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How topological defects, unavoidable at symmetry-breaking phase transitions in a wide range of systems, evolve through consecutive phase transitions with different broken symmetries remains unexplored. Nd2SrFe2O7, a bilayer ferrite, exhibits two intriguing structural phase transitions and dense networks of the so-called type-II Z8 structural vortices at room temperature, so it is an ideal system to explore the topological defect evolution. From our extensive experimental investigation, we demonstrate that the cooling rate at the second-order transition (1290oC) plays a decisive role in determining the vortex density at room temperature, following the universal Kibble-Zurek mechanism. In addition, we discovered a transformation between topologically-distinct vortices (Z8 to Z4 vortices) at the first-order transition (550oC), which conserves the number of vortex cores. Remarkably, the Z4 vortices consist of two phases with an identical symmetry but two distinct magnitudes of an order parameter. Furthermore, when lattice distortion is enhanced by chemical doping, a new type of topological defects emerges: loop domain walls with orthorhombic distortions in the tetragonal background, resulting in unique pseudo-orthorhombic twins. Our findings open a new avenue to explore the evolution of topological defects through multiple phase transitions., Comment: 21 pages, 8 figures

Topological phases such as polar skyrmions have been a fertile playground for ferroelectric oxide superlattices, with exotic physical phenomena such as negative capacitance. Herein, using phase-field simulations, we demonstrate the local control of the skyrmion phase with electric potential applied through a top electrode. Under a relatively small electric potential, the skyrmions underneath the electrode can be erased and recovered reversibly. A topologically protected transition from the symmetric to asymmetric skyrmion bubbles is observed at the edge of the electrode. While a topological transition to a labyrinthine domain requires a high applied potential, it can switch back to the skyrmion state with a relatively small electric potential. The topological transition from +1 to 0 occurs before the full destruction of the bubble state. It is shown that the shrinking and bursting of the skyrmions leads to a large reduction in the dielectric permittivity, the magnitude of which depends on the size of the electrode., Comment: 17 Pages 4 figures

Strongly correlated materials that exhibit an insulator-metal transition are key candidates in the search for new computing platforms. Understanding the pathways and timescales underlying the electrically-driven insulator-metal transition is crucial for uncovering the fundamental limits of device operation. Using stroboscopic electron diffraction, we perform synchronized time-resolved measurements of atomic motions and electronic transport in operating vanadium dioxide switches. We discover an electrically-triggered, isostructural state that forms transiently on microsecond timescales, stabilized by local heterogeneities and interfacial interactions between the equilibrium phases. This metastable phase bears striking similarity to that formed under photoexcitation within picoseconds, suggesting a universal transformation pathway across eight orders of magnitude of timescale. Our results establish a new route for uncovering non-equilibrium and metastable phases in correlated materials, and open avenues for engineering novel dynamical behavior in nanoelectronics.

The collective dynamics of topological structures have been of great interest from both fundamental and applied perspectives. For example, the studies of dynamical properties of magnetic vortices and skyrmions not only deepened the understanding of many-body physics but also led to potential applications in data processing and storage. Topological structures constructed from electrical polarization rather than spin have recently been realized in ferroelectric superlattices, promising for ultrafast electric-field control of topological orders. However, little is known about the dynamics of such complex extended nanostructures which in turn underlies their functionalities. Using terahertz-field excitation and femtosecond x-ray diffraction measurements, we observe ultrafast collective polarization dynamics that are unique to polar vortices, with orders of magnitude higher frequencies and smaller lateral size than those of experimentally realized magnetic vortices. A previously unseen soft mode, hereafter referred to as a vortexon, emerges as transient arrays of nanoscale circular patterns of atomic displacements, which reverse their vorticity on picosecond time scales. Its frequency is significantly reduced at a critical strain, indicating a condensation of structural dynamics. First-principles-based atomistic calculations and phase-field modeling reveal the microscopic atomic arrangements and frequencies of the vortex modes. The discovery of subterahertz collective dynamics in polar vortices opens up opportunities for applications of electric-field driven data processing in topological structures with ultrahigh speed and density.

Polar skyrmions are predicted to emerge from the interplay of elastic, electrostatic and gradient energies, in contrast to the key role of the anti-symmetric Dzyalozhinskii-Moriya interaction in magnetic skyrmions. With the discovery of topologically-stable polar skyrmions, it is of both fundamental and practical interest to understand the microscopic nature and the possibility of temperature- and strain-driven phase transitions in ensembles of such polar skyrmions. Here, we explore the reversible transition from a skyrmion state (topological charge of -1) to a two-dimensional, tetratic lattice of merons (with topological charge of -1/2) upon varying the temperature and elastic boundary conditions in [(PbTiO3)16/(SrTiO3)16]8 lifted-off membranes. This topological phase transition is accompanied by a change in chirality, from zero-net chirality (in meronic phase) to net-handedness (in skyrmionic phase). To map these changes microscopically required developing new imaging methods. We show how scanning convergent beam electron diffraction provides a robust measure of the local polarization simultaneously with the strain state at sub-nm resolution, while also directly mapping the chirality of each skyrmion. Using this, we demonstrate strain as a crucial order parameter to drive isotropic-to-anisotropic structural transitions of chiral polar skyrmions to non-chiral merons, validated with X-ray reciprocal space mapping and theoretical phase-field simulations. These results revealed by our new measurement methods provide the first illustration of systematic control of rich variety of topological dipole textures by altering the mechanical boundary conditions, which may offer a promising way to control their functionalities in ferroelectric nanodevices using the local and spatial distribution of chirality and order., Comment: 39 pages, 5 figures, 14 supporting figures

A comprehensive thermochemical database is constructed based on high-throughput first-principles phonon calculations of over 3000 atomic structures in Ni, Fe, and Co alloys involving a total of 26 elements including Al, B, C, Cr, Cu, Hf, La, Mn, Mo, N, Nb, O, P, Re, Ru, S, Si, Ta, Ti, V, W, Y, and Zr, providing thermochemical data largely unavailable from existing experiments. The database can be employed to predict the equilibrium phase compositions and fractions at a given temperature and an overall chemical composition directly from first-principles by minimizing the chemical potential. It is applied to the additively manufactured nickel-based IN718 superalloy to analyze the phase evolution with temperature. In particular, we successfully predicted the formation of L1$_0$-FeNi, $\gamma'$-Ni$_3$(Fe,Al), $\alpha$-Cr, $\gamma$-Ni$_3$(Nb,Mo), $\gamma''$-Ni$_3$Nb , and $\eta$-Ni$_3$Ti at low temperatures, $\gamma'$-Ni$_3$Al, $\delta$-Ni$_3$Nb, $\gamma''$-Ni$_3$Nb, $\alpha$-Cr, and $\gamma$-Ni(Fe,Cr,Mo) at intermediate temperatures, and $\delta$-Ni$_3$Nb and $\gamma$-Ni(Fe,Cr,Mo) at high temperatures in IN718. These predictions are validated by EDS mapping of compositional distributions and corresponding identifications of phase distributions. The database is expected to be a valuable source for future thermodynamic analysis and microstructure prediction of alloys involving the 26 elements.

The Lorenz number (L) contained in the Wiedemann-Franz law represents the ratio of two kinetic parameters of electronic charge carriers: the electronic contribution to the thermal conductivity (K_el) and the electrical conductivity (sigma), , and can be expressed as LT=K_el/sigma where T is temperature. We demonstrate that the Lorenz number simply equals to the ratio of two thermodynamic quantities: the electronic heat capacity (c_el) and the electrochemical capacitance (c_N) through LT=c_el/c_N , a purely thermodynamic quantity, and thus it can be calculated solely based on the electron density of states of a material. It is shown that our thermodynamic formulation for the Lorenz number leads to: i) the well-known Sommerfeld value L=pi^2/3(k_B/e)^2 at the low temperature limit, ii) the Drude value L=3/2(k_B/e)^2 at the high temperature limit with the free electron gas model, and iii) possible higher values than the Sommerfeld limit for semiconductors. It is also demonstrated that the purely electronic contribution to the thermoelectric figure-of-merit can be directly computed using high-throughput DFT calculations without resorting to the computationally more expensive Boltzmann transport theory to the electronic thermal conductivity and electrical conductivity.

Ferroelectric topological objects (e.g. vortices, skyrmions) provide a fertile ground for exploring emerging physical properties that could potentially be utilized in future configurable nanoelectronic devices. Here, we demonstrate quasi-one-dimensional metallic high conduction channels along two types of exotic topological defects, i.e. the topological cores of (i) a quadrant vortex domain structure and (ii) a center domain (monopole-like) structure confined in high quality BiFeO3 nanoisland array, abbreviated as the vortex core and the center core. We unveil via phase-field simulations that the superfine (< 3 nm) metallic conduction channels along center cores arise from the screening charge carriers confined at the core whereas the high conductance of vortex cores results from a field-induced twisted state. These conducting channels can be repeatedly and reversibly created and deleted by manipulating the two topological states via an electric field, leading to an apparent electroresistance effect with an on/off ratio higher than 103. These results open up the possibility of utilizing these functional one-dimensional topological objects in high-density nanoelectronic devices such as ultrahigh density nonvolatile memory., Comment: manuscript (21 pages, 4 figures) plus supplementary information

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., Comment: 6 pages, 2 figures

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., Comment: 5 pages, 3 figures

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.