Altermagnets are a class of materials with compensated magnetic moments, in which spin sublattices are related by specific rotational symmetries other than inversion or translation. This allows time-reversal symmetry to be broken without a net magnetization. Cr-doped FeSb2 has been theoretically proposed as a candidate d-wave altermagnetic system, yet its magnetic ground state has remained unresolved. Here, we synthesize single crystals of Fe1-xCrxSb2 and investigate their electrical transport and magnetic properties, with a focus on Fe0.85Cr0.15Sb2. Magnetization measurements suggest spin-compensated ordering below 3.5 K, where magnetic moments align along the crystallographic b-direction. Transport measurements reveal a crossover from large positive to negative magnetoresistance, while an anomalous Hall response emerges below 5 K, indicating time-reversal symmetry breaking. Muon spin relaxation measurements confirm that the magnetic ordering below 3.5 K is bulk in nature. The absence of coherent oscillations in zero-field μSR spectra and of magnetic Bragg intensity in single-crystal neutron diffraction establishes that the magnetically ordered state is short-range or disordered, rather than collinear altermagnetic order. These results demonstrate that Cr-doping alone breaks time-reversal symmetry without stabilizing long-range altermagnetic order in FeSb2.
Altermagnets break a combination of time-reversal and rotational symmetries without generating a net magnetization. As such, the order parameter of d-wave altermagnets has the same symmetry as magnetic multipoles, and couples to the product of a magnetic field and uniaxial strain. We combine elastocaloric experiments, free-energy modeling, and first-principles calculations on MnF_2 to establish a thermodynamic probe of the predicted finite-temperature altermagnetic critical point. These results pave the way to explore altermagnetic quantum criticality in d-wave materials and beyond.
Uniaxial stress is a promising method to tune magnetic frustration, allowing its effects to be studied in a precise way. In this work, uniaxial stress is applied to the triangular-lattice antiferromagnet PdCrO2. The Cr-Cr magnetic interaction is very sensitive to interatomic separation, so laboratory-achievable stress can induce substantial changes in magnetic structure. Results from three types of measurement are presented: x-ray diffraction, the stress-strain relationship, and neutron diffraction. The combined data show that the elastic moduli of PdCrO2are strongly affected by stress-induced changes in magnetic structure. A new, first-order stress-induced magnetic transition is observed, at which the lattice constant shrinks by 0.21%. The lattice stiffens dramatically across this transition: the Young's modulus increases by≈80GPa, and the Poisson ratio falls from≈1to≈0.4. This stiffening indicates that the magnetic order 'locks,' that is, becomes insensitive to lattice strain. This locking might occur because the new stress-induced magnetic order nests the Fermi surface of the Pd sheets. Other frustrated magnets, including candidate spin liquids, may show similarly strong coupling between magnetic and elastic degrees of freedom.
Similar to transitions in a range of correlated quantum materials, the valence transition exhibits a strong coupling to the crystal lattice, rendering it highly sensitive to stress tuning. In the present work, we determine the effect of uniaxial stress, which breaks the lattice symmetry, on the valence transition temperature and its crossover temperature in pure and Ag-substituted YbInCu 4 . Our key result is that hydrostatic stress is more effective in tuning this transition than uniaxial stress. Based on a symmetry decomposition of the stress-induced strains, we argue that this observation can be quantitatively understood, given that the valence transition is mostly sensitive to symmetric strains and thus volume changes of the lattice. These results support the notion that the valence transition can give rise to critical elasticity close to its critical endpoint.
Geometric frustration is a key ingredient in the emergence of exotic states of matter, such as the quantum spin liquid in Mott insulators. Although there has been intense interest in experimentally tuning frustration in candidate materials, achieving precise and continuous control has remained a major hurdle—particularly in accessing the properties of the ideally frustrated lattice. Here, we show that large, finely controlled anisotropic strains can effectively tune the degree of geometric frustration in the Mott insulating κ ‐ ( ET ) 2 Cu 2 ( CN ) 3 —a slightly anisotropic triangular-lattice quantum magnet. Using thermodynamic measurements of the elastocaloric effect, we experimentally map out a temperature-strain phase diagram that captures both the ground state of the isotropic lattice and the less frustrated parent state. Our results provide a benchmark for calculations of the triangular-lattice Hubbard model as a function of frustration and highlight the power of lattice engineering as a route to realizing perfectly frustrated quantum materials.
Similar to transitions in a range of correlated quantum materials, the valence transition exhibits a strong coupling to the crystal lattice, rendering it highly sensitive to stress tuning. In the present work, we determine the effect of uniaxial stress, which breaks the lattice symmetry, on the valence transition temperature and its crossover temperature in pure and Ag-substituted YbInCu4. Our key result is that hydrostatic stress is more effective in tuning this transition than uniaxial stress. Based on a symmetry decomposition of the stress-induced strains, we argue that this observation can be quantitatively understood, given that the valence transition is mostly sensitive to symmetric strains and thus volume changes of the lattice. These results support the notion that the valence transition can give rise to critical elasticity close to its critical endpoint.
Similar to transitions in a range of correlated quantum materials, the valence transition exhibits a strong coupling to the crystal lattice, rendering it highly sensitive to stress tuning. In the present work, we determine the effect of uniaxial stress, which breaks the lattice symmetry, on the valence transition temperature and its crossover temperature in pure and Ag-substituted YbInCu_4. Our key result is that hydrostatic stress is more effective in tuning this transition than uniaxial stress. Based on a symmetry decomposition of the stress-induced strains, we argue that this observation can be quantitatively understood, given that the valence transition is mostly sensitive to symmetric strains and thus volume changes of the lattice. These results support the notion that the valence transition can give rise to critical elasticity close to its critical endpoint.
Geometric frustration is a key ingredient in the emergence of exotic states of matter, such as the quantum spin liquid in Mott insulators. While there has been intense interest in experimentally tuning frustration in candidate materials, achieving precise and continuous control has remained a major hurdle – particularly in accessing the properties of the ideally frustrated lattice. Here, we show that large, finely controlled anisotropic strains can effectively tune the degree of geometric frustration in the Mott insulating κ-(ET)_2Cu_2(CN)_3 – a slightly anisotropic triangular-lattice quantum magnet. Using thermodynamic measurements of the elastocaloric effect, we experimentally map out a temperature-strain phase diagram that captures both the ground state of the isotropic lattice and the less frustrated parent state. Our results provide a new benchmark for calculations of the triangular-lattice Hubbard model as a function of frustration and highlight the power of lattice engineering as a route to realizing perfectly frustrated quantum materials.
Uniaxial stress has proven to be a powerful experimental tuning parameter for effectively controlling lattice, charge, orbital, and spin degrees of freedom in quantum materials. In addition, its ability to manipulate the symmetry of materials has garnered significant attention. Recent technical progress to combine uniaxial stress cells with quantum oscillation and angle-resolved photoemission techniques allowed to study the electronic structure as function of uniaxial stress. This review provides an overview on experimental advancements in methods and examines studies on diverse quantum materials, encompassing the semimetal WTe2, the unconventional superconductor Sr2RuO4, Fe-based superconductors, and topological materials.
Lattice strains of appropriate symmetry have served as an excellent tool to explore the interaction of superconductivity in the iron-based superconductors with orthorhombic-nematic and stripe spin-density-wave (SSDW) order. In this Letter, we contribute to a broader understanding of the coupling of strain to superconductivity and competing normal-state orders by studying CaKFe4As4 under large, in-plane strains of B1g and B2g symmetry. In contrast to the majority of iron-based superconductors, pure CaKFe4As4 exhibits superconductivity with a relatively high transition temperature of Tc∼35K in proximity of a noncollinear, tetragonal, hedgehog spin-vortex crystal (SVC) order. Through experiments and calculations, we demonstrate an anisotropic in-plane strain response of Tc and the favored SVC configuration in CaKFe4As4. This supports a scenario, in which the change in spin fluctuations dominates the strain response of superconducting Tc. Overall, by suggesting moderate B2g strains as an effective parameter to change the stability of SVC and SSDW, we outline a pathway to a unified phase diagram of iron-based superconductivity. Published by the American Physical Society 2024
We report on a new technique for measuring the dynamic Young's modulus, $E$, of quantum materials at low temperatures as a function of static tuning strain, $\epsilon$, in piezoactuator-driven pressure cells. In addition to a static tuning of stress and strain, we apply a small-amplitude, finite-frequency a.c. (1 Hz$ \lesssim \omega \lesssim $1000 Hz) uniaxial stress, $\sigma_{ac}$, to the sample and measure the resulting a.c. strain, $\epsilon_{ac}$, using a capacitive sensor to obtain the associated modulus $E$. We demonstrate the performance of the new technique through proof-of-principle experiments on the unconventional superconductor Sr$_2$RuO$_4$, which is known for its rich temperature-strain phase diagram. In particular, we show that the magnitude of $E$, measured using this a.c. technique at low frequencies, exhibits a pronounced nonlinear elasticity, which is in very good agreement with previous Young's modulus measurements on Sr$_2$RuO$_4$ under [100] strain using a d.c. method (Noad et al., Science 382, 447-450 (2023)). By combining the new a.c. Young's modulus measurements with a.c. elastocaloric measurements in a single measurement, we demonstrate that these a.c. techniques are powerful in detecting small anomalies in the elastic properties of quantum materials. Finally, using the case of Sr$_2$RuO$_4$ as an example, we demonstrate how the imaginary component of the modulus can provide additional information about the nature of ordered phases.
EuCd$_2$As$_2$ is an antiferromagnetic semimetal, that can host non-trivial topological properties, depending upon its magnetic state and excitations. Here, we report the synthesis and characterization of Eu(Cd$_{1-x}$Ag$_x$)$_2$As$_2$ and Eu$_{1-y}$Na$_y$Cd$_2$As$_2$, and study the evolution and nature of magnetic order with doping. Temperature-substitution phase diagrams are constructed from the electrical resistance and magnetic susceptibility data. We observe a splitting of the magnetic transition into two different transitions, and the gradual increase in one of the transition temperatures with Ag- and Na-substitution. The other transition remains more or less independent of doping. We further show that a magnetic state with a net ferromagnetic moment is stabilized by both Ag and Na doping and this can be explained by considering the changes in band filling due to substitution as suggested by density functional theory (DFT) calculations. We thus show that chemical substitution and the subsequent changes in band filling could be a pathway to tune the magnetic ground state and to stabilize a ferromagnetic phase in EuCd$_2$As$_2$.
YbPtBi is one of the heavy-fermion systems with largest Sommerfeld coefficient $\gamma$ and is thus classified as a `super'-heavy fermion material. In this work, we resolve the long-debated question about the hierarchy of relevant energy scales, such as crystal-electric field (CEF) levels, Kondo and magnetic ordering temperature, in YbPtBi. Through measurements of the a.c. elastocaloric effect and generic symmetry arguments, we identify an \textit{elastic level splitting} that is uniquely associated with the symmetry-allowed splitting of a quartet CEF level. This quartet, which we identify to be the first excited state at $\Delta/k_\text B\approx1.6\,\rm K$ above the doublet ground state at ambient pressure, is well below the Kondo temperature $T_\text K\approx10\,\rm K$. Thus, our analysis provides strong support for models that predict that the heavy electron mass is a result of an enhanced degeneracy of the CEF ground state, i.e., a quasi-sextet in YbPtBi. At the same time, our study shows the potential of the a.c. elastocaloric effect to control and quantify strain-induced changes of the CEF schemes, opening a different route to disentangle the CEF energy scales from other relevant energy scales in correlated quantum materials.
YbPtBi is one of the heavy-fermion systems with largest Sommerfeld coefficient γ and is thus classified as a ‘super’-heavy fermion material. In this work, we resolve the long-debated question about the hierarchy of relevant energy scales, such as crystal-electric field (CEF) levels, Kondo and magnetic ordering temperature, in YbPtBi. Through measurements of the a.c. elastocaloric effect and generic symmetry arguments, we identify an elastic level splitting that is unambiguously associated with the symmetry-allowed splitting of a quartet CEF level. This quartet, which we identify to be the first excited state at Δ/kB ≈ 1.6 K above the doublet ground state at ambient pressure, is well below the proposed Kondo temperature TK ≈ 10 K. Consequently, this analysis of the energy scheme can provide support models that predict that the heavy electron mass is a result of an enhanced degeneracy of the CEF ground state, i.e., a quasi-sextet in YbPtBi. At the same time, our study shows the potential of the a.c. elastocaloric effect to control and quantify strain-induced changes of the CEF schemes, opening a different route to disentangle the CEF energy scales from other relevant energy scales in correlated quantum materials.
Lattice strains of appropriate symmetry have served as an excellent tool to explore the interaction of superconductivity in the iron-based superconductors with nematic and stripe spin-density wave (SSDW) order, which are both closely tied to an orthorhombic distortion. In this work, we contribute to a broader understanding of the coupling of strain to superconductivity and competing normal-state orders by studying CaKFe$_4$As$_4$ under large, in-plane strains of $B_{1g}$ and $B_{2g}$ symmetry. In contrast to the majority of iron-based superconductors, pure CaKFe$_4$As$_4$ exhibits superconductivity with relatively high transition temperature of $T_c\,\sim\,$35 K in proximity of a non-collinear, tetragonal, hedgehog spin-vortex crystal (SVC) order. Through experiments, we demonstrate an anisotropic in-plane strain response of $T_c$, which is reminiscent of the behavior of other pnictides with nematicity. However, our calculations suggest that in CaKFe$_4$As$_4$, this anisotropic response correlates with the one of the SVC fluctuations, highlighting the close interrelation of magnetism and high-$T_c$ superconductivity. By suggesting moderate $B_{2g}$ strains as an effective parameter to change the stability of SVC and SSDW, we outline a pathway to a unified phase diagram of iron-based superconductivity.
The honeycomb antiferromagnet BaCo2(AsO4)(2), in which small in-plane magnetic fields (H1 approximate to 0.26 T and H2 approximate to 0.52 T at T = 1.8 K < T-N approximate to 5.4 K) induce two magnetic phase transitions, has attracted attention as a possible candidate material for the realization of Kitaev physics based on the 3d element Co2+. Here, we report on the change in the transition temperature T-N and the critical fields H1 and H2 of BaCo2(AsO4)(2) with hydrostatic pressure up to similar to 20 kbar, as determined from magnetization and specific heat measurements. Within this pressure range, a marginal increase in the magnetic ordering temperature is observed. At the same time, the critical fields are changed significantly (up to similar to 25-35%). Specifically, we find that H1 is increased with hydrostatic pressure, i.e., the antiferromagnetic state is stabilized, whereas H2, which was previously associated with a transition into a proposed Kitaev spin-liquid state, decreases with increasing pressure. We discuss to what extent these results are compatible with suggested models with sizable third-nearest-neighbor exchange. Overall, the results put constraints on the magnetic models that are used to describe the low-temperature magnetic properties of BaCo2(AsO4)(2).
The families of organic charge-transfer salts κ-(BEDT-TTF)2X and κ-(BETS)2X, where BEDT-TTF and BETS stand for the organic donor molecules C10H8S8 and C10H8S4Se4, respectively, and X for an inorganic electron acceptor, have been proven to serve as a powerful playground for the investigation of the physics of frustrated Mott insulators. These materials have been ascribed a model character, since the dimerization of the organic molecules allows to map these materials onto a single band Hubbard model, in which the dimers reside on an anisotropic triangular lattice. By changing the inorganic unit X or applying physical pressure, the correlation strength and anisotropy of the triangular lattice can be varied. This has led to the discovery of a variety of exotic phenomena, including quantum-spin liquid states, a plethora of long-range magnetic orders in proximity to a Mott metal-insulator transition, and unconventional superconductivity. While many of these phenomena can be described within this effective one-band Hubbard model on a triangular lattice, it has become evident in recent years that this simplified description is insufficient to capture all observed magnetic and electronic properties. The ingredients for generalized models that are relevant include, but are not limited to, spin-orbit coupling, intra-dimer charge and spin degrees of freedom, electron-lattice coupling, as well as disorder effects. Here, we review selected theoretical and experimental discoveries that clearly demonstrate the relevance thereof. At the same time, we outline that these aspects are not only relevant to this class of organic charge-transfer salts, but are also receiving increasing attention in other classes of inorganic strongly correlated electron systems. This reinforces the model character that the κ-phase organic charge-transfer salts have for understanding and discovering novel phenomena in strongly correlated electron systems from a theoretical and experimental point of view.
Members of the CaK(Fe$_{1-x}$Mn$_{x}$)$_{4}$As$_{4}$ series have been synthesized in single crystalline form and characterized by elemental analysis, thermodynamic and transport measurements. These measurements show that the superconducting transition temperature decreases monotonically and is finally suppressed below 1.8 K. For $x$-values greater than 0.016, signatures of a magnetic transition can be detected in both thermodynamic and transport measurements in which kink-like features allow for the determination of the transition temperature, $T^*$, that increases as Mn substitution increases. A temperature-composition ($T$-$x$) phase diagram is constructed, revealing a half-dome of superconductivity with the magnetic transition temperature, $T^*$, appearing near 26 K for $x$ $\sim$ 0.017 and rising slowly up to 33 K for $x$ $\sim$ 0.036. Specific heat data are used to track the jump in specific heat at $T_c$; The CaK(Fe$_{1-x}$Mn$_x$)$_4$As$_4$ data does not follow the scaling of $\Delta$$C_{p}$ with $T_{c}^3$ as many of the other Fe-based superconducting systems do. Elastoresistivity coefficients, $2m_{66}$ and $m_{11}-m_{12}$, as a function of temperature are also measured. $2m_{66}$ and $m_{11}-m_{12}$ are qualitatively similar to CaK(Fe$_{1-x}$Ni$_x$)$_4$As$_4$. This may indicate that the magnetic order in Mn substituted system may be still the same as CaK(Fe$_{1-x}$Ni$_x$)$_4$As$_4$. A clear change in $H^\prime_{c2}$($T$)/$T_c$, where $H^\prime_{c2}$($T$) is d$H_{c2}$($T$)/d$T$, at $x$ $\sim$ 0.015 is observed and probably is related to change of the Fermi surface due to magnetic order. Coherence lengths and the London penetration depths are also calculated based on $H_{c1}$ and $H_{c2}$ data. Coherence lengths as the function of $x$ also shows the changes near $x$ = 0.015.
We present the pressure-temperature phase diagram La5Co2Ge3 up to similar to 5 GPa, which was constructed from magnetization, resistivity, and specific heat measurements. At ambient pressure, La5Co2Ge3 is an itinerant ferromagnet with a Curie temperature T-C similar to 4 K. Upon increasing pressure up to similar to 1.7 GPa, Tc is suppressed down to similar to 3 K. Upon further increasing pressure, our results suggest that La5Co2Ge3 enters a different low-temperature ground state. The corresponding transition temperature T* has a nonmonotonic pressure dependence up to similar to 5 GPa. Our results demonstrate that the ferromagnetic quantum critical point in La5Co2Ge3 is avoided by the appearance of a different, likely magnetically ordered, state that has an antiferromagnetic component.
Organic salts represent an ideal experimental playground for studying the interplay between magnetic and charge degrees of freedom, which has culminated in the discovery of several spin-liquid candidates such as κ-(ET)_{2}Cu_{2}(CN)_{3} (κ-Cu). Recent theoretical studies indicate the possibility of chiral spin liquids stabilized by ring exchange, but the parent states with chiral magnetic order have not been observed in this material family. In this Letter, we discuss the properties of the recently synthesized κ-(BETS)_{2}Mn[N(CN)_{2}]_{3} (κ-Mn). Based on analysis of specific heat, magnetic torque, and NMR measurements combined with ab initio calculations, we identify a spin-vortex crystal order. These observations definitively confirm the importance of ring exchange in these materials and support the proposed chiral spin-liquid scenario for triangular lattice organics.