Charge-ordered System Research Articles

The impact of Rashba spin-orbit coupling in charge-ordered systems

We study the impact of the Rashba spin–orbit coupling (RSOC) on the stability of charge-density wave (CDW) in systems with large electron-phonon coupling (EPC). Here, the EPC is considered in the framework of the Holstein model at the half-filled square lattice. We obtain the phase diagram of the Rashba–Holstein model using the Hartree–Fock mean-field theory, and identify the boundaries of the CDW and Rashba metal phases. We notice that the RSOC disfavors the CDW phase, driving the system to a correlated Rashba metal. Also, we employ a cluster perturbation theory (CPT) approach to investigate the phase diagram beyond the Hartree–Fock approximation. The quantum correlations captured by CPT indicate that the RSOC is even more detrimental to CDW than previously anticipated. That is, the Rashba metal region is observed to be expanded in comparison to the mean-field case. Additionally, we investigate pairing correlations, and the results further strengthen the identification of critical points.

Intersite Coulomb Interactions in Charge-Ordered Systems.

Using abinitio approaches for extended Hubbard interactions coupled to phonons, we reveal that the intersite Coulomb interaction plays important roles in determining various distinctive phases of the paradigmatic charge-ordered materials of Ba_{1-x}K_{x}AO_{3} (A=Bi and Sb). We demonstrated that all their salient doping dependent experiment features such as breathing instabilities, anomalous phonon dispersions, and transition between charge-density wave and superconducting states can be accounted for very well if self-consistently obtained nearest neighbor Hubbard interactions are included, thus establishing a minimal criterion for reliable descriptions of spontaneous charge orders in solids.

Ferroelectricity in Charge-Ordering Crystals with Centrosymmetric Lattices

The switchability between the two ferroelectric (FE) states of an FE material makes FEs widely used in memories and other electronic devices. However, for conventional FEs, its FE switching only occurs between the two FE states whose spatial inversion symmetry is broken. The search for FE materials is therefore subject to certain limitations. We propose a new type of FEs whose FE states still contain spatial inversion centers. The change in polarization of this new type of FEs originates from electronic transfer between two centrosymmetric FE states under an external electric field. Taking BaBiO3 as an example, we show that charge-ordering systems can be a typical representative of this new type of FEs. Moreover, unlike traditional ferroelectrics, the change in polarization in this new type of FEs is quantum in nature with the direction dependent on the specific FE transition path. Our work therefore not only extends the concept of FEs but may also open up a new way to find multiferroics.

Strain dependent spin-blockade effect realization in the charge-disproportionated SrCoO2.5 thin films

The spin-blockade phenomena occur in the charge-ordered systems because of the non-conservation of the spin-states of the charges across the charge hopping process. Here, we have investigated the validation of the spin-blockade phenomena in a different kind of charge-ordered system, viz. charge-disproportionated SrCoO2.5 thin film, where O-2p hole is the key parameter for such charge-ordering. It is observed with the help of the polarization-dependent O K-edge x-ray absorption spectroscopy that the spin-blockade increases with the decrease in charge-disproportionation vis-à-vis O-2p hole density in the SrCoO2.5 films. The spin-blockade has been realized in terms of the lowest energy charge fluctuation energetics in the SrCoO2.5 films. Our results provide a fundamental understanding of the spin-blockade phenomena in both the usual charge-ordered and unusual charge-disproportionated systems, which would lead to a path forward toward novel material designing.

Charge order textures induced by non-linear couplings in a half-doped manganite

The self-organization of strongly interacting electrons into superlattice structures underlies the properties of many quantum materials. How these electrons arrange within the superlattice dictates what symmetries are broken and what ground states are stabilized. Here we show that cryogenic scanning transmission electron microscopy (cryo-STEM) enables direct mapping of local symmetries and order at the intra-unit-cell level in the model charge-ordered system Nd1/2Sr1/2MnO3. In addition to imaging the prototypical site-centered charge order, we discover the nanoscale coexistence of an exotic intermediate state which mixes site and bond order and breaks inversion symmetry. We further show that nonlinear coupling of distinct lattice modes controls the selection between competing ground states. The results demonstrate the importance of lattice coupling for understanding and manipulating the character of electronic self-organization and that cryo-STEM can reveal local order in strongly correlated systems at the atomic scale.

Analysis of Glass Behavior of Lu2Fe3O7 with Distributed Equivalent Circuit Model

We report an analysis of the dielectric glasslike state of the spin- and charge-ordered system Lu2Fe3O7, which has structural and physical properties analogous to those of the electronic ferroelect...

Intertwined chiral charge orders and topological stabilization of the light-induced state of a prototypical transition metal dichalcogenide

The fundamental idea that the constituents of interacting many body systems in complex quantum materials may self-organise into long range order under highly non-equilibrium conditions leads to the notion that entirely new and unexpected functionalities might be artificially created. However, demonstrating new emergent order in highly non-equilibrium transitions has proven surprisingly difficult. In spite of huge recent advances in experimental ultrafast time-resolved techniques, methods that average over successive transition outcomes have so far proved incapable of elucidating the emerging spatial structure. Here, using scanning tunneling microscopy, we report for the first time the charge order emerging after a single transition outcome initiated by a single optical pulse in a prototypical two-dimensional dichalcogenide 1T-TaS2. By mapping the vector field of charge displacements of the emergent state, we find surprisingly intricate, long-range, topologically non-trivial charge order in which chiral domain tiling is intertwined with unpaired dislocations which play a crucial role in enhancing the emergent states’ remarkable stability. The discovery of the principles that lead to metastability in charge-ordered systems opens the way to designing novel emergent functionalities, particularly ultrafast all-electronic non-volatile cryo-memories.

Langevin approach to lattice dynamics in a charge-ordered polaronic system

We use a Langevin approach to treat the finite temperature dynamics of displacement variables in the half-filled spinless Holstein model. Working in the adiabatic regime we exploit the smallness of the adiabatic parameter to simplify the memory effects and estimate displacement costs from an "instantaneous" electronic Hamiltonian. We use a phenomenological damping rate, and uncorrelated thermal noise. The low temperature state has checkerboard charge order (CO) and the Langevin scheme generates equilibrium thermodynamic properties that accurately match Monte Carlo results. It additionally yields the dynamical structure factor, $D({\bf q}, \omega)$, from the displacement field $x({\bf r}, t)$. We observe four regimes with increasing temperature, $T$, classified in relation to the charge ordering temperature, $T_c$, and the `polaron formation' temperature $T_P$, with $ T_c \ll T_P$. For $T \ll T_c$ the oscillations are harmonic, leading to dispersive phonons, with increasing $T$ bringing in anharmonic, momentum dependent, corrections. For $T \sim T_c$, thermal tunneling events of the $x({\bf r})$ field occur, with a propagating `domain' pattern at wavevector ${\bf q} \sim (\pi, \pi)$ and low energy weight in $D({\bf q}, \omega)$. When $T_c < T < T_P$, the disordered polaron regime, domain structures vanish, the dispersion narrows, and low energy weight is lost. For $T \gtrsim T_P$ we essentially have uncorrelated local oscillations. We propose simple models to analyse this rich dynamics.

The Importance of Topological Defects in Photoexcited Phase Transitions Including Memory Applications

Photoinduced phase transitions have become a very important field of study with the advent of diverse time-resolved experimental techniques whose time resolution matches the electron, lattice, and spin relaxation dynamics associated with elementary excitations in quantum materials. Most techniques currently available rely on stroboscopic data-averaging over multiple transition outcomes. However, each time a transition takes place, fluctuations close to the time of the transition ensure that the phase transition outcome is different, with the emergence of different topological defect textures. In this paper, we briefly review the non-perturbative processes in selected charge-ordered quantum systems and the methods for their observation with different time-resolved techniques and scanning tunneling microscopy, which avoids the problem of averaging. The topological defect dynamics are seen to play an essential role in stabilizing emergent states in non-equilibrium transitions, appearing on different timescales as well as determining the emergent properties of the system. The phenomena are fundamentally important for understanding the fabric of matter in the Universe, as well as for possible applications in non-volatile memory devices.

Metastable Superconductivity in Two-Dimensional IrTe2 Crystals.

Two-dimensional (2D) materials exhibit unusual physical and chemical properties that are attributed to the thinning-induced modification of their electronic band structure. Recently, reduced thickness was found to dramatically impact not only the static electronic structure, but also the dynamic ordering kinetics. The ordering kinetics of first-order phase transitions becomes significantly slowed with decreasing thickness, and metastable supercooled states can be realized by thinning alone. We therefore focus on layered iridium ditelluride (IrTe2), a charge-ordering system that is transformed into a superconductor by suppressing its first-order transition. Here, we discovered a persistent superconducting zero-resistance state in mechanically exfoliated IrTe2 thin flakes. The maximum superconducting critical temperature ( Tc) was identical to that which is chemically optimized, and the emergent superconductivity was revealed to have a metastable nature. The discovered robust metastable superconductivity suggests that 2D material is a new platform to induce, control, and functionalize metastable electronic states that are inaccessible in bulk crystals.

Coexistence of magnetic order and valence fluctuations in the Kondo lattice systemCe2Rh3Sn5

We report on the electronic band structure, structural, magnetic and thermal properties of Ce$_2$Rh$_3$Sn$_5$. Ce $L_{\mathrm{III}}$-edge XAS spectra give direct evidence for an intermediate valence behaviour. Thermodynamic measurements reveal magnetic transitions at $T_{\mathrm{N1}}\approx$ 2.9 K and $T_{\mathrm{N2}}\approx$ 2.4 K. Electrical resistivity shows behaviour typical for Kondo lattices. The coexistence of magnetic order and valence fluctuations in a Kondo lattice system we attribute to a peculiar crystal structure in which Ce ions occupy two distinct lattice sites. Analysis of the structural features of Ce$_2$Rh$_3$Sn$_5$, together with results of electronic band structure calculations and thermodynamic data indicate that Ce2 ions are in an intermediate valence state with the ground state electronic configuration close to 4$f^0$, whereas Ce1 ions are trivalent (4$f^1$) and contribute to the low temperature magnetic ordering. Thus, our joined experimental and theoretical investigations classify Ce$_2$Rh$_3$Sn$_5$ as a multivalent charge-ordered system.

Photoinduced ultrafast charge-order melting: Charge-order inversion and nonthermal effects

The effect of photoexcitation is studied for a system with checkerboard charge order induced by displacements of ligands around a metal site. The motion of the ligands is treated classically and the electronic charges are simplified to two-level molecular bond charges. The calculations are done for a checkerboard charge-ordered system with about 100 000 ligand oscillators coupled to a fixed-temperature bath. The initial photoexcitation is followed by a rapid decrease in the charge-order parameter within 50–100 femtoseconds while leaving the correlation length almost unchanged. Depending on the fluence, a complete melting of the charge order occurs in less than a picosecond. While for low fluences, the system returns to its original state, for full melting, it recovers to its broken-symmetry state leading to an inversion of the charge order. Finally, for small long-range interactions, recovery can be slow due to domain formation.

Neutron and magnetic studies ofLa0.7Sr0.3Mn1−xCrxO3(x≤0.7): A homogeneous charge-ordered system

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Strong enhancement of the ferromagnetic phase and local order in Ru substituted manganites studied by EXAFS and dc magnetization measurements

We report extended X-ray absorption fine structure (EXAFS) and dc magnetization measurements performed on (La1-xCax) (Mn1-yRuy)O3 samples (x = 0.37 and 0.75 and y = 0.03 or 0.08).In the nanoscale phase inhomogeneity scenario characteristic of these complex oxides, we compare the effects induced by the partial substitution of Mn with mixed valence non-Jahn-Teller Ru5+ and at most very weak Jahn-Teller Ru4+ ions with those induced by the already studied analogous substitutions of Mn with non-Jahn-Teller Cr3+ or Ni2+ or Jahn-Teller Cu2+.We find evidence both from dc magnetization and EXAFS that the ruthenium doping induces a huge effect, clearly enhancing (more efficiently than is the case for the other dopants) the double exchange effect and consequently the metallic/ferromagnetic phase and the local structural order at the expenses of the charge-ordered phase component. In the x = 0.75 long-range charge-ordered system these effects are much more evident, as expected, while for x = 0.37 the magnetic ion partial substitution does not significantly modify the metal-insulator and ferromagnetic transitions, already present in the parent compound.

Ultrafast electronic photoinduced phase transition in a two-dimensional charge-ordering system

We investigate the ground- and excited-state properties of a two-dimensional charge-ordering system, and theoretically demonstrate that multielectron excitations by one photon occur substantially as a result of frustration effects. These multielectron excitations are naturally regarded as domain excitations, which involve a simultaneous excitation of a part of the system lattice. Furthermore, we show that such domain excitations not only suppress the original charge-ordering phase strongly but also enhance another phase of charge ordering. As a result of such a global change, the overall photoinduced optical conductivity spectra are also modified drastically from the original spectrum, with the modified spectra exhibiting midgap and gapless features.

Magnetic Field Effect in One-Dimensional Charge Ordering Systems

We study the effects of an external magnetic field on charge ordering in the one-dimensional extended Hubbard model at quarter filling by the quantum Monte Carlo method. We find that the Zeeman coupling enhances the charge order correlation, which is prominent when the system is located in the critical regime near the charge ordering transition at zero magnetic field. This behavior is interpreted in terms of the crossover to the fully spin-polarized limit where the model is exactly solvable. Furthermore, by incorporating the interchain Coulomb repulsion, we show that the charge-ordering transition temperature is increased by the magnetic field. We also discuss the relevance of our results to magnetoresistance effects observed in molecular conductors.

Pressure-temperature phase diagram of a charge-ordered organic conductor studied byC13NMR

We performed $^{13}\mathrm{C}$ NMR measurements on the quasi-one-dimensional (Q1D) charge-ordered system $(\mathrm{DI}\ensuremath{-}DCNQI{)}_{2}\mathrm{Ag}$ under ambient and applied pressure to clarify the pressure-temperature phase diagram. For pressures up to 15 kbar, the NMR spectra exhibit complicated splitting at low temperatures, indicating a ``generalized 3D Wigner crystal'' state. In this pressure region, we find that increased pressure causes a decrease in the charge disproportionation ratio, along with a decrease in the transition temperature of the generalized 3D Wigner crystal. In the high-pressure region, near 20 kbar, where a 1D confined liquid crosses over to a 3D Fermi liquid at high temperatures, the ground state is replaced by a nonmagnetic insulating state that is qualitatively different from the generalized 3D Wigner crystal.

Charge-Cluster Glass: Electrons Struggle by Frustration

Systematic investigation of glass formation in molecular charge-ordering systems has clarified the importance of geometrical frustration. In these materials, by kinetically preventing charge order “crystallization”, a new state called charge-cluster glass is observed.

Interplay between Charge and Magnetic Orderings in YbPd

The pressure-temperature phase diagram of an intermediate-valence compound YbPd was revealed via simultaneous ac-calorimetry and electrical resistivity measurements. Two successive structural phase transition temperatures, $T_1$ = 125 K and $T_2$ = 110 K, are found to decrease with increasing pressure. The magnetic ordering transition at $T_{\rm N} ~sim$ 1.9 K decreases monotonically up to 1.7 GPa and disappears discontinuously at $P_{\rm c} sim$ 1.9 GPa, where the structural phase transition at $T_2$ is also suppressed. At $P_{\rm c}$, enhancement of the effective mass and residual resistivity are observed. Another probable magnetic phase transition, however, is found to take place at $T_{\rm ML} sim$0.3 K and smoothly varies even when crossing $P_{\rm c}$. Structural phase transitions at ambient pressure were also studied by a single crystal X-ray diffraction measurement. Below $T_2$, a tetragonal lattice distortion with doubling of the unit cell along the c-axis is observed, and thus there are two inequivalent Yb-sites below $P_{\rm c}$. These results indicate that one Yb-site, having larger valence configuration and thus smaller Kondo temperature, orders at $T_{\rm N}$. The other phase transition at $T_{\rm ML}$ seems to couple to the crystal structure for $T_2 < T < T_1$. YbPd is a unique system exhibiting magnetic orderings in metallic charge-ordered Yb systems.

Anisotropy-induced crossover from Drude conductivity to charge-density-wave excitations in a stripe-type charge-ordered manganite

The half-doped Pr${}_{0.5}$Sr${}_{0.5}$MnO${}_{3}$ (PSMO) manganite represents a unique stripe type of charge orbital order that induces transport and magnetic anisotropy. Low-energy charge dynamics in PSMO (110) epitaxial film were investigated along and across two dissimilar in-plane orthogonal axes, [1-10] and [001], by recording the complex refractive index in the energy range of 1--7 meV. We report a novel observation of a gradual crossover from Drude-like metallic conductivity to charge-density-wave (CDW)--like collective excitations as the polarized terahertz excitation field is swept across the orthogonal in-plane axes. This is a rare manifestation of a CDW mode in a highly conducting stripe-type charge-ordered (CO) system, which is fundamentally different from the CDW modes of checkerboard CO. Interestingly, the contrasting charge dynamics along orthogonal in-plane axes form an intrinsic electronic switch, apparently a consequence of the unique CO of PSMO.