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Tiannan Yang

Publications and source records attributed to Tiannan Yang.

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Chemical heterogeneity at conducting ferroelectric domain walls

Natural interfaces in ferroic oxides have developed into versatile playgrounds for studying electronic correlation effects in 2D systems. The microscopic origin of the emergent local electronic properties is often debated, however, as quantitative atomic-scale characterization remains challenging. A prime example is enhanced conductivity at ferroelectric domain walls, attributed to mechanisms ranging from local band gap reduction to point defect accumulations. Here, we resolve the microscopic mechanisms for domain wall conduction in the ferroelectric model system BiFeO3, by combining transport measurements with atom probe tomography to quantify the local chemical composition and correlate it with the electrical properties. Significant chemical variations along the walls are observed, demonstrating an outstanding chemical flexibility at domain walls, which manifest in spatially varying physical properties. The results give a unifying explanation for the diverse electronic behavior observed and establish the fundamental notion that multiple conduction mechanisms can coexist within individual domain walls.

cond-mat.mtrl-sci

Terahertz-field activation of polar skyrons

Unraveling collective modes arising from coupled degrees of freedom is crucial for understanding complex interactions in solids and developing new functionalities. Unique collective behaviors emerge when two degrees of freedom, ordered on distinct length scales, interact. Polar skyrmions, three-dimensional electric polarization textures in ferroelectric superlattices, disrupt the lattice continuity at the nanometer scale with nontrivial topology, leading to previously unexplored collective modes. Here, using terahertz-field excitation and femtosecond x-ray diffraction, we discovered subterahertz collective modes, dubbed 'skyrons', which appear as swirling patterns of atomic displacements functioning as atomic-scale gearsets. Momentum-resolved time-domain measurements of diffuse scattering revealed an avoided crossing in the dispersion relation of skyrons. We further demonstrated that the amplitude and dispersion of skyrons can be controlled by sample temperature and electric-field bias. Atomistic simulations and dynamical phase-field modeling provided microscopic insights into the three-dimensional crystallographic and polarization dynamics. The discovery of skyrons and their coupling with terahertz fields opens avenues for ultrafast control of topological polar structures.

cond-mat.mtrl-sci

Optical Control of Adaptive Nanoscale Domain Networks

Adaptive networks can sense and adjust to dynamic environments to optimize their performance. Understanding their nanoscale responses to external stimuli is essential for applications in nanodevices and neuromorphic computing. However, it is challenging to image such responses on the nanoscale with crystallographic sensitivity. Here, the evolution of nanodomain networks in (PbTiO3)n/(SrTiO3)n superlattices was directly visualized in real space as the system adapts to ultrafast repetitive optical excitations that emulate controlled neural inputs. The adaptive response allows the system to explore a wealth of metastable states that were previously inaccessible. Their reconfiguration and competition were quantitatively measured by scanning x-ray nanodiffraction as a function of the number of applied pulses, in which crystallographic characteristics were quantitatively assessed by assorted diffraction patterns using unsupervised machine-learning methods. The corresponding domain boundaries and their connectivity were drastically altered by light, holding promise for light-programmable nanocircuits in analogy to neuroplasticity. Phase-field simulations elucidate that the reconfiguration of the domain networks is a result of the interplay between photocarriers and transient lattice temperature. The demonstrated optical control scheme and the uncovered nanoscopic insights open opportunities for remote control of adaptive nanoscale domain networks.

cond-mat.mes-hall

Non-equilibrium pathways to emergent polar supertextures

Ultrafast stimuli can stabilize metastable states of matter inaccessible by equilibrium means. Establishing the spatiotemporal link between ultrafast excitation and metastability is crucial to understanding these phenomena. Here, we use single-shot optical-pump, X-ray-probe measurements to provide snapshots of the emergence of a persistent polar vortex supercrystal in a heterostructure that hosts a fine balance between built-in electrostatic and elastic frustrations by design. By perturbing this balance with photoinduced charges, a starting heterogenous mixture of polar phases disorders within a few picoseconds, resulting in a soup state composed of disordered ferroelectric and suppressed vortex orders. On the pico-to-nanosecond timescales, transient labyrinthine fluctuations form in this soup along with a recovering vortex order. On longer timescales, these fluctuations are progressively quenched by dynamical strain modulations, which drive the collective emergence of a single supercrystal phase. Our results, corroborated by dynamical phase-field modeling, reveal how ultrafast excitation of designer systems generates pathways for persistent metastability.

cond-mat.mtrl-sci

Temperature-dependent Multi-well Free-energy Landscape for Phase Transitions: PbTiO3 as a Prototype

It has been a long challenge to analytically construct the quantitative temperature-dependent multi-well free-energy landscape over the space of order parameters describing phase transitions and associated critical phenomena. Here we propose a simple analytical model for the free energy landscape based on a priori concept of Boltzmann thermal mixing among multiple parabolic potentials representing different energetically degenerated ground states in contrast to the popular Landau theory using the high-temperature disordered state as a reference. The model recovers both the Weiss molecular field theory and the temperature dependent behaviors of the second order Landau coefficient. It is rather remarkable that such a simple analytical expression can describe a wide variety of properties across the ferroelectric phase transition in PbTiO3, including the temperature dependences of the spontaneous polarization, the heat capacities, the permittivity tensor, and the lattice parameters. The approach also allows parametrization of the free energy function across phase transitions based directly on the 0 K thermodynamics data that can be obtained from DFT calculations. We anticipate that the approach can be equally applied to other types of critical phenomena, e.g., the superconducting phase transition, the metal-insulator transition, and the magnetic transitions.

cond-mat.mtrl-sci

Real-space imaging of polar and elastic nano-textures in thin films via inversion of diffraction data

Exploiting the emerging nanoscale periodicities in epitaxial, single-crystal thin films is an exciting direction in quantum materials science: confinement and periodic distortions induce novel properties. The structural motifs of interest are ferroelastic, ferroelectric, multiferroic, and, more recently, topologically protected magnetization and polarization textures. A critical step towards heterostructure engineering is understanding their nanoscale structure, best achieved through real-space imaging. X-ray Bragg coherent diffractive imaging visualizes sub-picometer crystalline displacements with tens of nanometers spatial resolution. Yet, it is limited to objects spatially confined in all three dimensions and requires highly coherent, laser-like x-rays. Here we lift the confinement restriction by developing real-space imaging of periodic lattice distortions: we combine an iterative phase retrieval algorithm with unsupervised machine learning to invert the diffuse scattering in conventional x-ray reciprocal-space mapping into real-space images of polar and elastic textures in thin epitaxial films. We first demonstrate our imaging in PbTiO3/SrTiO3 superlattices to be consistent with published phase-field model calculations. We then visualize strain-induced ferroelastic domains emerging during the metal-insulator transition in Ca2RuO4 thin films. Instead of homogeneously transforming into a low-temperature structure (like in bulk), the strained Mott insulator splits into nanodomains with alternating lattice constants, as confirmed by cryogenic scanning transmission electron microscopy. Our study reveals the type, size, orientation, and crystal displacement field of the nano-textures. The non-destructive imaging of textures promises to improve models for their dynamics and enable advances in quantum materials and microelectronics.

cond-mat.mtrl-sci

Electric-field control of the nucleation and motion of isolated three-fold polar vertices

Recently various topological polar structures have been discovered in oxide thin films. Despite the increasing evidence of their switchability under electrical and/or mechanical fields, the dynamic property of isolated ones, which is usually required for applications such as data storage, is still absent. Here, we show the controlled nucleation and motion of isolated three-fold vertices under an applied electric field. At the PbTiO3/SrRuO3 interface, a two-unit-cell thick SrTiO3 layer provides electrical boundary conditions for the formation of three-fold vertices. Utilizing the SrTiO3 layer and in situ electrical testing system, we find that isolated three-fold vertices can move in a controllable and reversible manner with a velocity up to ~629 nm s-1. Microstructural evolution of the nucleation and propagation of isolated three-fold vertices is further revealed by phase-field simulations. This work demonstrates the ability to electrically manipulate isolated three-fold vertices, shedding light on the dynamic property of isolated topological polar structures.

cond-mat.mtrl-sci

Thermodynamic and electron-transport properties of Ca3Ru2O7 from first-principles phonon calculations and Boltzmann transport theory

This work demonstrates a first-principles-based approach to obtaining finite temperature thermal and electronic transport properties which can be employed to model and understand mesoscale structural evolution during electronic, magnetic, and structural phase transitions. A computationally tractable model was introduced to estimate the temperature dependence of the electron relaxation time. The model is applied to Ca3Ru2O7 with a focus on understanding its electrical resistivity across the electronic phase transition at 48 K. A quasiharmonic phonon approach to the lattice vibrations was employed to account for thermal expansion while the Boltzmann transport theory including spin-orbit coupling was used to calculate the electron-transport properties, including the temperature dependence of electrical conductivity.

cond-mat.mtrl-sci

A Solution to the Temperature Evolution of Multi-well Free-energy Landscape

It has been a grand challenge to resolve the temperature evolution of multi-well free-energy landscape which is fundamentally relevant to phase transitions and associated critical phenomena as listed by Ginzburg [Rev. Mod. Phys. 76 (2004) 981]. To address this challenge, here we provide a simple solution based on a priori concept of Boltzmann thermal mixing among multiple parabolic potentials. The success and the impact of the present approach have been extensively demonstrated using a variety of materials, including Nb, YBa2Cu3O(7-x), Ca3Ru2O7, Ni, BiFeO3, and PbTiO3.

cond-mat.stat-mech

Large Itinerant Electron Exchange Coupling in the Magnetic Topological Insulator MnBi2Te4

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with applications in spintronics and quantum information. The emergence of such phases relies on strong interaction between localized spins and itinerant states comprising the topological bands, and the subsequent formation of an exchange gap. However, this interaction has never been measured in any intrinsic magnetic topological material. Using a multimodal approach, this exchange interaction is measured in MnBi2Te4, the first realized intrinsic magnetic topological insulator. Interrogating nonequilibrium spin dynamics, itinerant bands are found to exhibit a strong exchange coupling to localized Mn spins. Momentum-resolved ultrafast electron scattering and magneto-optic measurements reveal that itinerant spins disorder via electron-phonon scattering at picosecond timescales. Localized Mn spins, probed by resonant X-ray scattering, disorder concurrently with itinerant spins, despite being energetically decoupled from the initial excitation. Modeling the results using atomistic simulations, the exchange coupling between localized and itinerant spins is estimated to be >100 times larger than superexchange interactions. This implies an exchange gap of >25 meV should occur in the topological surface states. By directly quantifying local-itinerant exchange coupling, this work validates the materials-by-design strategy of utilizing localized magnetic order to create and manipulate magnetic topological phases, from static to ultrafast timescales.

cond-mat.mtrl-sci

Subterahertz collective dynamics of polar vortices

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.

cond-mat.mes-hall

Theory and phase-field simulations on electrical control of spin cycloids in a multiferroic

Cycloidal spin orders are common in multiferroics. One of the prototypical examples is BiFeO3 (BFO) which shows a large polarization and a cycloidal antiferromagnetic order at room temperature. Here we employ Landau theory and phase-field simulations to analyze the coupled switching dynamics of polarization and cycloidal antiferromagnetic orders in BFO. We are able to identify 14 types of transitional spin structures between two cycloids and 9 electric-field-induced spin switching paths. We demonstrate the electric-field-induced rotation of wave vectors of the cycloidal spins and discover 2 types of cycloidal spin switching dynamics: fast local spin flips and slow rotation of wave vectors. Also, we construct road maps to achieve the switching between any two spin cycloids through multi-step applications of electric fields. The work provides a theoretical framework for the phenomenological description of spin cycloids and a fundamental understanding of the switching mechanisms to achieve electrical control of magnetic orders.

cond-mat.mtrl-sci

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