Strong Antiferromagnetic Correlations Research Articles

Unraveling pairon excitations and the antiferromagnetic contributions in the cuprate specific heat

Thermal measurements, such as entropy and specific heat, reveal key elementary excitations for understanding the cuprates. In this paper, we study the specific heat measurements on three different compounds La2−xSrxCuO4, Bi2Sr2CaCu2O8+δ and YBa2Cu3O7−δ and show that the data are compatible with ‘pairons’ and their excitations. However, the precise fits require the contribution of the antiferromagnetic entropy deduced from the magnetic susceptibility χ(T).Two temperature scales are involved in the excitations above the critical temperature Tc: the pseudogap T∗, related to pairon excitations, and the magnetic correlation temperature, Tmax, having very different dependencies on the carrier density (p). In agreement with our previous analysis of χ(T), the Tmax(p) line is not the signature of a gap in the electronic density of states, but is rather the temperature scale of strong local antiferromagnetic correlations which dominate for low carrier concentration. These correlations progressively evolve into paramagnetic fluctuations in the overdoped limit.Our results are in striking contradiction with the model of Tallon and Storey (2023), who reaffirm the idea of a T-independent gap Eg, whose temperature scale Tg=Eg/kB decreases linearly with p and vanishes at a critical value pc∼0.19.Finally, we discuss the unconventional fluctuation regime above Tc, which is associated with a mini-gap δ∼ 2meV in the pairon excitation spectrum. This energy scale is fundamental to the condensation mechanism.

Combinatorial Synthesis of Cation-Disordered Manganese Tin Nitride MnSnN2 Thin Films with Magnetic and Semiconducting Properties

Magnetic semiconductors may soon improve the energy efficiency of microelectronics, but materials exhibiting these dual properties remain underexplored. Here, we report the computational prediction and realization of a new magnetic and semiconducting material, MnSnN2, via combinatorial sputtering of thin films. Grazing incidence wide-angle X-ray scattering and laboratory X-ray diffraction studies show MnSnN2 exhibits a wurtzite-like crystal structure with cation disorder. This new material has a wide composition tolerance, with a single-phase region ranging from 20% < Mn/(Mn + Sn) < 65%. Spectroscopic ellipsometry identifies an optical absorption onset of 1 eV, consistent with the computationally predicted 1.2 eV bandgap. Resistivity measurements as a function of temperature support the semiconducting nature of MnSnN2. Hall effect measurements show carrier density has a weak inverse correlation with temperature, indicating that the charge transport mechanisms are more complex than in a pristine semiconductor. Magnetic susceptibility measurements reveal a low-temperature magnetic ordering transition (≈10 K) for MnSnN2 and strong antiferromagnetic correlations. This finding contrasts with bulk, cation-ordered MnSiN2 and MnGeN2, which exhibited antiferromagnetic ordering above 400 K in previous studies. To probe the origin of this difference, we perform Monte Carlo simulations of cation-ordered and cation-disordered MnSnN2. They reveal that cation disorder lowers the magnetic transition temperature relative to the ordered phase. In addition to discovering a new compound, this work shows that future efforts could use cation (dis)order to tune magnetic transitions in semiconducting materials for precise control of properties in microelectronics.

Formation of CuO$_2$ sublattices by suppression of interlattice correlations in tetragonal CuO

We investigate the tetragonal phase of the binary transition metal oxide CuO (t-CuO) within the context of cellular dynamical mean-field theory. Due to its strong antiferromagnetic correlations and simple structure, analysing the physics of t-CuO is of high interest as it may pave the way towards a more complete understanding of high-temperature superconductivity in hole-doped antiferromagnets. In this work we give a formal justification for the weak-coupling assumption that has previously been made for the interconnected sublattices within a single layer of t-CuO by studying the non-local self-energies of the system. We compute momentum-resolved spectral functions using a Matrix Product State (MPS)-based impurity solver directly on the real axis, which does not require any numerically ill-conditioned analytic continuation. The agreement with photoemission spectroscopy indicates that a single-band Hubbard model is sufficient to capture the material’s low energy physics. We perform calculations on a range of different temperatures, finding two magnetic regimes, for which we identify the driving mechanism behind their respective insulating state. Finally, we show that in the hole-doped regime the sublattice structure of t-CuO has interesting consequences on the symmetry of the superconducting state.

High-Throughput Selection and Experimental Realization of Two New Ce-Based Nitride Perovskites: CeMoN3 and CeWN3.

Nitride perovskites have only been experimentally realized in very few cases despite the widespread existence and commercial importance of perovskite materials. From oxide perovskites used in ultrasonics to halide perovskites that have revolutionized the photovoltaics industry, the discovery of new perovskite materials has historically impacted a wide number of fields. Here, we add two new perovskites, CeWN3 and CeMoN3, to the list of experimentally realized perovskite nitrides using high-throughput computational screening and subsequent high-throughput thin film growth techniques. Candidate compositions are first down-selected using a tolerance factor and then thermochemical stability. A novel competing fluorite-family phase is identified for both material systems, which we hypothesize is a transient intermediate phase that crystallizes during the evolution from an amorphous material to a stable perovskite. Different processing routes to overcome the competing fluorite phase and obtain phase-pure nitride perovskites are demonstrated for the CeMoN3–x and CeWN3–x material systems, which provide a starting point for the development of future nitride perovskites. Additionally, we find that these new perovskite phases have interesting low-temperature magnetic behavior: CeMoN3–x orders antiferromagnetically below TN ≈ 8 K with indications of strong magnetic frustration, while CeWN3–x exhibits no long-range order down to T = 2 K but has strong antiferromagnetic correlations. This work demonstrates the importance and effectiveness of using high-throughput techniques, both computational and experimental: they are integral to optimize the process of realizing two entirely novel nitride perovskites.

Realization of a Fermi-Hubbard Optical Tweezer Array.

We use lithium-6 atoms in an optical tweezer array to realize an eight-site Fermi-Hubbard chain near half filling. We achieve single site detection by combining the tweezer array with a quantum gas microscope. By reducing disorder in the energy offsets to less than the tunneling energy, we observe Mott insulators with strong antiferromagnetic correlations. The measured spin correlations allow us to put an upper bound on the entropy of 0.26(4)k_{B} per atom, comparable to the lowest entropies achieved with optical lattices. Additionally, we establish the flexibility of the tweezer platform by initializing atoms on one tweezer and observing tunneling dynamics across the array for uniform and staggered 1D geometries.

Evidence for canonical spin glass behaviour in polycrystalline Mn1.5Fe1.5Al Heusler alloy

Magnetic properties of magnetically frustrated polycrystalline Mn1.5Fe1.5Al Heusler type alloy with a β-Mn structure were systematically studied using dc magnetization, ac susceptibility, magnetic relaxation and magnetic memory effect measurements to understand its magnetic ground state. The Mn1.5Fe1.5Al alloy system exhibits a sharp peak at low temperature around 34.5 K with strong antiferromagnetic correlations (θCW ∼ −639 K) and a high degree of frustration (fp ∼ 18.7) which suggest the presence of competing magnetic interactions. Despite of strong antiferromagnetic correlations, this peak has spin-glass character as confirmed by the observations of bifurcation of the zero-field-cooled and field-cooled magnetization curves below the irreversibility temperature, field dependent shift of the irreversibility temperature, unidirectional exchange bias effect on the field-cooled M-H hysteresis loop, exponential decay of the temperature variation of remanence and coercivity, frequency dependent shift of the spin glass freezing temperature (Tf) as per the dynamic scaling laws given by the critical slowing down model and Vogel-Fulcher law, magnetic relaxation and magnetic memory effect below Tf. The observation of a clear asymmetric response with respect to the temperature cycling in the magnetic relaxation measurements validates the hierarchical model of the spin-glass magnetic relaxation in Mn1.5Fe1.5Al alloy. Since the behaviour exhibited by the Mn1.5Fe1.5Al alloy has perfect similarity with the well-known atomic spin glasses like CuMn, AuFe, therefore, it may be considered as canonical spin-glass system.

Defect-mediated ferromagnetism in correlated two-dimensional transition metal phosphorus trisulfides.

Controlling the magnetic spin states of two-dimensional (2D) van der Waals (vdW) materials with strong electronic or magnetic correlation is important for spintronic applications but challenging. Crystal defects that are often present in 2D materials such as transition metal phosphorus trisulfides (MPS3) could influence their physical properties. Here, we report the effect of sulfur vacancies on the magnetic exchange interactions and spin ordering of few-layered vdW magnetic Ni1−xCoxPS3 nanosheets. Magnetic and structural characterization in corroboration with theoretical calculations reveal that sulfur vacancies effectively suppress the strong intralayer antiferromagnetic correlation, giving rise to a weak ferromagnetic ground state in Ni1−xCoxPS3 nanosheets. Notably, the magnetic field required to tune this ferromagnetic state (<300 Oe) is much lower than the value needed to tune a typical vdW antiferromagnet (> several thousand oersted). These findings provide a previously unexplored route for controlling competing correlated states and magnetic ordering by defect engineering in vdW materials.

Imaging the formation and surface phase separation of the CE phase

The CE phase is an extraordinary phase exhibiting the simultaneous spin, charge, and orbital ordering due to strong electron correlation. It is an ideal platform to investigate the role of the multiple orderings in the phase transitions and discover emergent properties. Here, we use a cryogenic high-field magnetic force microscope to image the phase transitions and properties of the CE phase in a Pr0.5Ca0.5MnO3 thin film. In a high magnetic field, we observed a clear suppression of magnetic susceptibility at the charge-ordering insulator transition temperature (TCOI), whereas, at the Néel temperature (TN), no significant change is observed. This observation favors the scenario of strong antiferromagnetic correlation developed below TCOI but raises questions about the Zener polaron paramagnetic phase picture. Besides, we discoverd a phase-separated surface state in the CE phase regime. Ferromagnetic phase domains residing at the surface already exist in zero magnetic field and show ultra-high magnetic anisotropy. Our results provide microscopic insights into the unconventional spin- and charge-ordering transitions and revealed essential attributes of the CE phase, highlighting unusual behaviors when multiple electronic orderings are involved.

Proximate Quantum Spin Liquid on Designer Lattice.

Complementary to bulk synthesis, here we propose a designer lattice with extremely high magnetic frustration and demonstrate the possible realization of a quantum spin liquid state from both experiments and theoretical calculations. In an ultrathin (111) CoCr2O4 slice composed of three triangular and one kagome cation planes, the absence of a spin ordering or freezing transition is demonstrated down to 0.03 K, in the presence of strong antiferromagnetic correlations in the energy scale of 30 K between Co and Cr sublattices, leading to the frustration factor of ∼1000. Persisting spin fluctuations are observed at low temperatures via low-energy muon spin relaxation. Our calculations further demonstrate the emergence of highly degenerate magnetic ground states at the 0 K limit, due to the competition among multiply altered exchange interactions. These results collectively indicate the realization of a proximate quantum spin liquid state on the synthetic lattice.

Iron oxidation state in La0.7Sr1.3Fe0.7Ti0.3O4 and La0.5Sr1.5Fe0.5Ti0.5O4 layered perovskites: Magnetic properties

La0.5Sr1.5Fe0.5Ti0.5O4 and La0.7Sr1.3Fe0.7Ti0.3O4 solid solutions with the layered perovskite structure were synthesized using a solid state method. Structural properties of obtained samples were characterized using X-ray diffraction and X-ray fluorescence analyses. Magnetic properties were investigated using magnetometry, electron spin resonance (ESR) and Mössbauer spectroscopy methods. Based on magnetization and ESR measurements it was suggested the presence of Fe4+ ions in addition to trivalent iron ions that was exactly confirmed by Mössbauer spectroscopy investigations. Based on all experimental results one can suggest the presence of the electronic phase separation in the investigated samples – the simultaneous existence of the paramagnetic phase and magnetically correlated regions, which form due to the mixed-valence iron ions. So the paramagnetic phase with strong antiferromagnetic correlation exists in both samples, while the second phase is ferromagnetically and ferrimagnetically correlated regions in La0.5Sr1.5Fe0.5Ti0.5O4 and La0.7Sr1.3Fe0.7Ti0.3O4, respectively.

Variational study of the ground state and spin dynamics of the spin- 12 kagome antiferromagnetic Heisenberg model and its implication for herbertsmithite ZnCu3(OH)6Cl2

We find that the best RVB state of the spin-$\frac{1}{2}$ Kagome antiferromagnetic Heisenberg model(spin-$\frac{1}{2}$ KAFH) is described by a $Z_{2}$ gapped mean field ansatz, which hosts a mean field spinon dispersion very different from that of the widely studied $U(1)$ Dirac spin liquid state. However, we find that the physical spin fluctuation spectrum calculated from the Gutzwiller projected RPA(GRPA) theory above such an RVB state is actually gapless and is almost identical to that above the $U(1)$ Dirac spin liquid state. We find that such a peculiar behavior can be attributed to the unique flat band physics on the Kagome lattice, which makes the mapping between the mean field ansatz and the RVB state non-injective. We find that the spin fluctuation spectrum of the spin-$\frac{1}{2}$ KAFH is not at all featureless, but is characterized by a prominent spectral peak at about $0.25J$ around the $\mathbf{M}$ point, which is immersed in a broad continuum extending to $2.7J$. Based on these results, we argue that the spectral peak below 2 meV in the inelastic neutron scattering(INS) spectrum of Hebertsmithite ZnCu$_{3}$(OH)$_{6}$Cl$_{2}$, which has been attributed to the contribution of Cu$^{2+}$ impurity spins occupying the Zn$^{2+}$ site, should rather be understood as the intrinsic contribution from the Kagome layer. We propose to verify such a picture by measuring the Knight shift on the Cu site, rather than the O site, which is almost blind to the spin fluctuation at the $\mathbf{M}$ point as a result of the strong antiferromagnetic correlation between nearest neighboring spins on the Kagome lattice.

Spin-chain correlations in the frustrated triangular lattice material CuMnO2

The Ising triangular lattice remains the classic test-case for frustrated magnetism. Here we report neutron scattering measurements of short range magnetic order in CuMnO2, which consists of a distorted lattice of Mn3+ spins with single-ion anisotropy. Physical property measurements on CuMnO2 are consistent with 1D correlations caused by anisotropic orbital occupation. However the diffuse magnetic neutron scattering seen in powder measurements has previously been fitted by 2D Warren-type correlations. Using neutron spectroscopy, we show that paramagnetic fluctuations persist up to ∼25 meV above TN = 65 K. This is comparable to the incident energy of typical diffractometers, and results in a smearing of the energy integrated signal, which hence cannot be analysed in the quasi-static approximation. We use low energy XYZ polarised neutron scattering to extract the purely magnetic (quasi)-static signal. This is fitted by reverse Monte Carlo analysis, which reveals that two directions in the triangular layers are perfectly frustrated in the classical spin-liquid phase at 75 K. Strong antiferromagnetic correlations are only found along the b-axis, and our results hence unify the pictures seen by neutron scattering and macroscopic physical property measurements.

Microscopic spinon-chargon theory of magnetic polarons in the t−J model

The interplay of spin and charge degrees of freedom, introduced by doping mobile holes into a Mott insulator with strong anti-ferromagnetic (AFM) correlations, is at the heart of strongly correlated matter such as high-Tc cuprate superconductors. Here we capture this interplay in the strong coupling regime and propose a trial wavefunction of mobile holes in an AFM. Our method provides a microscopic justification for a class of theories which describe doped holes moving in an AFM environment as meson-like bound states of spinons and chargons. We discuss a model of such bound states from the perspective of geometric strings, which describe a fluctuating lattice geometry introduced by the fast motion of the chargon. This is demonstrated to give rise to short-range hidden string order, signatures of which have recently been revealed by ultracold atom experiments. We present evidence for the existence of such short-range hidden string correlations also at zero temperature by performing numerical DMRG simulations. To test our microscopic approach, we calculate the ground state energy and dispersion relation of a hole in an AFM, as well as the magnetic polaron radius, and obtain good quantitative agreement with advanced numerical simulations at strong couplings. We discuss extensions of our analysis to systems without long range AFM order to systems with short-range magnetic correlations.

Strong vorticity fluctuations and antiferromagnetic correlations in axisymmetric fluid equilibria

The macroscale structure and microscale fluctuation statistics of late-time asymptotic steady state flows in cylindrical geometries is studied using the methods of equilibrium statistical mechanics. The axisymmetric assumption permits an effective two-dimensional description in terms of the (toroidal) flow field $\sigma$ about the cylinder axis and the vorticity field $\xi$ that generates mixing within the (poloidal) planes of fixed azimuth. As for a number of other 2D fluid systems, extending the classic 2D Euler equation, the flow is constrained by an infinite number of conservation laws, beyond the usual kinetic energy and angular momentum. All must be accounted for in a consistent equilibrium description. It is shown that the most directly observable impact of the conservation laws is on $\sigma$, which displays interesting large-scale radius-dependent flow structure. However, unlike in some previous treatments, we find that the thermodynamic temperature is always positive. As a consequence, except for an infinitesimal boundary layer that maintains the correct (conserved) value of the overall poloidal circulation, the impact on $\xi$ resides in the statistics of the strongly fluctuating, fine-scale mixing, where it is sensitive to `antiferromagnetic' microscale correlations that help maintain the analogue of local charge neutrality. The poloidal flow is macroscopically featureless, displaying no large scale circulating jet- or eddy-like features (which typically emerge as negative temperature states in analogous Euler and quasigeostrophic equilibria).

The t−t′−t″−U Hubbard model and Fermi-level peak

Using the strong-coupling diagram technique, low-temperature spectral properties of the two-dimensional fermionic Hubbard model are considered for strong and moderate Hubbard repulsions U. The electron hopping to the nearest, second and third neighbors is taken into account with hopping constants and , respectively. The nonzero values of and lead to strong asymmetry in magnetic properties with respect to the hole and electron doping—for U = 8t strong antiferromagnetic correlations are retained up to the electron concentration , while they are destroyed completely at . When the temperature is decreased to T ≲ 0.1t, in a wide range of electron concentrations there appear narrow and intensive peaks at the Fermi level (FL) in densities of states. For U ≲ 6t the peaks are seen even at half-filling, while for larger U they arise as the FL leaves the Mott gap. The peaks are connected with a narrow band emerging at low temperatures. We identify states forming the band with spin-polaron excitations—bound states of correlated electrons and mobile spin excitations. Obtained low-temperature spectral functions are used for interpreting the peak-dip-hump structure observed in the photoemission of Nd2−xCexCuO4. In the case of hole doping, the calculated Fermi contour contains arcs near nodal points with pseudogaps near antinodal points, while for electron doping the spectral intensity is suppressed at hot spots, in agreement with experimental observations in cuprate perovskites.

Antiferromagnetic and d -wave pairing correlations in the strongly interacting two-dimensional Hubbard model from the functional renormalization group

Using the dynamical mean-field theory (DMFT) as a `booster-rocket', the functional renormalization group (fRG) can be upgraded from a weak-coupling method to a powerful computation tool for strongly interacting fermion systems. The strong local correlations are treated non-perturbatively by the DMFT, while the fRG flow can be formulated such that it is driven exclusively by non-local correlations, which are more amenable to approximations. We show that the full frequency dependence of the two-particle vertex needs to be taken into account in this approach, and demonstrate that this is actually possible -- in spite of the singular frequency dependence of the vertex at strong coupling. We are thus able to present the first results obtained from the DMFT-boosted fRG for the two-dimensional Hubbard model in the strongly interacting regime. We find strong antiferromagnetic correlations from half-filling to 18 percent hole-doping, and, at the lowest temperature we can access, a sizable $d$-wave pairing interaction driven by magnetic correlations at the edge of the antiferromagnetic regime.

Strongly correlated superconductivity

We investigate the electronic properties of the ground state of strongly correlated electron systems. We use an optimization variational Monte Carlo method for the two-dimensional Hubbard model and the three-band d-p model. The many-body wavefunction is improved and optimized by introducing variational parameters that control the correlation between electrons. The on-site repulsive Coulomb interaction U induces strong antiferromagnetic (AF) correlation. There is a crossover from weakly to strongly correlated regions as U increases. We show an idea that high-temperature superconductivity occurs as a result of this crossover in the strongly correlated region where U is greater than the bandwidth.

Quantum State Engineering of a Hubbard System with Ultracold Fermions.

Accessing new regimes in quantum simulation requires the development of new techniques for quantum state preparation. We demonstrate the quantum state engineering of a strongly correlated many-body state of the two-component repulsive Fermi-Hubbard model on a square lattice. Our scheme makes use of an ultralow entropy doublon band insulator created through entropy redistribution. After isolating the band insulator, we change the underlying potential to expand it into a half-filled system. The final many-body state realized shows strong antiferromagnetic correlations and a temperature below the exchange energy. We observe an increase in entropy, which we find is likely caused by the many-body physics in the last step of the scheme. This technique is promising for low-temperature studies of cold-atom-based lattice models.

TRILEX and GW +EDMFT approach to d -wave superconductivity in the Hubbard model

We generalize the recently introduced TRILEX approach (TRiply Irreducible Local EXpansion) to superconducting phases. The method treats simultaneously Mott and spin-fluctuation physics using an Eliashberg theory supplemented by local vertex corrections determined by a self-consistent quantum impurity model. We show that, in the two-dimensional Hubbard model, at strong coupling, TRILEX yields a $d$-wave superconducting dome as a function of doping. Contrary to the standard cluster dynamical mean field theory (DMFT) approaches, TRILEX can capture $d$-wave pairing using only a single-site effective impurity model. We also systematically explore the dependence of the superconducting temperature on the bare dispersion at weak coupling, which shows a clear link between strong antiferromagnetic (AF) correlations and the onset of superconductivity. We identify a combination of hopping amplitudes particularly favorable to superconductivity at intermediate doping. Finally, we study within $GW$+EDMFT the low-temperature $d$-wave superconducting phase at strong coupling in a region of parameter space with reduced AF fluctuations.

One-dimensional repulsive Fermi gas in a tunable periodic potential

By using unbiased continuos-space quantum Monte Carlo simulations, we investigate the ground state properties of a one-dimensional repulsive Fermi gas subjected to a commensurate periodic optical lattice (OL) of arbitrary intensity. The equation of state and the magnetic structure factor are determined as a function of the interaction strength and of the OL intensity. In the weak OL limit, Yang's theory for the energy of a homogeneous Fermi gas is recovered. In the opposite limit (deep OL), we analyze the convergence to the Lieb-Wu theory for the Hubbard model, comparing two approaches to map the continuous-space to the discrete-lattice model: the first is based on (noninteracting) Wannier functions, the second effectively takes into account strong-interaction effects within a parabolic approximation of the OL wells. We find that strong antiferromagnetic correlations emerge in deep OLs, and also in very shallow OLs if the interaction strength approaches the Tonks-Girardeau limit. In deep OLs we find quantitative agreement with density matrix renormalization group calculations for the Hubbard model. The spatial decay of the antiferromagnetic correlations is consistent with quasi long-range order even in shallow OLs, in agreement with previous theories for the half-filled Hubbard model.