton irradiation as a non-destructive tool for controlling their magnetic properties. Specifically, the exfoliable Cr2Si2Te6 (CST) is a ferromagnetic semiconductor with the Curie temperature (TC) of ~32 K. Here, we have investigated the magnetic properties of CST upon proton irradiation as a function of fluence (1 x 1015, 5 x 1015, 1 x 1016, 5 x 1016, and 1 x 1018 H+/cm2) by employing variable-temperature, variable-field magnetization measurements coupled with electron paramagnetic resonance (EPR) spectroscopy and detail how the magnetization, magnetic anisotropy and EPR spectral parameters vary as a function of proton fluence across the magnetic phase transition. While the TC remains constant as a function of proton fluence, we observed that the saturation magnetization and magnetic anisotropy diverge at the proton fluence of 5 x 1016 H+/cm2, which is prominent in the ferromagnetic phase, in particular. This work demonstrates that proton irradiation is a feasible method for modifying the magnetic properties and local magnetic interactions of vdWs crystals, which represents a significant step forward in the design of future spintronic and magneto-electronic applications.

Intermetallic narrow-gap semiconductors have been intensively explored due to their large thermoelectric power at low temperatures and a possible role of strong electronic correlations in their unusual thermodynamic and transport properties. Here we study the optical spectra and vibrational properties of $\mathrm{FeGa_3}$ single crystal. The optical conductivity indicates that $\mathrm{FeGa_3}$ has a direct band gap of $\sim 0.7$\,eV, consistent with density functional theory (DFT) calculations. Most importantly, we find a substantial spectral weight also below 0.4~eV, which is the energy of the indirect (charge) gap found in resistivity measurements and ab initio calculations. We find that the spectral weight below the gap decreases with increasing temperature, which indicates that it originates from the impurity states and not from the electronic correlations. Interestingly, we did not find any signatures of the impurity states in vibrational spectra. The infrared and Raman vibrational lines are narrow and weakly temperature dependent. The vibrational frequencies are in excellent agreement with our DFT calculations, implying a modest role of electronic correlations. Narrow M\" ossbauer spectral lines also indicate high crystallinity of the sample.

We report a broadband study of the charge dynamics in the van der Waals (vdW) magnetic materials 2H-$M_x$TaS$_2$ ($M$ = Mn and Co), which span the onset of both long-range antiferromagnetic (AFM) and ferromagnetic (FM) order, depending on the intercalation $M$ and its concentration $x$. We discover a spectral weight ($SW$) shift from high to low energy scales for FM compositions, while reversely $SW$ is removed from low towards high spectral energies for AFM compounds. This maps the related reconstruction of the electronic band structure along the crossover from the FM to AFM order, which restores an occupation balance in the density of states between spin majority and minority bands of the intercalated 3$d$ elements., Comment: 5 pages, 2 Figures, Supplementary Material provided by the Journal

We report a thermal transport study of IrSbSe, which crystallizes in a noncentrosymmetric cubic structure with the $P2_13$ space group and shows a narrow-gap semiconducting behavior. The large discrepancy between the activation energy for conductivity [$E_\rho$ = 128(2) meV] and for thermopower [$E_S$ = 17.7(9) meV] from 200 to 300 K indicates the polaronic transport mechanism. Electrical resistivity varies as $exp(T_0/T)^{1/4}$ and thermopower varies as $T^{1/2}$ at low temperatures, indicating that it evolves into the Mott's variable-range hopping dominant conduction with decreasing temperature. IrSbSe shows relatively low value of thermal conductivity ($\sim$ 1.65 W/K$\cdot$m) and thermopower of about 0.24 mV/K around 100 K, yet poor electrical conductivity. On the other hand, high vacancy defect concentration on both Ir and Sb atomic sites of up to 15\%, suggests high defect tolerance and points to possibility of future improvement of carrier density by chemical substitution or defect optimization.

Visualizing atomic-orbital degrees of freedom is a frontier challenge in scanned microscopy. Some types of orbital order are virtually imperceptible to normal scattering techniques because they do not reduce the overall crystal lattice symmetry. A good example is dxz/dyz ({\pi},{\pi}) orbital order in tetragonal lattices. For enhanced detectability, here we consider the quasiparticle scattering interference (QPI) signature of such ({\pi},{\pi}) orbital order in both normal and superconducting phases. The theory reveals that sublattice-specific QPI signatures generated by the orbital order should emerge strongly in the superconducting phase. Sublattice-resolved QPI visualization in superconducting CeCoIn5 then reveals two orthogonal QPI patterns at lattice-substitutional impurity atoms. We analyze the energy dependence of these two orthogonal QPI patterns and find the intensity peaked near E=0, as predicted when such ({\pi}) orbital order is inte,{\pi}rtwined with d-wave superconductivity. Sublattice-resolved superconductive QPI techniques thus represent a new approach for study of hidden orbital order., Comment: 19 pages, 5 figures

Charge density waves (CDWs) with superconductivity, competing Fermi surface instabilities and collective orders, have captured much interest in two-dimensional van der Waals (vdW) materials. Understanding of CDW suppression mechanism, its connection to emerging superconducting state and electronic correlations provides opportunities for engineering the electronic properties of vdW heterostructures and thin film devices. Using combination of the thermal transport, X-ray photoemission spectroscopy, Raman measurements, and first-principle calculations, we observe an increase in electronic correlations of the conducting states as CDW is suppressed in ZrTe$_3$ with 5\% Cu and Ni intercalation in the vdW gap. As superconductivity emerges, intercalation brings decoupling of quasi-one-dimensional conduction electrons with phonons as a consequence of intercalation-induced lattice expansion but also a drastic increase in Zr$^{2+}$ at the expense of Zr$^{4+}$ metal atoms. These observation demonstrate the potential of atomic intercalates in vdW gap for ground state tuning but also illustrate the crucial role of Zr metal valence in formation of collective electronic orders.

Among several well-known transition metal-based compounds, the van der Waals (vdW) Fe3-xGeTe2 (FGT) magnet is a strong candidate for use in two-dimensional (2D) magnetic devices due to its strong perpendicular magnetic anisotropy, sizeable Curie temperature (TC ~ 154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the TC remains far too low for practical applications, there has been a successful push toward improving it via external driving forces such as pressure, irradiation, and doping. Here we present experimental evidence of a novel room-temperature (RT) ferromagnetic phase induced by the electrochemical intercalation of common tetrabutylammonium cations (TBA+) into FGT bulk crystals. We obtained Curie temperatures as high as 350 K with chemical and physical stability of the intercalated compound. The temperature-dependent Raman measurements in combination with vdW-corrected ab initio calculations suggest that charge transfer (electron doping) upon intercalation could lead to the observation of RT ferromagnetism. This work demonstrates that molecular intercalation is a viable route in realizing high-temperature vdW magnets in an inexpensive and reliable manner.

Low-temperature (down to $\sim$ 50 mK) thermal conductivity measurements with the heat flow direction along the inter-plane tetragonal $c$-axis, $\kappa_c$, were used to study the superconducting state of heavy fermion CeIrIn$_5$. Measurements were performed in the magnetic fields both parallel to the heat flow direction, $H\parallel c$, and transverse to it, $H \parallel a$. Inter-plane heat conductivity in $H \parallel c$ configuration shows negligible initial increase with magnetic field and a rapid rise on approaching $H_{c2}$ from below, similar to the expectations for the superconducting gap without line nodes. This observation is in stark contrast to monotonic increase found in the previous in-plane heat transport measurements. In the configuration with the magnetic field breaking the tetragonal symmetry of the lattice, $H \parallel a$, $\kappa_c$ reveals non-monotonic evolution with temperature and magnetic field suggesting sub-phase boundary in the superconducting state. The characteristic temperature $T_{kink} \sim$ 0.07~K of the sub-boundary is well within the domain of bulk superconductivity $T_c \sim$ 0.4~K and $H_{c2}\sim$ 1.0~T. These results are consistent with a superconducting gap with an equatorial line node and polar point nodes, a gap symmetry of the D$_{4h}$ point group, for which magnetic field along the tetragonal plane breaks the degeneracy of the multi-component order parameter and induces a phase transition with nodal topology change., Comment: 11 pages, 7 figures

Perfect $T$-linear resistivity associated with universal scattering rate: $1/\tau =\alpha k_B T/\hbar$ with $\alpha \sim 1$, so-called Planckian metal state, has been observed in the normal state of a variety of strongly correlated superconductors close to a quantum critical point. However, the microscopic origin of this intriguing phenomena and its link to quantum criticality still remains an outstanding open problem. In this work, we observe the quantum-critical $T/B$-scaling of the Planckian metal state in the resistivity and heat capacity of heavy-electron superconductor Ce$_{1-x}$Nd$_x$CoIn$_5$ in magnetic fields near the edge of antiferromagnetism, driven by critical Kondo hybridization at the critical doping $x_c \sim 0.03$. We further provide the first microscopic mechanism to account for the Planckian state in a quantum critical system based on the critical charge fluctuations near Kondo breakdown transition at $x_c$ within the quasi-two-dimensional Kondo-Heisenberg lattice model. This mechanism simultaneously captures the observed universal Planckian scattering rate as well as the quantum-critical scaling and power-law divergence in thermodynamic observables near criticality. Our mechanism is generic to Planckian metal states in a variety of quantum critical superconductors near Kondo destruction., Comment: 14 pages, 7 figure, 1 table

Intrinsic, two-dimensional (2D) ferromagnetic semiconductors are an important class of materials for spin-charge conversion applications. Cr$_2$Ge$_2$Te$_6$ retains long-range magnetic order in bilayer at cryogenic temperatures and shows complex magnetic interactions with considerable magnetic anisotropy. Here, we performed a series of structural, magnetic, X-ray scattering, electronic, thermal transport and first-principles calculation studies which reveal that localized electronic charge carriers in Cr$_2$Ge$_2$Te$_6$ are dressed by surrounding lattice and are involved in polaronic transport via hopping that is sensitive on details of magnetocrystalline anisotropy. This opens possibility for manipulation of charge transport in Cr$_2$Ge$_2$Te$_6$ - based devices by electron-phonon- and spin-orbit coupling-based tailoring of polaron properties.

Two-dimensional transition metal trichalcogenides (TMTC's) feature covalently bonded metal-chalcogen layers separated by the van der Waals (vdW) gap. Similar to transition metal dichalcogenides (TMDCs), TMTCs often host charge density waves (CDWs) and superconductivity but unlike TMDCs atomic chains in the crystal structure give rise to quasi one-dimensional (quasi 1D) conduction. ZrTe$_3$ features CDW below $T_{\textrm{CDW}}$ = 63 K and filamentary superconductivity below 2 K that can be enhanced by pressure or chemical substitution. Here we report the presence of mixed valent Zr$^{2+}$ and Zr$^{4+}$ atoms in ZrTe$_3$ crystals that is reduced by doping in ZrTe$_{3-x}$Se$_x$ and Zr$_{1-y}$Hf$_y$Te$_3$. Superconductivity is enhanced via disorder in Te2-Te3 atomic chains that are associated with CDW formation. Hf substitution on Zr atomic site enhances $T_{\textrm{CDW}}$ due to unperturbed Te2-Te3 chain periodicity and enhanced electron-phonon coupling. Weak electronic correlations in ZrTe$_{3-x}$Se$_x$ are likely governed by the lattice contraction effects.

We report thermoelectric studies of FeS$_{1-x}$Se$_x$ ($x$ = 0, 0.06) superconducting single crystals that feature high irreversibility fields and critical current density $J_c$ comparable to materials with much higher superconducting critical temperatures ($T_c$'s). The ratio of $T_c$ to the Fermi temperature $T_F$ is very small indicating weak electronic correlations. With a slight selenium substitution on sulfur site in FeS both $T_c$/$T_F$ and the effective mass $m^*$ rise considerably, implying increase in electronic correlation of the bulk conducting states. The first-principle calculations show rise of the density of states at the Fermi level in FeS$_{0.94}$Se$_{0.06}$ when compared to FeS which is related not only to Fe but also to chalcogen-derived electronic states.

We report a detailed study of electrical and thermal transport properties in 2H-M$_x$TaS$_2$ (M = Mn, Co) magnets where M atoms are intercalated in the van der Waals gap. The intercalation induces ferromagentism with an easy-plane anisotropy in 2H-Mn$_x$TaS$_2$, but ferromagnetism with a strong uniaxial anisotropy in 2H-Co$_{0.22}$TaS$_2$, which finally evolves into a three-dimensional antiferromagnetism in 2H-Co$_{0.34}$TaS$_2$. Temperature-dependent electrical resistivity shows metallic behavior for all samples. Thermopower is negative in the whole temperature range for 2H-Co$_x$TaS$_2$, whereas the sign changes from negative to positive with increasing Mn for 2H-Mn$_x$TaS$_2$. The diffusive thermoelectric response dominates in both high- and low-temperature ranges for all samples. A clear kink in electrical resistivity, a weak anomaly in thermal conductivity, as well as a slope change in thermopower were observed at the magnetic transitions for 2H-Mn$_{0.28}$TaS$_2$ ($T_\textrm{c}$ $\approx$ 82 K) and 2H-Co$_{0.34}$TaS$_2$ ($T_\textrm{N}$ $\approx$ 36 K), respectively, albeit weaker for lower $x$ crystals. Co-intercalation promoted ferromagnetic to antiferromagnetic transition is further confirmed by the Hall resistivity; the sign change of the ordinary Hall coefficient indicates a multi-band behavior in 2H-Co$_x$TaS$_2$.

A Raman scattering study covering the entire substitution range of the FeSe$_{1-x}$S$_x$ solid solution is presented. Data were taken as a function of sulfur concentration $x$ for $0\le x \le 1$, of temperature and of scattering symmetry. All type of excitations including phonons, spins and charges are analyzed in detail. It is observed that the energy and width of iron-related B$_{1g}$ phonon mode vary continuously across the entire range of sulfur substitution. The A$_{1g}$ chalcogenide mode disappears above $x=0.23$ and reappears at a much higher energy for $x=0.69$. In a similar way the spectral features appearing at finite doping in A$_{1g}$ symmetry vary discontinuously. The magnetic excitation centered at approximately 500 cm$^{-1}$ disappears above $x=0.23$ where the A$_{1g}$ lattice excitations exhibit a discontinuous change in energy. The low-energy mode associated with fluctuations displays maximal intensity at the nemato-structural transition and thus tracks the phase boundary.

We carried out a comprehensive study of the structural, electrical transport, thermal and thermodynamic properties in ferrimagnetic Mn$_3$Si$_2$Te$_6$ single crystals. Mn and Te $K$-edge X-ray absorption spectroscopy and synchrotron powder X-ray diffraction were measured to provide information on the local atomic environment and the average crystal structure. The dc and ac magnetic susceptibility measurements indicate a second-order paramagnetic to ferrimagnetic transition at $T_c$ $\sim$ 74 K, which is further confirmed by the specific heat measurement. Mn$_3$Si$_2$Te$_6$ exhibits semiconducting behavior along with a large negative magnetoresistance of -87\% at $T_c$ and relatively high value of thermopower up to $\sim$ 10 mV/K at 5 K. Besides the rapidly increasing resistivity $\rho(T)$ and thermopower $S(T)$ below 20 K, the large discrepancy between activation energy for resistivity $E_\rho$ and thermopower $E_S$ above 20 K indicates the polaronic transport mechanism. Furthermore, the thermal conductivity $\kappa(T)$ of Mn$_3$Si$_2$Te$_6$ is notably rather low, comparable to Cr$_2$Si$_2$Te$_6$, and is strongly suppressed in magnetic field across $T_c$, indicating the presence of strong spin-lattice coupling, also similar with Cr$_2$Si$_2$Te$_6$.

Van der Waals (vdW) ferromagnets are an important class of materials for spintronics applications. The recent discovery of atomically vdW magnets CrI$_3$ and Cr$_2$Ge$_2$Te$_6$ has triggered a renaissance in the area of two-dimensional (2D) magnetism. Herein we systematically studied 2H-Mn$_{0.28}$TaS$_2$ single crystal, a 2D vdW ferromagnet with $T_c$ $\sim$ 82.3 K and a large in-plane magnetic anisotropy. Mn $K$-edge x-ray absorption spectroscopy was measured to provide information on its electronic state and local atomic environment. The detailed magnetic isotherms measured in the vicinity of $T_c$ indicates that the spin coupling inside 2H-Mn$_{0.28}$TaS$_2$ is of a three-dimensional (3D) Heisenberg-type coupled with the attractive long-range interaction between spins that decay as $J(r)\approx r^{-4.85}$. Both resistivity $\rho(T)$ and thermopower $S(T)$ exhibit anomalies near $T_c$, confirming that the hole-type transport carriers strongly interact with local moments. An unusual angle-dependent magnetoresistance is further observed, suggesting a possible field-induced novel magnetic structure.

We report ferromagnetism in 2H-Co$_{0.22}$TaS$_2$ single crystals where Co atoms are intercalated in the van der Waals gap, and a systematic study of its magnetic critical behavior in the vicinity of $T_c \sim 28$ K. The obtained critical exponents $\beta$ = 0.43(2), $\gamma$ = 1.15(1), and $\delta = 3.54(1)$ fulfill the Widom scaling relation $\delta = 1+\gamma/\beta$ and follow the scaling equation. This indicates that the spin coupling in 2H-Co$_{0.22}$TaS$_2$ is of three-dimensional Hersenberg type coupled with long-range magnetic interaction, and that the exchange interaction decays with distance as $J(r)\approx r^{-4.69}$. 2H-Co$_{0.22}$TaS$_2$ exhibits a weak temperature-dependent metallic behavior in resistivity and negative values of thermopower with dominant electron-type carriers, in which obvious anomalies were observed below $T_c$ as well as the anomalous Hall effect (AHE). The linear scaling behavior between the modified anomalous Hall resistivity $\rho_{xy}/\mu_0H$ and longitudinal resistivity $\rho_{xx}^2M/\mu_0H$ implies that the origin of AHE in 2H-Co$_{0.22}$TaS$_2$ should be dominated by the extrinsic side-jump mechanism., Comment: arXiv admin note: text overlap with arXiv:2110.10908

We study the evolution of temperature-dependent resistivity with controlled point-like disorder induced by 2.5 MeV electron irradiation in stoichiometric compositions of the "3-4-13" stannides, $(\text{Ca,Sr})_{3}(\text{Ir,Rh})_{4}\text{Sn}_{13}$.Three of these cubic compounds exhibit a microscopic coexistence of charge-density wave (CDW) order and superconductivity (SC), while $\text{Ca}_{3}\text{Rh}_{4}\text{Sn}_{13}$ does not develop CDW order. As expected, the CDW transition temperature, $T_{\text{CDW}}$, is universally suppressed by irradiation in all three compositions. The superconducting transition temperature, $T_{c}$, behaves in a more complex manner. In $\text{Sr}_{3}\text{Rh}_{4}\text{Sn}_{13}$, it increases initially in a way consistent with a direct competition of CDW and SC, but quickly saturates at higher irradiation doses. In the other three compounds, $T_{c}$ is monotonically suppressed by irradiation. The strongest suppression is found in $\text{Ca}_{3}\text{Rh}_{4}\text{Sn}_{13}$, which does not have CDW order. We further examine this composition by measuring the London penetration depth, $\lambda(T)$, from which we derive the superfluid density. The result unambiguously points to a weak-coupling, full single gap, isotropic superconducting state. Therefore, we must explain two seemingly incompatible experimental observations: a single isotropic superconducting gap and a significant suppression of $T_{c}$ by non-magnetic disorder. We conduct a quantitative theoretical analysis based on a generalized Anderson theorem which points to an unconventional multiband $s^{+-}$-pairing state where the sign of the order parameter is different on one (or a small subset) of the smaller Fermi surface sheets, but remains overall fully-gapped.

We examine the magnetic properties of the quasi 2D ferrimagnetic single crystal Mn3Si2Te6 (MST) through critical phenomena and magnetic entropy analysis in the easy axis (H || ab) as a function of proton irradiance. Employing a modified asymptotic analysis method, we find that upon proton irradiation the critical exponents do not fall into any particular universality class but lie close to mean field critical exponents ({\gamma} = 1, \b{eta} = 0.5). The presence of long-range interactions can be safely assumed for the pristine and irradiated cases of MST examined in this work. Further analysis on the effective spatial dimensionality reveal that MST remains at d = 3 under proton irradiation transitioning from an n = 1 spin dimensionality to n = 2 and n=3 for 1 x 10^15 and 5 x 10^15 H+/cm^2, indicating an XY interaction and a Heisenberg interaction, respectively. The pair (spin-spin) correlation function reveals an increase in magnetic correlations at the proton irradiance of 5 x 10^15 H+/cm^2. In conjunction, the maximum change in magnetic entropy obtained from isothermal magnetization at 3 T is the largest for 5 x 10^15 H+/cm^2 with a value of 2.45 J/kgK at T = 73.66 K, in comparison to 1.60 J/kgK for pristine MST at T = 73 K. Magnetic entropy derived from zero-field heat capacity does not show large deviations across the proton irradiated samples. This suggests that the antiferromagnetic coupling between the Mn sites is stable even after proton irradiation. Such result implies that magnetization is enhanced through a strengthening of the super-exchange interaction between Mn atoms mediated through Te rather than a weakening of the AFM component. Overall, our study finds that the magnetic interactions are manipulated the greatest when MST is irradiated at 5 x 10^15 H+/cm^2.

We present a polarization-resolved, high-resolution Raman scattering study of the three consecutive charge density wave (CDW) regimes in $1T$-TaS$_2$ single crystals, supported by \textit{ab initio} calculations. Our analysis of the spectra within the low-temperature commensurate (C-CDW) regime shows $\mathrm{P3}$ symmetry of the system, thus excluding the previously proposed triclinic stacking of the "star-of-David" structure, and promoting trigonal or hexagonal stacking instead. The spectra of the high-temperature incommensurate (IC-CDW) phase directly project the phonon density of states due to the breaking of the translational invariance, supplemented by sizeable electron-phonon coupling. Between 200 and 352\,K, our Raman spectra show contributions from both the IC-CDW and the C-CDW phase, indicating their coexistence in the so-called nearly-commensurate (NC-CDW) phase. The temperature-dependence of the symmetry-resolved Raman conductivity indicates the stepwise reduction of the density of states in the CDW phases, followed by a Mott transition within the C-CDW phase. We determine the size of the Mott gap to be $\Omega_{\rm gap}\approx 170-190$ meV, and track its temperature dependence.

We carried out a comprehensive study of electronic transport, thermal and thermodynamic properties in FeCr$_2$Te$_4$ single crystals. It exhibits bad-metallic behavior and anomalous Hall effect (AHE) below a weak-itinerant paramagentic-to-ferrimagnetic transition $T_c$ $\sim$ 123 K. The linear scaling between the anomalous Hall resistivity $\rho_{xy}$ and the longitudinal resistivity $\rho_{xx}$ implies that the AHE in FeCr$_2$Te$_4$ is most likely dominated by extrinsic skew-scattering mechanism rather than intrinsic KL or extrinsic side-jump mechanism, which is supported by our Berry phase calculations., Comment: arXiv admin note: text overlap with arXiv:1811.07015

We report quantum oscillation measurements of LaAlGe, a Lorentz-violating type-II Weyl semimetal with tilted Weyl cones. Very small quasiparticle masses and very high Fermi velocities were detected at the Fermi surface. Whereas three main frequencies have been observed, angular dependence of two Fermi surface sheets indicates possible two-dimensional (2D) character despite the absence of the 2D structural features such as van der Waals bonds. Such conducting states may offer a good platform for low-dimensional polarized spin current in magnetic RAlGe (R = Ce, Pr) materials., Comment: 5 pages, 3 figures

We report discovery of new antiferromagnetic semimetal EuZnSb$_2$, obtained and studied in the form of single crystals. Electric resistivity, magnetic susceptibility and heat capacity indicate antiferromagnetic order of Eu with $T_N$ = 20 K. The effective moment of Eu$^{2+}$ inferred from the magnetization and specific heat measurement is 3.5 $\mu_B$, smaller than the theoretical value of Eu$^{2+}$ due to presence of both Eu$^{3+}$ and Eu$^{2+}$. Magnetic field-dependent resistivity measurements suggest dominant quasi two dimensional Fermi surfaces whereas the first-principle calculations point to the presence of Dirac fermions. Therefore, EuZnSb$_2$ could represent the first platform to study the interplay of dynamical charge fluctuations, localized magnetic 4$f$ moments and Dirac states with Sb orbital character., Comment: 9 pages, 4 figures

We report giant thermopower S = 2.5 mV/K in CoSbS single crystals, a material that shows strong high-temperature thermoelectric performance when doped with Ni or Se. Changes of low temperature thermopower induced by magnetic field point to mechanism of electronic diffusion of carriers in the heavy valence band. Intrinsic magnetic susceptibility is consistent with the Kondo- Insulator-like accumulation of electronic states around the gap edges. This suggests that giant thermopower stems from temperature-dependent renormalization of the non-interacting bands and buildup of the electronic correlations on cooling., Comment: 6 pages, 4 figures

We report Fermi surface characteristics of Mo8Ga41, a two-gap superconductor with critical temperature Tc = 10 K, obtained from quantum oscillation measurements. Four major frequencies have been observed with relatively small quasiparticle masses. Angular dependence of major frequencies indicates three-dimensional Fermi surface sheets. This argues for a relatively isotropic superconducting state and, given its relatively high Tc, shows that a search for materials in this class could be of interest for superconducting wire applications., Comment: 4 pages, 3 figures

Ferromagnetic van der Waals (vdW) insulators are of great scientific interest for their promising applications in spintronics. It has been indicated that in the two materials within this class, CrI$_3$ and VI$_3$, the magnetic ground state, the band gap, and the Fermi level could be manipulated by varying the layer thickness, strain or doping. To understand how these factors impact the properties, a detailed understanding of the electronic structure would be required. However, the experimental studies of the electronic structure of these materials are still very sparse. Here, we present the detailed electronic structure of CrI$_3$ and VI$_3$ measured by angle-resolved photoemission spectroscopy (ARPES). Our results show a band-gap of the order of 1 eV, sharply contrasting some theoretical predictions such as Dirac half-metallicity and metallic phases, indicating that the intra-atomic interaction parameter (U) and spin-orbit coupling (SOC) were not properly accounted for in the calculations. We also find significant differences in the electronic properties of these two materials, in spite of similarities in their crystal structure. In CrI$_3$, the valence band maximum is dominated by the I 5{\it p}, whereas in VI$_3$ it is dominated by the V 3{\it d} derived states. Our results represent valuable input for further improvements in the theoretical modeling of these systems., Comment: 8 pages, 4 figures

The contribution of bulk and surface to the electrical resistance along crystallographic \textit{b}- and \textit{c}-axes as a function of crystal thickness gives evidence for a temperature independent surface states in an antiferromagnetic narrow-gap semiconductor CrSb$_{2}$. ARPES shows a clear electron-like pocket at $\Gamma$-$Z$ direction which is absent in the bulk band structure. First-principles calculations also confirm the existence of metallic surface states inside the bulk gap. Whereas combined experimental probes point to enhanced surface conduction similar to topological insulators, surface states are trivial since CrSb$_2$ exhibits no band inversion.

We report anisotropic magnetocaloric effect and critical behavior in quasi-one-dimensional ferromagnetic CrSbSe$_3$ single crystal. The maximum magnetic entropy change $-\Delta S_M^{max}$ is 2.16 J kg$^{-1}$ K$^{-1}$ for easy $a$ axis (2.03 J kg$^{-1}$ K$^{-1}$ for hard $b$ axis) and the relative cooling power $RCP$ is 163.1 J kg$^{-1}$ for easy $a$ axis (142.1 J kg$^{-1}$ for hard $b$ axis) near $T_c$ with a magnetic field change of 50 kOe. The magnetocrystalline anisotropy constant $K_u$ is estimated to be 148.5 kJ m$^{-3}$ at 10 K, decreasing to 39.4 kJ m$^{-3}$ at 70 K. The rescaled $\Delta S_M(T,H)$ curves along all three axes collapse onto a universal curve, respectively, confirming the second order ferromagnetic transition. Further critical behavior analysis around $T_c \sim$ 70 K gives that the critical exponents $\beta$ = 0.26(1), $\gamma$ = 1.32(2), and $\delta$ = 6.17(9) for $H\parallel a$, while $\beta$ = 0.28(2), $\gamma$ = 1.02(1), and $\delta$ = 4.14(16) for $H\parallel b$. The determined critical exponents suggest that the anisotropic magnetic coupling in CrSbSe$_3$ is strongly dependent on orientations of the applied magnetic field., Comment: arXiv admin note: text overlap with arXiv:2007.07159

We carried out a comprehensive study of magnetic critical behavior in single crystals of ternary chalcogenide FeCr$_2$Te$_4$ that undergoes a ferrimagnetic transition below $T_c$ $\sim$ 123 K. Detailed critical behavior analysis and scaled magnetic entropy change indicate a second-order ferrimagentic transition. Critical exponents $\beta = 0.30(1)$ with $T_c = 122.4(5)$ K, $\gamma = 1.22(1)$ with $T_c = 122.8(1)$ K, and $\delta = 4.24(2)$ at $T_c$ $\sim$ 123 K suggest that the spins approach three-dimensional Ising ($\beta$ = 0.325, $\gamma$ = 1.24, and $\delta$ = 4.82) model coupled with the attractive long-range interactions between spins that decay as $J(r)\approx r^{-4.88}$. Our results suggest that the ferrimagnetism in FeCr$_2$Te$_4$ is due to itinerant ferromagnetism among the antiferromagnetically coupled Cr-Fe-Cr trimers., Comment: Accepted in PRB

Two-dimensional (2D) materials with intrinsic ferromagnetism provide unique opportunity to engineer new functionalities in nano-spintronics. One such material is CrI$_3$, showing long-range magnetic order in monolayer with the Curie temperature ($T_c$) of 45 K. Here we study detailed evolution of magnetic transition and magnetic critical properties in response to systematic reduction in crystal thickness down to 50 nm. Bulk $T_c$ of 61 K is gradually suppressed to 57 K, however, the satellite transition at $T^*$ = 45 K is observed layer-independent at fixed magnetic field of 1 kOe. The origin of $T^*$ is proposed to be a crossover from pinning to depinning of magnetic domain walls. The reduction of thickness facilitates a field-driven metamagnetic transition around 20 kOe with out-of-plane field, in contrast to the continuous changes with in-plane field. The critical analysis around $T_c$ elucidates the mean-field type interactions in microscale-thick CrI$_3$.

We present inelastic neutron scattering (INS) measurements of magnetic excitations in YbMnBi$_2$, which reveal features consistent with a direct coupling of magnetic excitations to Dirac fermions. In contrast with the large broadening of magnetic spectra observed in antiferromagnetic metals such as the iron pnictides, here the spin waves exhibit a small but resolvable intrinsic width, consistent with our theoretical analysis. The subtle manifestation of spin-fermion coupling is a consequence of the Dirac nature of the conduction electrons, including the vanishing density of states near the Dirac points. Accounting for the Dirac fermion dispersion specific to \ymb\ leads to particular signatures, such as the nearly wave-vector independent damping observed in the experiment., Comment: 8 pages, 11 figures including both main text and supplemental material

Van der Waals (vdWs) crystals have attracted a great deal of scientific attention due to their interesting physical properties and widespread practical applications. Among all, CrSiTe3 (CST) is a ferromagnetic semiconductor with the Curie temperature (TC) of ~32 K. In this letter, we study the magnetic properties of bulk CST single-crystal upon proton irradiation with the fluence of 1x1018 protons/cm2. Most significantly, we observed an enhancement (23%) in the saturation magnetization from 3.9 {\mu}B to 4.8 {\mu}B and is accompanied by an increase in the coercive field (465-542 Oe) upon proton irradiation. Temperature-dependent X-band electron paramagnetic resonance measurements show no additional magnetically active defects/vacancies that are generated upon proton irradiation. The findings from X-ray photoelectron spectroscopy and Raman measurements lead us to believe that modification in the spin-lattice coupling and introduction of disorder could cause enhancement in saturation magnetization. This work demonstrates that proton irradiation is a feasible method in modifying the magnetic properties of vdWs crystals, which represents a significant step forward in designing future spintronic and magneto-electronic applications., Comment: The results remain inconclusive

We present Raman spectroscopy measurements of the van der Waals bonded ferromagnet Fe$_{3-x}$GeTe$_2$, together with lattice dynamics. Four out of eight Raman active modes are observed and assigned, in agreement with numerical calculations. The energies and line-widths of the observed modes display an unconventional temperature dependence at about 150 K and 220 K, followed by the nonmonotonic evolution of the Raman continuum. Whereas the former can be related to the magnetic phase transition, the origin of the latter anomaly remains an open question.

We present a comprehensive study on anisotropic magnetocaloric porperties of the van der Waals weak-itinerant ferromagnet Fe$_{3-x}$GeTe$_2$ that features gate-tunable room-temperature ferromagnetism in few-layer device. Intrinsic magnetocrystalline anisotropy is observed to be temperature-dependent and most likely favors the long-range magnetic order in thin Fe$_{3-x}$GeTe$_2$ crsytal. The magnetic entropy change $-\Delta S_M$ also reveals an anisotropic characteristic between $H // ab$ and $H // c$, which could be well scaled into a universal curve. The peak value $-\Delta S_M^{max}$ of 1.20 J kg$^{-1}$ K$^{-1}$ and the corresponding adiabatic temperature change $\Delta T_{ad}$ of 0.66 K are deduced from heat capacity with out-of-plane field change of 5 T. By fitting of the field-dependent parameters of $-\Delta S_M^{max}$ and the relative cooling power RCP, it gives $-\Delta S_M^{max} \propto H^n$ with $n = 0.603(6)$ and $RCP \propto H^m$ with $m = 1.20(1)$ when $H // c$. Given the high and tunable $T_c$, Fe$_{3-x}$GeTe$_2$ crystals are of interest for fabricating the heterostructure-based spintronics device.

We present a comprehensive investigation on anisotropic magnetic and magnetocaloric properties of the quasi-two-dimensional weak itinerant ferromagnet trigonal Cr$_{0.62}$Te single crystals. Magnetic-anisotropy-induced satellite transition $T^*$ is observed at low fields applied parallel to the $ab$ plane below $T_c$. The $T^*$ is featured by an anomalous magnetization downturn, similar to that in structurally related CrI$_3$, and shows a monotonous shift towards lower temperature with increasing field. Magnetocrystalline anisotropy is also reflected in magnetic entropy change $\Delta S_M(T,H)$ and relative cooling power RCP. Given the high $T_c$, Cr$_{0.62}$Te crystals are materials of interest for nanofabrication in basic science and applied technology.

Layered van der Waals ferromagnets are promising candidates for designing new spintronic devices. Here we investigated the critical properties and magnetocaloric effect connected with ferromagnetic transition in layered van der Waals VI$_3$ single crystals. The critical exponents $\beta = 0.244(5)$ with a critical temperature $T_c = 50.10(2)$ K and $\gamma = 1.028(12)$ with $T_c = 49.97(5)$ K are obtained from the modified Arrott plot, whereas $\delta = 5.24(2)$ is obtained from a critical isotherm analysis at $T_c = 50$ K. The magnetic entropy change $-\Delta S_M(T,H)$ features a maximum at $T_c$, i.e., $-\Delta S_M^{max} \sim$ 2.64 (2.27) J kg$^{-1}$ K$^{-1}$ with out-of-plane (in-plane) field change of 5 T. This is consistent with $-\Delta S_M^{max}$ $\sim$ 2.80 J kg$^{-1}$ K$^{-1}$ deduced from heat capacity and the corresponding adiabatic temperature change $\Delta T_{ad}$ $\sim$ 0.96 K with out-of-plane field change of 5 T. The critical analysis suggests that the ferromagnetic phase transition in VI$_3$ is situated close to a three- to two-dimensional critical point. The rescaled $\Delta S_M(T,H)$ curves collapse onto a universal curve, confirming a second-order type of the magnetic transition and reliability of the obtained critical exponents.

Formation of electronic nematicity is a common thread of unconventional superconductors. In iron-based materials, the long-range nematic order is revealed by the orthorhombic lattice distortion, which importance is a highly controversial topic due the small magnitude of the distortion. Here, we study the local crystal structure of FeSe and its interaction with electronic degrees of freedom using ultrafast electron diffraction, x-ray pair distribution function analysis, and transmission electron microscopy and find a significant lattice response to local nematicity. The study demonstrates how local lattice distortions, which exist even at temperatures above the nematic phase transition, can be released by photoexcitation, leading to an enhancement of the crystalline order. The observed local atomic structures and their out-of-equilibrium behavior unravel a sophisticated coupling between the lattice and nematic order parameter in FeSe.

A detailed account of the local atomic structure and disorder at 5~K across the phase diagram of the high temperature superconductor K$_x$Fe$_{2-y}$Se$_{2-z}$S$_z$ $(0 \leq z \leq 2)$ is obtained from neutron total scattering and associated atomic pair distribution function (PDF) approaches. Various model independent and model dependent aspects of the analysis reveal a high level of structural complexity on the nanometer length-scale. Evidence is found for considerable disorder in the $c$-axis stacking of the FeSe$_{1-x}$S$_{x}$ slabs without observable signs of turbostratic character of the disorder. In contrast to the related FeCh (Ch = S, Se) type superconductors, substantial Fe-vacancies are present in K$_x$Fe$_{2-y}$Se$_{2-z}$S$_z$, deemed detrimental for superconductivity when ordered. Our study suggests that the distribution of vacancies significantly modifies the iron-chalcogen bond-length distribution, in agreement with observed evolution of the PDF signal. A crossover like transition is observed at a composition of $z\approx1$, from a predominantly vacancy-disordered state at the selenium end to a more vacancy-ordered (VO) phase closer to the sulfur end of the phase diagram. The S-content dependent measures of the local structure are found to exhibit distinct behavior on either side of this crossover, correlating well with the evolution of the superconducting state to that of a magnetic semiconductor towards the $z\approx2$ end. The behavior reinforces the idea of the intimate relationship of correlated Fe-vacancies order in the local structure and the emergent electronic properties., Comment: 15 pages, 11 figures

CeRhSi$_{3}$ is a superconductor under pressure coexisting with a weakly antiferromagnetic phase characterized by a Bragg peak at $\vec{q}_{0}$=($\sim$ 0.2, 0, 0.5) (N. Aso et al. J. Magn. Magn. Mater. 310, 602 (2007)). The compound is also a heavy fermion material with a large specific heat coefficient $\gamma$=110 mJ $\cdot$ mol$^{-1}$ $\cdot$ K$^{-2}$ and a high Kondo temperature of $T_{K}$=50 K indicative that CeRhSi$_{3}$ is in a strongly Kondo screened state. We apply high resolution neutron spectroscopy to investigate the magnetic fluctuations in the normal phase, at ambient pressures, and at low temperatures. We measure a commensurate dynamic response centered around the $\vec{Q}$=(0, 0, 2) position that gradually evolves to H$\sim$ 0.2 with decreasing temperature and/or energy transfers. The response is broadened both in momentum and energy and not reminiscent of sharp spin wave excitations found in insulating magnets where the electrons are localized. We parameterize the excitation spectrum and temperature dependence using a heuristic model utilizing the random phase approximation to couple relaxing Ce$^{3+}$ ground state Kramers doublets with a Kondo-like dynamic response. With a Ruderman-Kittel-Kasuya-Yosida (RKKY) exchange interaction within the $ab$ plane and an increasing single site susceptibility, we can qualitatively reproduce the neutron spectroscopic results in CeRhSi$_{3}$ and namely the trade-off between scattering at commensurate and incommensurate positions. We suggest that the antiferromagnetic phase in CeRhSi$_{3}$ is driven by weakly correlated relaxing localized Kramers doublets and that CeRhSi$_{3}$ at ambient pressures is on the border between a Rudderman-Kittel-Yosida antiferromagnetic state and a Kondo screened phase where static magnetism is predominately absent., Comment: (11 pages, 8 figures, to be published in Physical Review B)

We report pair distribution function measurements of the iron-based superconductor FeSe above and below the structural transition temperature. Structural analysis reveals a local orthorhombic distortion with a correlation length of about 4 nm at temperatures where an average tetragonal symmetry is observed. The analysis further demonstrates that the local distortion is larger than the distortion at temperatures where the average observed symmetry is orthorhombic. Our results suggest that the low-temperature macroscopic nematic state in FeSe forms from an imperfect ordering of orbital-degeneracy-lifted nematic fluctuations which persist up to at least 300 K., Comment: 6 pages, 4 figures

Superconductivity in the iron pnictides emerges from metallic parent compounds exhibiting intertwined stripe-type magnetic order and nematic order, with itinerant electrons suggested to be essential for both. Here we use X-ray and neutron scattering to show that a similar intertwined state is realized in semiconducting KFe$_{0.8}$Ag$_{1.2}$Te$_2$ (K$_5$Fe$_4$Ag$_6$Te$_{10}$) without itinerant electrons. We find Fe atoms in KFe$_{0.8}$Ag$_{1.2}$Te$_2$ form isolated $2\times2$ blocks, separated by nonmagnetic Ag atoms. Long-range magnetic order sets in below $T_{\rm N}\approx35$ K, with magnetic moments within the $2\times2$ Fe blocks ordering into the stripe-type configuration. A nematic order accompanies the magnetic transition, manifest as a structural distortion that breaks the fourfold rotational symmetry of the lattice. The nematic orders in KFe$_{0.8}$Ag$_{1.2}$Te$_2$ and iron pnictide parent compounds are similar in magnitude and how they relate to the magnetic order, indicating a common origin. Since KFe$_{0.8}$Ag$_{1.2}$Te$_2$ is a semiconductor without itinerant electrons, this indicates that local-moment magnetic interactions are integral to its magnetic and nematic orders, and such interactions may play a key role in iron-based superconductivity., Comment: supplemental material available upon request, to be published in PRL

Fundamental electronic principles underlying all transition metal compounds are the symmetry and filling of the $d$-electron orbitals and the influence of this filling on structural configurations and responses. Here we use a sensitive local structural technique, x-ray atomic pair distribution function analysis, to reveal the presence of fluctuating local-structural distortions at high temperature of one such compound, \cis . We show that this hitherto overlooked fluctuating symmetry lowering is electronic in origin and will significantly modify the energy-level spectrum and electronic and magnetic properties. The explanation is a local, fluctuating, orbital-degeneracy-lifted state. The natural extension of our result would be that this phenomenon is likely to be widespread amongst diverse classes of partially filled nominally degenerate d-electron systems, with potentially broad implications for our understanding of their properties., Comment: 10 pages 3 figures

Intrinsic, two-dimensional (2D) ferromagnetic semiconductors are an important class of materials for spintronics applications. Cr$_2$X$_2$Te$_6$ (X = Si and Ge) semiconductors show 2D Ising-like ferromagnetism, which is preserved in few-layer devices. The maximum magnetic entropy change associated with the critical properties around the ferromagnetic transition for Cr$_2$Si$_2$Te$_6$ $-\Delta S_M^{max} \sim$ 5.05 J kg$^{-1}$ K$^{-1}$ is much larger than $-\Delta S_M^{max} \sim$ 2.64 J kg$^{-1}$ K$^{-1}$ for Cr$_2$Ge$_2$Te$_6$ with an out-of-plane field change of 5 T. The rescaled $-\Delta S_M(T,H)$ curves collapse onto a universal curve independent of temperature and field for both materials. This indicates similar critical behavior and 2D Ising magnetism, confirming the magnetocrystalline anisotropy that could preserve the long-range ferromagnetism in few-layers of Cr$_2$X$_2$Te$_6$.

We report anomalous Hall effect (AHE) and transport properties of trigonal Cr$_5$Te$_8$ (tr-Cr$_5$Te$_8$) single crystals. The electrical resistivity as well as the Seebeck coefficient shows a clear kink at the paramagnetic-ferromagnetic transition of tr-Cr$_5$Te$_8$, which is also confirmed by the heat capacity measurement. The scaling behavior between anomalous Hall resistivity $\rho^A_{xy}$ and longitudinal resistivity $\rho_{xx}$ is linear below $T_c$. Further analysis suggests that the AHE in tr-Cr$_5$Te$_8$ is dominated by the skew-scattering mechanism rather than the intrinsic or extrinsic side-jump mechanism.