Low-temperature Ground State Research Articles

Role of Lanthanides and Bilayer Fe2As2 in the Electronic Properties of RbLn2Fe4As4O2 (Ln = Gd, Tb, and Dy) Superconductors.

The superconducting transition temperatures (Tc) of RbGd2Fe4As4O2, RbTb2Fe4As4O2, and RbDy2Fe4As4O2 are 35 K, 34.7 K, and 34.3 K without doping, respectively. For the first time, we have studied the high-temperature nonmagnetic state and the low-temperature magnetic ground state of 12442 materials, RbTb2Fe4As4O2 and RbDy2Fe4As4O2, using first principles calculations and comparing them with RbGd2Fe4As4O2. We also performed a detailed study of the effects of lanthanides and bilayer Fe2As2. We predict that the ground state of RbLn2Fe4As4O2 (Ln = Gd, Tb, and Dy) is spin-density-wave-type, in-plane, striped antiferromagnets, and the magnetic moment around each Fe atom is about 2 μB. We also found that the structural differences caused by the simple ionic radius have little effect on the properties of these three materials. Different lanthanide elements themselves play a major role in the electronic properties of the materials. It can be confirmed that the effect of Gd on RbLn2Fe4As4O2 is indeed different from that of Tb and Dy, and the presence of Gd is more conducive to interlayer electron transfer. This means that Gd can transfer more electrons from the GdO layer to the FeAs layer compared to Tb and Dy. Therefore, RbGd2Fe4As4O2 has a stronger internal coupling strength of the bilayer Fe2As2 layer. This can explain why the Tc of RbGd2Fe4As4O2 is slightly higher than that of RbTb2Fe4As4O2 and RbDy2Fe4As4O2.

Negative Magnetoresistance in Hopping Regime of Lightly Doped Thermoelectric SnSe

Semiconducting SnSe, an analog of black phosphorus, recently attracted great scientific interest due to a disputed report of a large thermoelectric figure of merit, which has not been reproduced subsequently. Here we concentrate on the low-temperature ground state. To gain a better understanding of the system, we present magneto-transport properties in high-quality single crystals of as-grown, lightly doped SnSe down to liquid helium temperatures. We show that SnSe behaves as a p-type doped semiconductor in the vicinity of a metal-insulator transition. Electronic transport at the lowest temperatures is dominated by the hopping mechanism. Negative magnetoresistance at low fields is well described by antilocalization, while positive magnetoresistance at higher fields is consistent with the shrinkage of localized impurity wavefunctions. At higher temperatures, a dilute metallic regime is realized where elusive T2 and B2 resistivity dependence is observed, posing a challenge to theoretical comprehension of the underlying physical mechanism.

Near room temperature stepwise spin state switching and photomagnetic effect in a mixed-valence molecular square.

A two-step thermo-induced spin-state switching was observed in a cyanide-bridged [Fe2Fe2] molecular square complex, {[Fe(pzTp)(CN)3]2[Fe(L)2]2}[Fe(pzTp)(CN)3]2·4CH3OH·2H2O [1·4MeOH·2H2O; pzTp = tetrakis(pyrazol-1-yl)borate and L = bis(1-ethylimidazol-2-yl)ketone (bik*)], which was characterized fully by single-crystal X-ray diffraction, (photo)magnetic measurements, and spectroscopic techniques. 1·4MeOH·2H2O exhibited a two-step thermo-induced spin transition with T1/2 (1) ↑ = 306 K and T1/2 (2) ↑ = 370 K converting the low-temperature ground state, {[(FeIIILS)2(FeIILS)2](FeIIILS)2} into the high-temperature state, {[(FeIIILS)2(FeIIHS)2](FeIIILS)2} via a stable intermediate phase. The desolvated phase, 1 also exhibited a gradual but reversible thermo-induced spin state change with a T1/2 value of 190 K, significantly shifted to a lower temperature. It also exhibited photo-induced spin-state switching at 20 K with the TLIESST value of 60 K.

Crossover in Low-temperature Ground State of Fe(Se,Te) Compounds

Crossover in Low-temperature Ground State of Fe(Se,Te) Compounds

Compositional phase stability in medium-entropy and high-entropy Cantor-Wu alloys from an ab initio all-electron Landau-type theory and atomistic modeling

We describe implementation and analysis of a first-principles theory, derived in an earlier work, for the leading terms in an expansion of a Gibbs free energy of a multi-component alloy in terms of order parameters that characterize potential, compositional phases. The theory includes effects of rearranging charge and other electronics from changing atomic occupancies on lattice sites. As well as the rigorous description of atomic short-range order in the homogeneously disordered phase, pairwise interaction parameters suited for atomistic modelling in a multicomponent setting can be calculated. From our study of an indicative series of the Cantor-Wu alloys, NiCo, NiCoCr, NiCoFeCr, and NiCoFeMnCr, we find that the interactions are not approximated well either as pseudobinary or restricted to nearest neighbour range. Our computed order-disorder transition temperatures are low, consistent with experimental observations, and the nature of the ordering is dominated by correlations between Ni, Co, and Cr, while Fe and Mn interact weakly. Further atomistic modelling suggests that there is no true single-phase low-temperature ground state for these multicomponent systems. Instead the single-phase solid solution is kept stable to low temperatures by the large configurational entropy and the Fe, Mn dilution effects. The computationally cost-effectiveness of our method makes it a good candidate for further exploration of the space of multicomponent alloys.

Charge-ordered state satisfying the Anderson condition in LiRh2O4 arising from local dimer order

We report on the charge-ordered structure of LiRh2O4 arising below the metal-insulator transition at 170 K. Structural studies using synchrotron X-rays have revealed that the charge-ordered states of Rh3+ and Rh4+ with dimerization are realized in the low-temperature phase below 170 K. Although the low-temperature ground state resembles that of CuIr2S4, a charge ordering pattern satisfying the Anderson condition is realized in LiRh2O4. Based on structural information such as the short-range order of dimers appearing above the transition temperature and the weakening of the correlation between rhodium one-dimensional chains appearing in the crystal structure, we argue that the Coulomb interaction plays an important role in determining the charge ordering patterns.

Phase diagram of CeSb2 from magnetostriction and magnetization measurements: Evidence for ferrimagnetic and antiferromagnetic states

Cerium diantimonide ($\mathrm{Ce}{\mathrm{Sb}}_{2}$) is one of a family of rare-earth-based magnetic materials that exhibit metamagnetism, enabling control of the magnetic ground state through an applied magnetic field. At low temperatures, $\mathrm{Ce}{\mathrm{Sb}}_{2}$ hosts a rich phase diagram with multiple magnetically ordered phases for many of which the order parameter is only poorly understood. In this paper, we report a study of its metamagnetic properties by scanning tunneling microscopy (STM) and magnetization measurements. We use STM measurements to characterize the sample magnetostriction with subpicometer resolution from magnetic field and temperature sweeps. This allows us to directly assess the bulk phase diagram as a function of field and temperature and relate spectroscopic features from tunneling spectroscopy to bulk phases. Our magnetostriction and magnetization measurements indicate that the low-temperature ground state at zero field is ferrimagnetic. Quasiparticle interference mapping shows evidence for a reconstruction of the electronic structure close to the Fermi energy upon entering the magnetically ordered phase.

One-dimensional narrow-band conductors

We review one-dimensional lattice models and the corresponding results that describe the low-temperature properties of quasi-one-dimensional lattice systems with long-range interaction. A widely known example is narrow-band low-dimensional conductors with long-range interelectron repulsion. The models deal with particles that live on the one-dimensional host lattice (chain), translation invariant or disordered, and interact via the long-range repulsive potential. The results are presented concerning the translation invariant host chain, in particular: the low-temperature thermodynamics incommensurable ground states and related devil-staircase form of various characteristics as functions of pertinent parameters, the self-localization of particles, a new branch of elementary excitations, etc. In the disordered case, where the sites of the host chain fluctuate randomly around the sites of the periodic chain, the low-temperature thermodynamics and the structure of the ground state are discussed in the framework of a certain model, which we call the cluster model and which seems to be a fairly reasonable approximation for low temperatures and small concentration of particles. Using analytical and numerical tools we analyze the thermodynamics and the ground state of the model. The latter proves to be a sequence of random domains and we study in detail their distribution.

Evolution of the electronic structure in Ta2NiSe5 across the structural transition revealed by resonant inelastic x-ray scattering

We utilized high-energy-resolution resonant inelastic X-ray scattering (RIXS) at both the Ta and Ni $L_3$-edges to map out element-specific particle-hole excitations in Ta$_2$NiSe$_5$ across the phase transition. Our results reveal a momentum dependent gap-like feature in the low energy spectrum, which agrees well with the band gap in element-specific joint density of states calculations based on ab initio estimates of the electronic structure in both the low temperature monoclinic and the high temperature orthorhombic structure. Below $T_c$, the RIXS energy-momentum map shows a minimal gap at the Brillouin zone center ($\sim$ 0.16 eV), confirming that Ta$_2$NiSe$_5$ possesses a direct band gap in its low temperature ground state. However, inside the gap, no signature of anticipated collective modes with an energy scale comparable to the gap size can be identified. Upon increasing the temperature to above $T_c$, whereas the gap at the zone center closes, the RIXS map at finite momenta still possesses the gross features of the low temperature map, suggesting a substantial mixing between the Ta and Ni orbits in the conduction and valence bands, which does not change substantially across the phase transition. Our experimental observations and comparison to the theoretical calculations lend further support that the phase transition and the corresponding gap opening in Ta$_2$NiSe$_5$ is largely structural by nature with possible minor contribution from the putative exciton condensate.

Multiband effect in elastoresistance of Fe(Se,Te)

We have investigated the elastoresistance of two Tex () compounds that have a close chemical composition but differ significantly in electronic properties. The first compound has a negative temperature coefficient of resistance and does not show any phase transitions other than a superconducting one. The elastoresistance of this compound approximately follows the law which is a special case of the Curie-Weiss law, which is usually observed for Fe(Se,S) with metallic conductivity. The second compound has a metallic type of conductivity and, in addition to the superconducting transition, there is also a phase transition at a temperature of about 30 K. The elastoresistance of the second compound is sign-reversing and can be approximated with the sum of two Curie-Weiss–type terms with opposite signs and different critical temperatures. We attribute this behavior to the competition of contributions to the elastoresistance from different band valleys. These competing contributions may appear since the composition of our compound is close to the critical point at which the low-temperature ground state in the 11 series of iron-based superconductors changes from electronic nematic order to magnetic order.

Sharp steps in magnetization, magnetoresistance, and magnetostriction in Pr0.6Sr0.4Co1−yGayO3

We report the magnetization, magnetoresistance, and magnetostriction in polycrystalline Pr0.6Sr0.4Co1−yGayO3 (y = 0.0–0.3) samples. Upon substitution of the non-magnetic Ga3+ cation for Co3+, the low temperature ground state transforms from a ferromagnetic metal for y = 0 to a cluster glass type semiconductor for y ≥ 0.2. The field-dependent magnetization, magnetoresistance, and magnetostriction for y ≥ 0.2 show reversible abrupt steps for both positive and negative magnetic fields at T ≤ 3 K, whereas all these quantities vary smoothly with the magnetic field above 4 K. Such steps in all three distinct physical quantities were never reported earlier in perovskite cobaltites, and they differ from observations made in manganites and intermetallic alloys. It is suggested that field-induced avalanche flipping of ferromagnetic clusters is the origin of observed steps in all these three quantities.

Neutron scattering study of commensurate magnetic ordering in single crystal CeSb2

Temperature and field-dependent magnetization M(T, H ) measurements and neutron scattering study of a single crystal CeSb2 are presented. Several anomalies in magnetization curves have been confirmed, i.e., at 15.6 K, 12 K, and 9.8 K, respectively. These three transitions are all metamagnetic transitions, which shift to lower temperatures as the magnetic field increases. In contrast to the previous studies that the anomaly at 15.6 K has been suggested as paramagnetic to ferromagnetic phase transition, in our measurement no hysteresis loop around zero field with either H ∥ c or H ⊥ c has been observed. The anomaly located at around 12 K is antiferromagnetic-like transition, and this turning point will clearly split into two when the magnetic field H ⩾ 2 kOe. A neutron scattering study reveals that the low temperature ground state of CeSb2 orders magnetically with commensurate propagation wave vectors k = (−1, ±1/6, 0) and k = (±1/6, −1, 0), with phase transition temperature TC ∼ 9.8 K.

Cluster functional renormalization group and absence of a bilinear spin liquid in the J1−J2 Heisenberg model

The pseudofermion functional renormalization group (pf-FRG) has been put forward as a semi-analytical scheme that, for a given microscopic spin model, allows to discriminate whether the low-temperature states exhibit magnetic ordering or a tendency towards the formation of quantum spin liquids. However, the precise nature of the putative spin liquid ground state has remained hard to infer from the original (single-site) pf-FRG scheme. Here we introduce a cluster pf-FRG approach, which allows for a more stringent connection between a microscopic spin model and its low-temperature spin liquid ground states. In particular, it allows to calculate spatially structured fermion bilinear expectation values on spatial clusters, which are formed by splitting the original lattice into several sublattices, thereby allowing for the positive identification of a family of bilinear spin liquid states. As an application of this cluster pf-FRG approach, we consider the $J_1$-$J_2$ SU($N$)-Heisenberg model on a square lattice, which is a paradigmatic example for a frustrated quantum magnet exhibiting quantum spin liquid behavior for intermediate coupling strengths. In the well-established large-$N$ limit of this model, we show that our approach correctly captures the emergence of the $\pi$-flux spin liquid state at low temperatures. For small $N$, where the precise nature of the ground state remains controversial, we focus on the widely studied case of $N=2$, for which we determine the low-temperature phase diagram near the strongly-frustrated regime after implementing the fermion number constraint by the flowing Popov-Fedotov method. Our results suggest that the $J_1$-$J_2$-Heisenberg model does not support the formation of a fermion bilinear spin liquid state.

Multiple Competing Magnetic Interactions in Na4Ni7(PO4)6

The low-temperature magnetic behavior and ground state of the candidate sodium-ion battery cathode compound Na4Ni7(PO4)6 have been investigated by physical property measurements and neutron powder ...

Quantum jamming transition to a correlated electron glass in 1T-TaS2.

Distinct many-body states may be created under non-equilibrium conditions through different ordering paths, even when their constituents are subjected to the same fundamental interactions. The phase-transition mechanism to such states remains poorly understood. Here, we show that controlled optical or electromagnetic perturbations can lead to an amorphous metastable state of strongly correlated electrons in a quasi-two-dimensional dichalcogenide. Scanning tunnelling microscopy reveals a hyperuniform pattern of localized charges, whereas multitip surface nanoscale conductivity measurements and tunnelling spectroscopy show an electronically gapless conducting state that is different from conventional Coulomb glasses and many-body localized systems. The state is stable up to room temperature and shows no signs of either local charge order or phase separation. The mechanism for its formation is attributed to a dynamical localization of electrons through mutual interactions. Theoretical calculations confirm the correlations between localized charges to be crucial for the state's unusual stability.

Magnetic Field-Driven Spin-Flop Transition in Orthorhombic GdGa

Structural and magnetic properties of GdGa are investigated using the combined results of X-ray diffraction and magnetization. DC magnetization measurements were carried out on as-cast and annealed specimens. Although, no considerable changes in the crystal parameters are observed by the effect of annealing, the change in the magnetic behavior is discernible. The low-temperature state is found to be simple antiferromagnetic with prevailing ferromagnetic exchange interactions in the paramagnetic state. The mismatch between the experimentally obtained effective magnetic moment of Gd in GdGa and the effective magnetic moment of $$\hbox {Gd}^{+3}$$ is attributed to the presence of finite-sizable spin–orbit coupling. Moreover, the weakly correlated antiferromagnetic low-temperature ground state can be easily tuned to the ferromagnetic state through a spin-flop process.

Phase Stability of Dynamically Disordered Solids from First Principles.

Theoretical studies of phase stability in solid materials with dynamic disorder are challenging due to the failure of the standard picture of atoms vibrating around fixed equilibrium positions. Dynamically disordered solid materials show immense potential in applications. In particular, superionic conductors, where the disorder results in exceptionally high ionic conductivity, are very promising as solid state electrolytes in batteries and fuel cells. The biggest obstacle in living up to this potential is the limited stability of the dynamically disordered phases. Here, we outline a method to obtain the free energy of a dynamically disordered solid. It is based on a stress-strain thermodynamic integration on a deformation path between a mechanically stable ordered variant of the disordered phase, and the dynamically disordered phase itself. We show that the large entropy contribution associated with the dynamic disorder is captured in the behavior of the stress along the deformation path. We apply the method to Bi_{2}O_{3}, whose superionic δ phase is the fastest known solid oxide ion conductor. We accurately reproduce the experimental transition enthalpy and the critical temperature of the phase transition from the low temperature ground state α phase to the superionic δ phase. The method can be used for a first-principles description of the phase stability of superionic conductors and other materials with dynamic disorder, when the disordered phase can be connected to a stable phase through a continuous deformation path.

3d-4f coupling and multiferroicity in frustrated Cairo Pentagonal oxide DyMn2O5

In solid state science, multifunctional materials and especially multiferroics have attracted a great deal of attention, as they open the possibility for next generation spintronic and data storage devices. Interestingly, while many of them host coexisting 3d and 4f elements, the role of the coupling between these two magnetic entities has remained elusive. By means of single crystal neutron diffraction and inelastic neutron scattering experiments we shed light on this issue in the particular case of the multiferroic oxide DyMn2O5. This compound undergoes a first order magnetic transition from a high temperature incommensurate phase to a low temperature commensurate one. Our investigation reveals that although these two phases have very different magnetic structures, the spin excitations are quite similar indicating a fragile low temperature ground state with respect to the high temperature one. Such a rare scenario is argued to be a manifestation of the competition between the exchange interaction and 4f magnetic anisotropy present in the system. It is concluded that the magnetic structure, hence the ferroelectricity, can be finely tuned depending on the anisotropy of the rare earth.

3d -electron Heisenberg pyrochlore Mn2Sb2O7

In frustrated magnetic systems, geometric constraints or the competition amongst interactions introduce extremely high degeneracy and prevent the system from readily selecting a low-temperature ground state. The most frustrated known spin arrangement is on the pyrochlore lattice, but nearly all magnetic pyrochlores have unquenched orbital angular momentum, constraining the spin directions through spin-orbit coupling. Pyrochlore Mn$_2$Sb$_2$O$_7$ is an extremely rare Heisenberg pyrochlore system, with directionally-unconstrained spins and low chemical disorder. We show that it undergoes a spin-glass transition at 5.5K, which is suppressed by disorder arising from Mn vacancies, indicating this ground state to be a direct consequence of the spins' interactions. The striking similarities to $3d$ transition metal pyrochlores with unquenched angular momentum suggests that the low spin-orbit coupling in the $3d$ block makes Heisenberg pyrochlores far more accessible than previously imagined.

On the multiferroic skyrmion-host GaV4S8

The lacunar spinel GaV4S8 exhibits orbital ordering at 44 K and shows a complex magnetic phase diagram below 12.7 K, which includes ferromagnetic and cycloidal spin order. At low but finite external magnetic fields, Néel-type skyrmions are formed in this material. Skyrmions are whirl-like spin vortices that have received great theoretical interest because of their non-trivial spin topology and that are also considered as basic entities for new data-storage technologies. Interestingly, we found that the orbitally ordered phase shows sizable ferroelectric polarisation and that excess spin-driven polarisations appear in all magnetic phases, including the skyrmion-lattice phase. Hence, GaV4S8 shows simultaneous magnetic and polar order and belongs to the class of multiferroics materials that attracted enormous attention in recent years. Here, we summarise the existing experimental information on the magnetic, electronic and dielectric properties of GaV4S8. By performing detailed magnetic susceptibility, resistivity, specific heat and dielectric experiments, we complement the low-temperature phase diagram. Specifically, we show that the low-temperature and low-field ground state of GaV4S8 seems to have a more complex spin configuration than purely collinear ferromagnetic spin order. In addition, at the structural Jahn–Teller transition the magnetic exchange interaction changes from antiferromagnetic to ferromagnetic. We also provide experimental evidence that the vanadium V4 clusters in GaV4S8 can be regarded as molecular units with spin 1/2. However, at high temperatures deviations in the susceptibility show up, indicating that either the magnetic moments of the vanadium atoms fluctuate independently or excited states of the V4 molecule become relevant.