Our magnetic, electrical, and thermal measurements on single-crystals of the novel Mott insulator, Sr2IrO4, reveal a novel giant magneto-electric effect (GME) arising from a frustrated magnetic/ferroelectric state whose signatures are: (1) a strongly enhanced electric permittivity that peaks near a newly observed magnetic anomaly at 100 K, (2) a large (~100%) magneto-dielectric shift that occurs near a metamagnetic transition, and (3) magnetic and electric polarization hysteresis. The GME and electric polarization hinge on a spin-orbit gapping of 5d-bands, rather than the magnitude and spatial dependence of magnetization, as traditionally accepted.
We present a new type of colossal magnetoresistance (CMR) arising from an anomalous collapse of the Mott insulating state via a modest magnetic field in a bilayer ruthenate, Ti-doped Ca$_3$Ru$_2$O$_7$. Such an insulator-metal transition is accompanied by changes in both lattice and magnetic structures. Our findings have important implications because a magnetic field usually stabilizes the insulating ground state in a Mott-Hubbard system, thus calling for a deeper theoretical study to reexamine the magnetic field tuning of Mott systems with magnetic and electronic instabilities and spin-lattic…
The Hall angle in the doped V_2O_3 is discussed on the basis of an extended Ginzburg-Landau theory of spin fluctuations. A spinon-like collective transport process beyond the ordinary quasiparticle transport theory is necessary to understand the experiment. At the same time a criticism of a quasiparticle transport theory on the basis of the fluctuation exchange (FLEX) approximation is made.
Transport and magnetic studies of Ca3Ru2O7 for temperatures ranging from 0.4 K to 56 K and magnetic fields, B, up to 45 T leads to strikingly different behavior when the field is applied along the different crystal axes. A ferromagnetic (FM) state with full spin polarization is achieved for B||a-axis, but colossal magnetoresistance is realized only for B||b-axis. For B||c-axis, Shubnikov-de Haas oscillations are observed and followed by a less resistive state than for B||a. Hence, in contrast to standard colossal magnetoresistive materials, the FM phase is the least favorable for electron hopp…
We investigate the Hall effect and the magnetoresistance of strongly correlated electron systems using the dynamical mean-field theory. We treat the low- and high-temperature limits analytically and explore some aspects of the intermediate-temperature regime numerically. We observe that a bipartite-lattice condition is responsible for the high-temperature result $σ_{xy}\sim 1/T^2$ obtained by various authors, whereas the general behavior is $σ_{xy}\sim 1/T$, as for the longitudinal conductivity. We find that Kohler's rule is neither obeyed at high nor at intermediate temperatures.
As a hallmark of electronic correlation, spin-charge interplay underlies many emergent phenomena in doped Mott insulators, such as high-temperature superconductivity, whereas the half-filled parent state is usually electronically frozen with an antiferromagnetic order that resists external control. We report on the observation of a new positive magnetoresistance that probes the staggered susceptibility of a pseudospin-half square-lattice Mott insulator built as an artificial SrIrO3/SrTiO3 superlattice. Its size is particularly large in the high-temperature insulating paramagnetic phase near th…
Using resonant inelastic x-ray scattering, we observe in the bilayer iridate Sr3Ir2O7, a spin-orbit coupling driven magnetic insulator with a small charge gap, a magnon gap of ~92 meV for both acoustic and optical branches. This exceptionally large magnon gap exceeds the total magnon bandwidth of ~70 meV and implies a marked departure from the Heisenberg model, in stark contrast to the case of the single-layer iridate Sr2IrO4. Analyzing the origin of these observations, we find that the giant magnon gap results from bond-directional pseudo-dipolar interactions that are strongly enhanced near t…
Electric field effect (EFE) controlled magnetoelectric transport in thin films of undoped and La-doped Sr$_{2}$IrO$_{4}$ (SIO) were investigated under the action of ionic liquid gating. Despite large carrier density modulation, the temperature dependent resistance measurements exhibit insulating behavior in chemically and EFE doped samples with the band filling up to 10\%. The ambipolar transport across the Mott gap is demonstrated by EFE tuning of the activation energy. Further, we observe a crossover from a negative magnetoresistance (MR) at high temperatures to positive MR at low temperatur…
We study the optical, Raman, and ac Hall response of the doped Mott insulator within the dynamical mean-field theory ($d=\infty$) for strongly correlated electron systems. The occurence of the {\it isosbectic} point in the optical conductivity is shown to be associated with the frequency dependence of the generalized charge susceptibility. We compute the Raman response, which probes the fluctuations of the "stress tensor", and show that the scattering is characterized by appreciable incoherent contributions. The calculated ac Hall constant and Hall angle also exhibit the isosbectic points. The…
Mott insulators have surprised us many times by hosting new and diverse quantum phenomena when the frozen electrons are perturbed by various stimuli. Superconductivity, metal-insulator transition, and colossal magnetoresistance induced by element substitution, pressure, and magnetic field are prominent examples. Here we report a novel phenomenon, namely giant diamagnetism, in the Mott insulator Ca2RuO4 induced by electric current. With application of 1 A/cm2 current, the strongest diamagnetism among all nonsuperconducting materials is induced as the system is tuned to a semimetallic state. The…
Coupling of charge and lattice degrees of freedom in materials can produce intriguing electronic phenomena, such as conventional superconductivity where the electrons are mediated by lattice for creating supercurrent. The Mott transition, which is a source for many fascinating emergent behaviors, is originally thought to be driven solely by correlated electrons with an Ising criticality. Recent studies on the known Mott systems have shown that the lattice degree of freedom is also at play, giving rise to either Landau or unconventional criticality. However, the underlying coupling mechanism of…
We have investigated the temperature evolution of magnetism and its interrelation with structural parameters in perovskite-based layered compound Sr$_2$IrO$_4$, which is believed to be a $J_{eff}$ = 1/2 Mott insulator. The structural distortion plays an important role in this material which induces a weak ferromagnetism in otherwise antiferromagnetically ordered magnetic state with transition temperature around 240 K. Interestingly, at low temperature below around 100 K, a change in magnetic moment has been observed. Temperature dependent x-ray diffraction measurements show sudden changes in s…
We investigate the finite temperature magnetothermoelectric response in the vicinity of a superfluid--Mott insulator quantum phase transition. We focus on the particle-hole symmetric transitions of the Bose--Hubbard model, and combine Lorentz invariance arguments with quantum Boltzmann calculations. By means of an epsilon expansion, we find that a non-vanishing thermoelectric tensor and a finite thermal conductivity are supported in this quantum critical regime. We comment on the singular Nernst effect in this problem.
This paper has been withdrawn by the authors because the results were incorrect due to the use of an impurity solver that fails at large interaction strength and above half-filling. This led, first, to the development of a new impurity solver (arXiv:1202.5814 or Phys.Rev. B 86, 085133 (2012)) and, second, to a complete revision of the thermopower results with different conclusions. Therefore a new paper on thermopower was submitted (arXiv:1209.4349) and the present one withdrawn.
The consequences of the Jahn-Teller (JT) orbital-lattice coupling for magnetism of pseudospin J_{eff}=1/2 and J_{eff}=0 compounds are addressed. In the former case, represented by Sr_2IrO_4, this coupling generates, through the so-called pseudo-JT effect, orthorhombic deformations of a crystal concomitant with magnetic ordering. The orthorhombicity axis is tied to the magnetization and rotates with it under magnetic field. The theory resolves a number of puzzles in Sr_2IrO_4 such as the origin of in-plane magnetic anisotropy and magnon gaps, metamagnetic transition, etc. In J_{eff}=0 systems, …
A zero temperature Anderson-Mott transition driven by spin disorder can be `tuned' by an applied magnetic field to achieve colossal magnetoconductance. Usually this is not possible since spin disorder by itself cannot localise a high density electron system. However, the presence of strong structural disorder can realise this situation, self consistently generating a disordered magnetic ground state. We explore such a model, constructed to understand amorphous GdSi, and highlight the emergence of a spin glass phase, Anderson-Mott signatures in transport and tunneling spectra, and unusual magne…
Giant magnetostriction in insulating magnetic materials is highly required for applications but is rarely observed. Here we show that giant magnetostriction (> 1500 ppm) can be achieved in an insulating transition metal oxide CaBaCo4O7 where the ferrimagnetic ordering at TC ~ 62 K is associated with a huge change in the lattice. Moreover, because this material is pyroelectric with a non-switchable electric polarization (P), the giant magnetostriction results in a record-breaking magnetoelectric effect - a gigantic change of electric polarization (deltaP ~ 1.6 μC/cm2) in response to the applied…
We present results on resistivity ($ρ$), magnetization ($M$), thermal conductivity ($κ$), magnetostriction ($\frac{ΔL}{L(0)}$) and specific heat ($C_{p}$) of charge-orbital ordered antiferromagnetic Nd$_{0.8}$Na$_{0.2}$MnO$_{3}$ compound. Magnetic field-induced antiferromagnetic/charge-orbital ordered insulating to ferromagnetic metallic transition leads to giant magnetothermal conductivity and magnetostriction effect. The low-temperature irreversibility behavior in $ρ$, $M$, $κ$ and $\frac{ΔL}{L(0)}$ due to field cycling together with striking similarity among the field and temperature depend…
Ca3Ru2O7 with a Mott-like transition at 48 K features different in-plane anisotropies of magnetization and magnetoresistance. Applying magnetic field along the magnetic easy-axis precipitates a spin-polarized state via a first-order metamagnetic transition, but does not lead to a full suppression of the Mott state, whereas applying magnetic field along the magnetic hard axis does, causing a resistivity reduction of three orders of magnitude. The colossal magnetoresistivity is attributed to the collapse of the orbital ordered and spin-polarized state. Evidence for a density wave is also present…
We report the structural, magnetic, exchange bias and magnetotransport effect in Sr$_{4}$Fe$_{3}$CoO$_{11}$. The material crystallizes in the orthorhombic $\textit{Cmmm}$ space group. It shows antiferromagnetic (G-type) transition (T$_{N}$ = 255 K) along with interesting temperature induced magnetization reversal (T$_{Comp.}$= 47 K measured at 100 Oe). The magnetic reversal can be elucidated considering the increased magnetocrystalline anisotropy with Co substitution. Magnetoresistance measurements shows an interesting crossover from negative to positive side at $\sim$ 100 K. The negative magn…
The electronic and magnetic properties of SrFeO$_{3-δ}$ single crystals with controlled oxygen content ($0 \leq δ\leq 0.19$) have been studied systematically by susceptibility, transport and spectroscopic techniques. An intimate correlation between the spin-charge ordering and the electronic transport behavior is found. Giant negative as well as positive magnetoresistance are observed.
We investigate the tunability of the structural, electronic and magneto transport properties of polycrystalline Sr2IrO4 sample. The extent of bifurcation of the magnetisation curves during the field cooled and zero field cooled cycles establishes that the magnetic anisotropy in the as-prepared sample is more as compared to the vacuum annealed one. Based on the behaviours of the structural parameters and the magnetic studies, our results show that the canted AFM structure is stabilised in a larger temperature range in the case of the annealed sample as compared to the as prepared one. At low te…
The magnetocaloric effect, that consists of adiabatic temperature changes in a varying external magnetic field, appears not only when the amplitude is changed, but in cases of anisotropic magnetic materials also when the direction is varied. In this article we investigate the magnetocaloric effect theoretically for the archetypical single molecule magnets Fe8 and Mn12 that are rotated with respect to a magnetic field. We complement our calculations for equilibrium situations with investigations of the influence of non-equilibrium thermodynamic cycles.
One important aspect of the magneto-structural transition in MnCoGe and related materials is the reduction in saturation magnetization from the orthorhombic to the hexagonal phase. Here, by combining an element specific magnetization probe such as x-ray magnetic circular dichroism and band structure calculations, we show that the magnetic moment instability between orthorhombic and hexagonal structures originates from a reduction in the Mn sub-lattice magnetization. The consequences of the moment instability for the magnetocaloric effect are discussed.
Magnetopological mechanics in Maxwell lattice frustrated Mott insulators
International Center for Quantum Materials, School of Physics, Peking University（北京大学物理学院量子材料国际中心）；Collaborative Innovation Center of Quantum Matter（量子物质协同创新中心）
Obtaining strong magnetoelectric couplings in bulk materials and heterostructures is an ongoing challenge. We demonstrate that manganite heterostructures of the form ${\rm (Insulator)/(LaMnO_3)_n/(CaMnO_3)_n/(Insulator)}$ show strong multiferroicity in magnetic manganites where ferroelectric polarization is realized by charges leaking from ${\rm LaMnO_3}$ to ${\rm CaMnO_3}$ due to repulsion. Here, an effective nearest-neighbor electron-electron (electron-hole) repulsion (attraction) is generated by cooperative electron-phonon interaction. Double exchange, when a particle virtually hops to its …
The effect of giant dielectric permittivity due to phase separation accompanied by charged inhomogeneities in low-doped manganites is discussed. The effect appears in the vicinity of the second-order magnetic phase transition and is caused by long-range Coulomb forces. The long-range Coulomb interaction is responsible for the formation of inhomogeneous charged states and determines their characteristic length scales. We derive the phase diagram of the inhomogeneous charged states in the framework of the phenomenological theory of phase transitions. The large value of the static dielectric func…
Uniquely in Cu2OSeO3, the Skyrmions, which are topologically protected magnetic spin vortex-like objects, display a magnetoelectric coupling and can be manipulated by externally applied electric (E) fields. Here, we explore the E-field coupling to the magnetoelectric Skyrmion lattice phase, and study the response using neutron scattering. Giant E-field induced rotations of the Skyrmion lattice are achieved that span a range of $\sim$25$^{\circ}$. Supporting calculations show that an E-field-induced Skyrmion distortion lies behind the lattice rotation. Overall, we present a new approach to Skyr…
We report the discovery of giant and anisotropic magnetoresistance due to the orbital rearrangement in a non-magnetic correlated metal. In particular, we measured the magnetoresistance under fields up to 31.4 T in the cubic Pr-based heavy fermion superconductor PrV$_2$Al$_{20}$ with a non-magnetic $Γ_3$ doublet ground state, exhibiting antiferro-quadrupole ordering below 0.7 K. For the [100] direction, we find that the high-field phase appears between 12 T and 25 T, accompanied by a large jump at 12 T in the magnetoresistance ($ΔMR \sim $ 100 $\% $) and in the anisotropic magnetoresistivity (A…
X-ray absorption near edge spectra (XANES) and magnetization of Zn doped MnV2O4 have been measured and from the magnetic measurement the critical exponents and magnetocaloric effect have been estimated. The XANES study indicates that Zn doping does not change the valence states in Mn and V. It has been shown that the obtained values of critical exponents \b{eta}, γ and δ do not belong to universal class and the values are in between the 3D Heisenberg model and the mean field interaction model. The magnetization data follow the scaling equation and collapse into two branches indicating that the…
Motivated by recent terahertz (THz) spectroscopy measurements in $α$-RuCl$_3$, we develop a theory for magnetoelectric (ME) effects in Mott insulators of $d^5$ transition metal ions in an octahedral crystal field. For $4d$ and $5d$ compounds, the relatively wide-spread orbitals favor charge fluctuations of localized electrons to neighboring ions and a significant ME effect from electronic mechanisms is expected. From a three-orbital Hubbard model with strong spin-orbit coupling, we derive the mechanisms for the electric polarization originating from virtual hopping of the localized holes carry…
The in-plane and out-of-plane magnetoresistance (MR) of single crystals of La_2CuO_4, lightly doped (x=0.03) with either Sr (La_{2-x}Sr_xCuO_4) or Li (La_2Cu_{1-x}Li_xO_4), have been measured in the fields applied parallel and perpendicular to the CuO_2 planes. Both La_{1.97}Sr_{0.03}CuO_4 and La_2Cu_{0.97}Li_{0.03}O_4 exhibit the emergence of a positive MR at temperatures (T) well below the spin glass (SG) transition temperature T_{sg}, where charge dynamics is also glassy. This positive MR grows as T->0 and shows hysteresis and memory. In this regime, the in-plane resistance R_{ab}(T,B) is d…
We present a unique example of giant magnetoelectric effect in a conventional multiferroic HoMnO3, where polarization is very large (~56 mC/m2) and the ferroelectric transition temperature is higher than the magnetic ordering temperature by an order. We attribute the uniqueness of the giant magnetoelectric effect to the ferroelectricity induced entirely by the off-center displacement of rare earth ions with large magnetic moments. This finding suggests a new avenue to design multiferroics with large polarization and higher ferroelectric transition temperature as well as large magnetoelectric e…
The presence of free spins in granular Al films is directly demonstrated by $μ$SR measurements. A Mott transition is observed by probing the increase of the spin-flip scattering rate of conduction electrons as the nano-size metallic grains are being progressively decoupled. Analysis of the magneto-resistance in terms of an effective Fermi energy shows that it becomes of the order of the grains electrostatic charging energy at a room temperature resistivity $ρ\approx 50,000~μΩ~cm$, at which a metal to insulator transition is known to exist. As this transition is approached the magneto-resistanc…
A giant magnetoelectric polarization is found in HoAl$_3$(BO$_3$)$_4$. The polarization in transverse field geometry at 70 kOe reaches 3600 $μC/m^2$ which is significantly higher than reported values of linear magnetoelectric or even multiferroic compounds. The magnetostrictive effect is also measured and compared with the magnetoelectricity. The results show that spin-lattice coupling in HoAl$_3$(BO$_3$)$_4$ is extremely strong and that the magnetic field causes a large polar distortion of the ionic positions in the unit cell.
We report on giant positive magnetoresistance effect observed in VOx thin films, epitaxially grown on SrTiO3 substrate. The MR effect depends strongly on temperature and oxygen content and is anisotropic. At low temperatures its magnitude reaches 70% in a magnetic field of 5 T. Strong electron-electron interactions in the presence of strong disorder may qualitatively explain the results. An alternative explanation, related to a possible magnetic instability, is also discussed.
We provide a possible theoretical explanation for the recently observed giant positive magnetoresistance in high mobility low density {\it quasi}-two dimensional electron and hole systems. Our explanation is based on the strong coupling of the parallel field to the {\it orbital} motion arising from the {\it finite} layer thickness and the large Fermi wavelength of the {\it quasi}-two dimensional system at low carrier densities.
We report room temperature giant baro-resistance ($\approx$128\%) in $Fe_{49}(Rh_{0.93}Pd_{0.07})_{51}$. With the application of external pressure and magnetic field the temperature range of giant baro-resistance ($\approx$600\% at 5K and 19.9 kbar and 8 Tesla) and magnetoresistance ($\approx$-85\% at 5K and 8 tesla) can be tuned from 5 K to well above room temperature. As the AFM state is stabilized at room temperature under external pressure, it shows giant room temperature magnetoresistance ($\approx$-55\%) with magnetic field. Due to coupled magnetic and latticel changes, the isothermal ch…
MBE-grown, 5 nm-thick annealed Ga0.95Mn0.05As films with Tc~90K demonstrate transition from metallic to insulating state below To~10K, where sheet resistances Rsh~h/e2 and both longitudinal Rxx and transverse Rxy components become comparable. Below metal-insulator transition we found giant anisotropic magnetoresistance (GAMR), which depends on orientation of magnetization to crystallographic axes and manifests itself in positive magnetoresistance near 50% for Rxx at T=1.7K, H//[110] crystallographic direction and parallel to current in contrast to smaller and negative magnetoresistance for H//…
We study the giant magnetoresistance of nanogranular magnets in the presence of an external magnetic field and finite temperature. We show that the magnetization of arrays of nanogranular magnets has hysteretic behaviour at low temperatures leading to a double peak in the magnetoresistance which coalesces at high temperatures into a single peak. We numerically calculate the magnetization of magnetic domains and the motion of domain walls in this system using a combined mean-field approach and a model for an elastic membrane moving in a random medium, respectively. From the obtained results, we…
A magnetization-induced rotation in the third-order nonlinear optical response is observed in out-of-plane-magnetized epitaxial EuO films. We discuss the relation of this nonlinear magneto-optical rotation to the linear Faraday rotation. It is allowed in all materials but, in contrast to the linear Faraday rotation, not affected by the reduction of the thickness of the material. Thus, the third-order magneto-optical rotation is particularly suitable for probing the magnetization of functional magnetic materials such as ultra-thin films and multilayers.
Obtaining strong magnetoelectric couplings in bulk materials and heterostructures is an ongoing challenge. We demonstrate that manganite heterostructures of the form ${\rm (Insulator)/(LaMnO_3)_n/(CaMnO_3)_n/(Insulator)}$ show strong multiferroicity in magnetic manganites where ferroelectric polarization is realized by charges leaking from ${\rm LaMnO_3}$ to ${\rm CaMnO_3}$ due to repulsion. Here, an effective nearest-neighbor electron-electron (electron-hole) repulsion (attraction) is generated by cooperative electron-phonon interaction. Double exchange, when a particle virtually hops to its …
The results of dc magnetization, electrical and magnetoresistance and heat capacity measurements (2-300 K) on Tb7Rh3, crystallizing in Th7Fe3-type hexagonal structure, are reported. In this compound, magnetic ordering sets in around 90 K with additional transitions at low temperatures and the temperature coefficient of resistivity (R), dR/dT, is negative over a wide temperature range in the paramagnetic state. The present magnetization results reveal that this compound is apparently characterized by rich features in the magnetic-field-temperature phase diagram. A point of major emphasis is tha…
In solid state physics, giant magnetoresistance is the large change in electrical resistance due to an external magnetic field. Here we show that giant magnetoresistance is possible in a spin chain composed of weakly interacting layers of strongly coupled spins. This is found for all system sizes even down to a minimal system of four spins. The mechanism driving the effect is a mismatch in the energy spectrum resulting in spin excitations being reflected at the boundaries between layers. This mismatch, and thus the current, can be controlled by external magnetic fields resulting in giant magne…
Using high resolution neutron diffraction and capacitance dilatometry we show that the thermal evolution of the helimagnetic state in CoMnSi is accompanied by a change in inter-atomic distances of up to 2%, the largest ever found in a metallic magnet. Our results and the picture of competing exchange and strongly anisotropic thermal expansion that we use to understand them sheds light on a new mechanism for large magnetoelastic effects that does not require large spin-orbit coupling.
The nature of the charge order in the charge frustrated compound LuFe$_2$O$_4$ and its effect on magnetocapacitance were examined on the basis of first-principles electronic structure calculations and Monte Carlo simulations of electrostatic energy. Our work shows that two different types of charge order of almost equal stability (i.e., $\sqrt{3}\times \sqrt{3}$ and chain types) occur in the W-layers of LuFe$_2$O$_4$, and that the ground state of LuFe$_2$O$_4$ has a ferrielectric arrangement of the W-layers with $\sqrt{3}\times \sqrt{3}$ charge order. The giant magnetocapacitance effect of LuF…
We synthesized nonmagnetic PtBi$_2$ single crystals and observed a giant linear magneto-resistance (MR) up to 684\% under a magnetic field $μ_0H$ = 15 T at $T$ = 2 K. The linear MR decreases with increasing temperature, but it is still as large as 61\% under $μ_0H$ of 15 T at room temperature. Such a giant linear MR is unlikely to be described by the quantum model as the quantum condition is not satisfied. Instead, we found that the slope of MR scales with the Hall mobility, and it can be well explained by a classical disorder model.
We report on the magnetotransport properties of a prototype Mott insulator/band insulator perovskite heterojunction in magnetic fields up to 31 T and at temperatures between 360 mK and 10 K. Shubnikov-de Haas oscillations in the magnetoresistance are observed. The oscillations are two-dimensional in nature and are interpreted as arising from either a single, spin-split subband or two subbands. In either case, the electron system that gives rise to the oscillations represents only a fraction of the electrons in the space charge layer at the interface. The temperature dependence of the oscillati…
