arXiv subjects

Long-Qing Chen

Publications and source records attributed to Long-Qing Chen.

At least 91 records · Page 5Linked to original sources

arXiv2020

Landau theory of metal-insulator transition in VO$_\text{2}$ doped with metal ions

Metal-ion doping can effectively regulate the metal-insulator transition temperature in $\mathrm{VO}_2$. Experiments found that the pentavalent and hexavalent ion doping dramatically reduces the transition temperature while the trivalent ion doping increases the transition temperature and induces intermediate phases. Based on the phase-field model of the metal-insulator transition in $\mathrm{VO}_2$ we developed previously, we formulate a Landau potential of the metal-ion-doped $\mathrm{VO}_2$ taking account of the effects of doping on the electron correlation and lattice structure. The effect of metal-ion doping on the lattice structure is accounted for in a phenomenological way. Using the Landau potential, we calculate the temperature-dopant-concentration phase diagrams of $\mathrm{VO}_2$ doped with various metal ions consistent with the experiments and provide explanation to the different behaviors of different metal-ion doping. The phenomenological theory can provide estimations of phase diagrams of $\mathrm{VO}_2$ doped with other metal ions.

cond-mat.mtrl-sci↗

arXiv2020

Transient Electronic Phase Separation During Metal-Insulator Transitions

From thermodynamic analysis we demonstrate that during metal-insulator transitions in pure matters, a nonequilibrium homogeneous state may be unstable against charge density modulations with certain wavelengths, and thus evolves to the equilibrium phase through transient electronic phase separation. This phase instability occurs as two inequalities between the first and the second derivatives of the free energy with respect to the order parameter are fulfilled. The dominant wavelength of the modulated phase is also derived. The computer simulation further confirms the theoretical derivation. Employing the pre-established phase-field model of VO$_2$, we show that this transient electronic phase separation may take place in VO$_2$ upon photoexcitation.

cond-mat.str-el↗

arXiv2020

Unexpected Giant Microwave Conductivity in a Nominally Silent BiFeO3 Domain Wall

Nanoelectronic devices based on ferroelectric domain walls (DWs), such as memories, transistors, and rectifiers, have been demonstrated in recent years. Practical high-speed electronics, on the other hand, usually demand operation frequencies in the giga-Hertz (GHz) regime, where the effect of dipolar oscillation is important. In this work, an unexpected giant GHz conductivity on the order of 103 S/m is observed in certain BiFeO3 DWs, which is about 100,000 times greater than the carrier-induced dc conductivity of the same walls. Surprisingly, the nominal configuration of the DWs precludes the ac conduction under an excitation electric field perpendicular to the surface. Theoretical analysis shows that the inclined DWs are stressed asymmetrically near the film surface, whereas the vertical walls in a control sample are not. The resultant imbalanced polarization profile can then couple to the out-of-plane microwave fields and induce power dissipation, which is confirmed by the phase-field modeling. Since the contributions from mobile-carrier conduction and bound-charge oscillation to the ac conductivity are equivalent in a microwave circuit, the research on local structural dynamics may open a new avenue to implement DW nano-devices for RF applications.

cond-mat.mtrl-sci↗

arXiv2019

Enhanced flexoelectricity at reduced dimensions revealed by mechanically tunable quantum tunnelling

Flexoelectricity is a universal electromechanical coupling effect whereby all dielectric materials polarize in response to strain gradients. In particular, nanoscale flexoelectricity promises exotic phenomena and functions, but reliable characterization methods are required to unlock its potential. Here, we report anomalous mechanical control of quantum tunnelling that allows for characterizing nanoscale flexoelectricity. By applying strain gradients with an atomic force microscope tip, we systematically polarize an ultrathin film of otherwise nonpolar SrTiO$_{3}$, and simultaneously measure tunnel current across it. The measured tunnel current exhibits critical behaviour as a function of strain gradients, which manifests large modification of tunnel barrier profiles via flexoelectricity. Further analysis of this critical behaviour reveals significantly enhanced flexocoupling strength in ultrathin SrTiO$_{3}$, compared to that in bulk, rendering flexoelectricity more potent at the nanoscale. Our study not only suggests possible applications exploiting dynamic mechanical control of quantum effect, but also paves the way to characterize nanoscale flexoelectricity.

cond-mat.mtrl-sci↗

arXiv2019

Periodicity doubling cascades: direct observation in ferroelastic materials

Very sensitive responses to external forces are found near phase transitions. However, phase transition dynamics and pre-equilibrium phenomena are difficult to detect and control. We have directly observed that the equilibrium domain structure following a phase transition in BaTiO3, a ferroelectric and ferroelastic material, is attained by halving of the domain periodicity, sequentially and multiple times. The process is reversible, displaying periodicity doubling as temperature is increased. This observation is backed theoretically and can explain the fingerprints of domain period multiplicity observed in other systems, strongly suggesting this as a general model for pattern formation during phase transitions in ferroelastic materials.

cond-mat.mtrl-sci↗

arXiv2018

Isothermal current-driven insulator-to-metal transition in VO$_\text{2}$ through strong correlation effect

Electric current has been experimentally demonstrated to be able to drive the insulator-to-metal transition (IMT) in VO$_2$. The main mechanisms involved are believed to be the Joule heating effect and the strong electron-correlation effect. These effects are often entangled with each other in experiments, which complicates the understanding of the essential nature of the observations. We formulate a phase-field model to investigate theoretically in mesoscale the pure correlation effect brought by the current on the IMT in VO$_2$, i.e., the isothermal process under the current. We find that a current with a large density ($\sim 10^1$ nA/nm$^2$) induces a few-nanosecond ultrafast switch in VO$_2$, in agreement with the experiment. The temperature-current phase diagram is further calculated, which reveals that the current may induce the M2 phase at low temperatures. The current is also shown capable of driving domain walls to move. Our work may assist related experiments and provide guidance to the engineering of VO$_2$-based electric switching devices.

cond-mat.mtrl-sci↗

arXiv2018

Phase-field modeling of non-isothermal grain coalescence in the unconventional sintering techniques

A thermodynamically consistent phase-field model is developed to study the non-isothermal grain coalescence during the sintering process, with a potential application to the simulation in unconventional sintering techniques, e.g. spark plasma sintering, field-assisted sintering, and selective laser sintering, where non-equilibrium and high temperature gradient exist. In the model, order parameters are adopted to represent the bulk and atmosphere/pore region, as well as the crystallographic orientations. Based on the entropy analysis, the temperature-dependent free energy density is developed, which includes contributions from the internal energy (induced by the change of temperature and order parameters) and the order parameter related configurational entropy. The temperature-dependent model parameters are determined by using the experimental data of surface and grain boundary energies and interface width. From laws of thermodynamics, the kinetics for the order parameters and the order-parameter-coupled heat transfer are derived. The model is numerically implemented by the finite element method. Grain coalescence from two identical particles shows that non-isothermal condition leads to the unsymmetric morphology and curved grain boundary due to the gradients of on-site surface and grain-boundary energies induced by the local temperature inhomogeneity. More simulations on the non-isothermal grain coalescence from two non-identical and multiple particles present the temporal evolution of grain shrinkage/growth, neck growth, and porosity, demonstrating the capability and versatility of the model. It is anticipated that the work could provide a contribution to the research community of unconventional sintering techniques that can be used to model the non-isothermal related microstructural features.

cond-mat.mtrl-sci↗

arXiv2018

Dynamics of liquid crystal on hexagonal lattice

Nematic liquid crystal (LC) molecules adsorbed on two dimensional materials are aligned along the crystal directions of the hexagonal lattice. It was demonstrated that short electric pulses can reorient the aligned LC molecules in the preferred armchair direction of hexagonal boron nitride (h-BN). Several states with a variety of colors were obtained by changing the direction and strength of the electric pulses. The ab initio calculations based on density functional theory was carried out to determine the favorable adsorption configurations of the LC molecules on the h-BN surface. A non-volatile display, in which pixel resolution can be determined by grains of hexagonal surface, is proposed, which can offer a pathway towards dynamic high-quality pixels with low power consumption, and could define a new paradigm for all non-volatile display applications.

cond-mat.soft↗

arXiv2018

A new symmetry-based framework for discovering minimum energy pathways

Physical systems evolve from one state to another along paths of least energy barrier. Without a priori knowledge of the energy landscape, multidimensional search methods aim to find such minimum energy pathways between the initial and final states of a kinetic process. However in many cases, the user has to repeatedly provide initial guess paths, thus ensuring that the reliability of the final result is heavily user-dependent. Recently, the idea of "distortion symmetry groups" as a complete description of the symmetry of a path has been introduced. Through this, a new framework is enabled that provides a powerful means of classifying the infinite collection of possible pathways into a finite number of symmetry equivalent subsets, and then exploring each of these subsets systematically using rigorous group theoretical methods. The method is shown to lead to the discovery of new, previously hidden pathways for the case studies of bulk ferroelectric switching and domain wall motion in proper and improper ferroelectrics, as well as in multiferroic switching. This approach is applicable to a wide variety of physical phenomena ranging from structural, electronic and magnetic distortions, diffusion, and phase transitions in materials.

cond-mat.mtrl-sci↗

arXiv2017

First-Principles Thermodynamic Theory of Seebeck Coefficients

Thermoelectric effects, measured by the Seebeck coefficients, refer to the phenomena in which a temperature difference or gradient imposed across a thermoelectric material induces an electrical potential difference or gradient, and vice versa, enabling the direct conversion of thermal and electric energies. All existing understanding and first-principles calculations of Seebeck coefficients have been based on the Boltzmann kinetic transport theory. Here we demonstrate that the Seebeck coefficient is a well-defined thermodynamic quantity that can be determined from the change in the chemical potential of electrons induced by the temperature change and thus can be efficiently computed solely based on the electronic density of states through first-principles calculations at different temperatures. The proposed approach is demonstrated using the prototype PbTe and SnSe thermoelectric materials. The proposed thermodynamic approach dramatically simplifies the calculations of Seebeck coefficients, making it possible to search for high performance thermoelectric materials using high-throughput first-principles calculations.

cond-mat.mtrl-sci↗

arXiv2017

Switchable polar spirals in tricolor oxide superlattices

There are increasing evidences that ferroelectric states at the nanoscale can exhibit fascinating topological structures including polar vortices and skyrmions,akin to those observed in the ferromagnetic systems. Here we report the discovery of a new type of polar topological structure,ordered array of nanoscale spirals in the tricolor ferroelectric superlattice system via phase field simulations. This polar spiral structure is composed of fine ordered semivortex arrays with vortex cores forming a wavy distribution. It is demonstrated that this tricolor system has an ultrahigh Curie temperature of 1000 K and a temperature of 650 K for the phase transformation from spiral structure to inplane orthorhombic domain structure, showing a greatly enhanced thermal stability than the recently discovered polar vortex lattices in the superlattice system. Moreover, the spiral structure has a net inplane polarization that could be switched by an experimentally feasible irrotational inplane field. The switching process involves a metastable vortex state, and is fully reversible.

cond-mat.mes-hall↗

arXiv2017

Blowing Polar Skyrmion Bubbles in Oxide Superlattices

Particle-like topological structures such as skyrmions and vortices have garnered ever-increasing interests due to the rich physical insights and potential broad applications. Here we discover the reversible switching between polar skyrmion bubbles and ordered vortex arrays in ferroelectric superlattices under an electric field, reminiscent of the Plateau-Raleigh instability in fluid mechanics. Electric field phase diagram is constructed, showing wide stability window for the observed polar skyrmions. This study is a demonstration for the computational design of ferroelectric topological structures and field-induced topological phase transitions.

cond-mat.mes-hall↗

arXiv2017

Mechanical Switching of Nanoscale Multiferroic Phase Boundaries

Tuning the lattice degree of freedom in nanoscale functional crystals is critical to exploit the emerging functionalities such as piezoelectricity, shape-memory effect, or piezomagnetism, which are attributed to the intrinsic lattice-polar or lattice-spin coupling. Here it is reported that a mechanical probe can be a dynamic tool to switch the ferroic orders at the nanoscale multiferroic phase boundaries in BiFeO 3 with a phase mixture, where the material can be reversibly transformed between the "soft" tetragonal-like and the "hard" rhombohedrallike structures. The microscopic origin of the nonvolatile mechanical switching of the multiferroic phase boundaries, coupled with a reversible 180° rotation of the in-plane ferroelectric polarization, is the nanoscale pressure-induced elastic deformation and reconstruction of the spontaneous strain gradient across the multiferroic phase boundaries. The reversible control of the room-temperature multiple ferroic orders using a pure mechanical stimulus may bring us a new pathway to achieve the potential energy conversion and sensing applications.

cond-mat.mtrl-sci↗

arXiv2017

Controlled manipulation of oxygen vacancies using nanoscale flexoelectricity

Oxygen vacancies, especially their distribution, are directly coupled to the electromagnetic properties of oxides and related emergent functionalities that have implication in device applications. Here using a homoepitaxial strontium titanate thin film, we demonstrate a controlled manipulation of the oxygen vacancy distribution using the mechanical force from a scanning probe microscope tip. By combining Kelvin probe force microscopy imaging and phase-field simulations, we show that oxygen vacancies can move under a stress-gradient-induced depolarisation field. When tailored, this nanoscale flexoelectric effect enables a controlled spatial modulation. In motion, the scanning probe tip thereby deterministically reconfigures the spatial distribution of vacancies. The ability to locally manipulate oxygen vacancies on-demand provides a tool for the exploration of mesoscale quantum phenomena, and engineering multifunctional oxide devices.

cond-mat.str-el↗

arXiv2017

A First-principles approach to predict Seebeck coefficients: Application to La3-xTe4

Theoretical descriptions of the Seebeck coefficient in terms of the differential electrical conductivity given by Cutler and Mott is the foundation of later works in terms of transmission function from the thermoelectric transport theory. On the other hand, recent studies in the literature have shown the relation between the Seebeck coefficient and chemical potential of electrons. In this work, this relation is rigorously derived from fundamental thermodynamics, and an formalism for the parameter-free calculation of the Seebeck coefficient based on the electronic density-of-states from first-principles calculations is presented. Numerical results are given using the n-type La3-xTe4 thermoelectric material as the prototype. With the rigid band approximation, the calculated temperature dependences of the Seebeck coefficients of La3-xTe4 as a function of carrier concentration show excellent agreements with experimental data.

cond-mat.mtrl-sci↗

arXiv2017

Strain induced incommensurate phases in hexagonal manganites

An incommensurate phase refers to a solid state in which the period of a superstructure is incommensurable with the primitive unit cell. Recently the incommensurate phase is induced by applying an in-plane strain to hexagonal manganites, which demonstrates single chiral modulation of six domain variants. Here we employ Landau theory in combination with the phase-field method to investigate the incommensurate phase in hexagonal manganites. It is shown that the equilibrium wave length of the incommensurate phase is determined by temperature and the magnitude of the applied strain, and a temperature-strain phase diagram is constructed for the stability of the incommensurate phase. Temporal evolution of domain structures reveals that the applied strain not only produces the force pulling the vortices and anti-vortices in opposite directions, but also results in the creation and annihilation of vortex-antivortex pairs.

cond-mat.mtrl-sci↗

arXiv2017

Three-dimensional vortex structures and dynamics in hexagonal manganites

Hexagonal manganites REMnO3 (RE, rare earths) have attracted significant attention due to their potential applications as multiferroic materials and the intriguing physics associated with the topological defects. The two-dimensional (2D) and 3D domain and vortex structure evolution of REMnO3 is predicted using the phase-field method based on a thermodynamic potential constructed from first-principles calculations. In 3D spaces, vortex lines show three types of topological changes, i.e. shrinking, coalescence, and splitting, with the latter two caused by the interaction and exchange of vortex loops. Compared to the coarsening rate of the isotropic XY model, the six-fold degeneracy gives rise to negligible differences with the vortex-antivortex annihilation controlling the scaling dynamics, whereas the anisotropy of interfacial energy results in a deviation. The temporal evolution of domain and vortex structures serves as a platform to fully explore the mesoscale mechanisms for the 0-D and 1-D topological defects.

cond-mat.mtrl-sci↗

arXiv2016

Domain and Phase De-strain - Formation of Ferroelastic Domain Structures

Phase decomposition is a well-known process leading to the formation of two-phase mixtures. Here we show that a strain imposed on a ferroelastic crystal promotes the formation of mixed phases and domains, i.e., domain and phase de-strain with local strains determined by a common tangent construction on the free energy versus strain curves. It is demonstrated that a domain structure can be understood using the concepts of domain/phase rule, lever rule, coherent and incoherent de-strain within the de-strain model description, in a complete analogy to phase decomposition. The proposed de-strain model is validated using phase-field simulations and experimental observations of PbTiO_3 and BiFeO_3 thin films as examples. The de-strain model provides a simple tool to guide and design domain structures of ferroelastic systems.

cond-mat.mtrl-sci↗