Multiferroicity induced by dislocated spin-density waves

We uncover a new pathway towards multiferroicity, showing how magnetism can drive ferroelectricity without relying on inversion symmetry breaking of the magnetic ordering. Our free-energy analysis demonstrates that any commensurate spin-density-wave ordering with a phase dislocation, even if it is collinear, gives rise to an electric polarization. Because of the dislocation, the electronic and magnetic inversion centers do not coincide, which turns out to be a sufficient condition for multiferroic coupling. The novel mechanism explains the formation of multiferroic phases at the magnetic commensurability transitions, such as the ones observed in YMn(2)O(5) and related compounds. We predict that in these multiferroics an oscillating electrical polarization is concomitant with the uniform polarization. On the basis of our theory, we put forward new types of magnetic materials that are potentially ferroelectric.     

General theory for the ferroelectric polarization induced by spin-spiral order

The ferroelectric polarization of triangular-lattice antiferromagnets induced by helical spin-spiral order is not explained by any existing model of magnetic-order-driven ferroelectricity. We resolve this problem by developing a general theory for the ferroelectric polarization induced by spin-spiral order and then by evaluating the coefficients needed to specify the general theory on the basis of density functional calculations. Our theory correctly describes the ferroelectricity of triangular-lattice antiferromagnets driven by helical spin-spiral order and incorporates known models of magnetic-order-driven ferroelectricity as special cases.     

A self-consistent approach to soft mode analysis in size driven ferroelectricity

The polarization distribution in a finite size system obtained through Landau phenomenology is shown to contain unphysical oscillatory parts [P. Khare, D. Sa, Solid State Commun. 150 (2010) 172]. Self-consistency in the solution has been used to remove such difficulty and the issue of soft mode in such system has been addressed. The temperature as well as the size dependence of the soft mode frequency is calculated and compared with the experiment. The extrapolation length for the size driven ferroelectricity is argued to behave in a way similar to that of correlation length in phase transition in bulk system.     

Toroidal ferroelectricity in PbTiO3 nanoparticles

We report from first-principles-based atomistic simulations that ferroelectricity can be sustained in PbTiO(3) nanoparticles of only a few lattice constants in size as a result of a toroidal ordering. We find that size-induced topological transformations lead to the stabilization of a ferroelectric bubble by the alignment of vortex cores along a closed path. These transformations, which are driven by the aspect ratio of the nanostructure, change the topology of the polarization field, producing a rich variety of polar configurations. For sufficiently flat nanostructures, a multibubble state bridges the gap between 0D nanodots and 2D ultrathin films. The thermal properties of the ferroelectric bubbles indicate that this state is suitable for the development of nanometric devices.     

低维铁电材料研究进展

铁电材料是一类重要的功能材料,铁电元件的小型化、集成化是当今铁电材料发展的一大趋势.但是尺寸效应、表面效应等的存在制约了传统块体铁电材料在纳米尺度下的应用,因而低维度纳米材料中的铁电性能研究成为当前材料科学领域的研究热点之一.本文综述了近年来理论和实验上关于低维铁电材料的探索,包括二维范德瓦耳斯层状铁电材料、共价功能化低维铁电材料、低维钙钛矿材料、外界调控以及二维"铁电金属"等材料的理论预言与实验铁电性的观测;也提出一些物理新机制来解释低维下的铁电性;最后对该领域今后的发展进行了展望.     

Room-temperature vertical ferroelectricity in rhenium diselenide induced by interlayer sliding

One variety of ferroelectricity that results from lateral relative movements between the adjacent atomic layers is referred to as sliding ferroelectricity, which generates an interfacial charge transfer and hence a polarization reversal. The mechanism of sliding ferroelectricity existent in van der Waals crystals is quite distinct from the conventional ferroelectric switching mechanisms mediated by ion displacement. It creates new possibilities for the design of two-dimensional (2D) ferroelectrics since it can be achieved even in non-polar systems. Before 2D ferroelectrics can be widely employed for practical implementations, however, there is still significant work to be done on several fronts, such as exploring ferroelectricity possibly in more potential 2D systems. Here, we report the experimental observation of room-temperature robust vertical ferroelectricity in layered semiconducting rhenium diselenide (ReSe₂), a representative member of the transition metal dichalcogenides material family, based on a combined research of nanoscale piezoresponse and second harmonic generation measurements. While no such ferroelectric behavior was seen in 1L ReSe₂, 2L ReSe₂ exhibits vertical ferroelectricity at ambient environment. Based on density-functional theory calculations, we deduce that the microscopic origin of ferroelectricity for ReSe₂ is uncompensated vertical charge transfer that is dependent on in-plane translation and switchable upon interlayer sliding. Our findings have important ramifications for the ongoing development of sliding ferroelectricity since the semiconducting properties and low switching barrier of ReSe₂ open up the fascinating potential for functional nanoelectronics applications.     

Absence of ferroelectric critical size in ultrathin PbTiO3 nanotubes: a density-functional theory study

We simulate from first principles the energetic, structural, and electronic properties of ferroelectric (FE) ultrathin PbTiO3 nanotubes. The nanotube possesses spontaneous polarization despite their sidewalls being thinner than the critical thickness at which the thin films lose ferroelectricity; this indicates the absence of an intrinsic critical size for ferroelectricity. The ground state of the nanotube is not purely FE since it primarily involves antiferrodistortive (AFD) rotations of oxygen atoms due to compression in the inner tube wall. The emergence of the AFD displacement plays a central role in stabilizing both the nanotubular structure and FE distortions due to direct AFD-FE coupling. Moreover, we predict intriguing rich phase transitions due to axial strains including polarization vortices as an important class of nanoscale FE ordering.     

Interface control of emergent ferroic order in Ruddlesden-Popper Sr(n+1)Ti(n)O(3n+1)

We discovered from first principles an unusual polar state in the low n Sr(n+1)Ti(n)O(3n+1) Ruddlesden-Popper (RP) layered perovskites in which ferroelectricity is nearly degenerate with antiferroelectricity, a relatively rare form of ferroic order. We show that epitaxial strain plays a key role in tuning the "perpendicular coherence length" of the ferroelectric mode, and does not induce ferroelectricity in these low-dimensional RP materials as is well known to occur in SrTiO(3). These systems present an opportunity to manipulate the coherence length of a ferroic distortion in a controlled way, without disorder or a free surface.     

Ferroelectricity driven by the noncentrosymmetric magnetic ordering in multiferroic TbMn(2)O(5): a first-principles study

The ground state structural, electronic, and magnetic properties of multiferroic TbMn(2)O(5) are investigated via first-principles calculations. We show that the ferroelectricity in TbMn(2)O(5) is driven by the noncentrosymmetric magnetic ordering, without invoking the spin-orbit coupling and noncollinear spins. The intrinsic electric polarization in this compound is calculated to be 1187 nC cm(-2), an order of magnitude larger than previously thought.     

Properties of polarization evolution in spun fibers

We study the properties of polarization evolution in sinusoidally spun fibers. It is found that, similar to linear birefringent fibers, the evolution of the state of polarization exhibits periodicity, which can be measured by distributed measurement, such as those made with a polarization optical time domain reflectometer. The spatial period is linked with the spin parameters and fiber beat length in a simple equation. In combination with a previous finding, it is shown that the spatial period is uniquely related to spun-fiber polarization mode dispersion. This suggests that distributed fiber polarization mode dispersion can be determined throughthe measurement of the spatial period obtained in a distributed measurement.     

钛酸钡纳米颗粒铁电性临界尺寸的理论分析

从铁电体的Eular-Lagrange方程出发, 取贝塞尔方程级数解的形式, 得到了钛酸钡陶瓷颗粒的总极化强度表达式, 分析了各系数对总极化强度的影响. 根据总极化强度表达式, 采用MATLAB软件对尺寸在100 nm以下的钛酸钡纳米颗粒的铁电性进行了仿真分析. 结合实际数据探讨了尺寸效应对陶瓷颗粒铁电性的影响, 获得了与实验数据相符的数值解和极小值, 从而预测了钛酸钡纳米颗粒铁电性存在的临界尺寸为6 nm.     

Surface effects and diffusive phase transition in ferroelectric thin films: A self-consistent approach

A self-consistent Landau phenomenological approach has been used to study the ferroelectric transition in films in the presence of various surface effects such as depolarization and strain. The polarization distribution of the film is computed and its variation with respect to temperature, thickness and strain is determined. The gradual decrease in polarization across the transition shows the diffusive behavior which is confirmed from the soft mode and the dielectric susceptibility analysis. The critical thickness below which ferroelectricity disappears is also computed. The degree of diffuseness in the transition is obtained from the susceptibility exponent which shows more and more diffusive behavior for smaller and smaller film thickness.     

An investigation on magnetism, spin–phonon coupling, and?ferroelectricity in multiferroic GdMn2O5

The magnetization, Raman spectroscopy, and ferroelectricity of multiferroic GdMn₂O₅ as a function of temperature and magnetic field are investigated. The complicated magnetic transitions at low temperatures are featured with anomalous Raman mode shifts, dielectric response, and ferroelectricity generation, indicating the significant spin–phonon coupling. It is argued that this coupling is possibly responsible for the electrical polarization generation associated with the incommensurate–commensurate transition.      

Coupling of magnetic and ferroelectric hysteresis by a multicomponent magnetic structure in Mn2GeO4

The olivine compound Mn(2)GeO(4) is shown to feature both a ferroelectric polarization and a ferromagnetic magnetization that are directly coupled and point along the same direction. We show that a spin spiral generates ferroelectricity, and a canted commensurate order leads to weak ferromagnetism. Symmetry suggests that the direct coupling between the ferromagnetism and ferroelectricity is mediated by Dzyaloshinskii-Moriya interactions that exist only in the ferroelectric phase, controlling both the sense of the spiral rotation and the canting of the commensurate structure. Our study demonstrates how multicomponent magnetic structures found in magnetically frustrated materials like Mn(2)GeO(4) provide a new route towards functional materials that exhibit coupled ferromagnetism and ferroelectricity.     

钙钛矿型氧化物非常规铁电研究进展

钙钛矿型氧化物因具有丰富的磁性、铁电、力学和光学等诸多功能属性,在电子信息通信材料器件领域中有广阔的应用前景.在各种物理性质之中,铁电极化因其产生机制多样,并能与磁性和晶格应变相互耦合形成多铁性等特点,近十多年来一直被作为凝聚态物理研究的国际热点问题.与以自发极化作为初级序参量的常规铁电材料不同,非常规铁电材料中的铁电极化是被其他的序参量诱导而产生的.本综述围绕无机钙钛矿型氧化物非常规铁电体的研究进展进行了总结.回顾了该体系经典唯象理论和原子尺度的微观模型,有序排列的人工钙钛矿超晶格型结构,以及稀土正铁氧体单晶的反铁磁畴壁结构中非常规铁电的极化强度大小及其诱导机制,为系统理解非常规铁电提供了理论途径.     

Dynamical magnetoelectric coupling in helical magnets

We develop a theory of collective mode dynamics in the helical magnets coupled to electric polarization via spin-orbit interaction. The low-lying modes associated with the ferroelectricity are not the transverse optical phonons, but are the spin waves hybridized with the electric polarization. This hybridization leads to the Drude-like dielectric function epsilon(omega) in the limit of zero magnetic anisotropy. There are two additional low-lying modes: phason of the spiral and rotation of helical plane along the polarization axis. Role of these low-lying modes in the neutron scattering and antiferromagnetic resonance is revealed, and a novel experiment to detect the dynamical magnetoelectric coupling is discussed.     

SrBi4Ti4O15的化学键性质和铁电性研究

通过原子环境计算方法分析了正交相SrBi₄Ti₄O₁₅晶体内的键络结构、各原子的空间配位数及局域团簇结构. 在此基础上, 结合晶体分解理论将SrBi₄Ti₄O₁₅晶体分解为多个二元赝晶体, 根据化学键介电理论计算得到各赝晶体所对应化学键的有效价电子密度、离子性等化学键性质. 通过键偶极矩建立了铁电体自发极化强度与化学键性质之间的关系, 求得正交相SrBi₄Ti₄O₁₅沿a轴方向的自发极化强度为28.03 μC/cm², 与实验结果和其他理论计算值符合较好.     

铁电极化子动力学理论

在铁电屏蔽理论的基础上发展铁电极化子动力学理论,用来解释铁电体的极化反转现象.理论结果与TGS单晶的实验结果符合得很好.由该理论还可进一步用来研究铁电发射的基本物理过程 关键词： 铁电极化子 极化反转 慢极化效应     

Displacement-type ferroelectricity with off-center magnetic ions in perovskite Sr(1-x)Ba(x)MnO3

We report a ferroelectric transition driven by the off-centering of magnetic Mn(4+) ions in antiferromagnetic Mott insulators Sr(1-x)Ba(x)MnO(3) with a perovskite structure. As x increases, the perovskite lattice shows the typical soft-mode dynamics, as revealed by the momentum-resolved inelastic x-ray scattering and far-infrared spectroscopy, and the ferroelectricity shows up for x ≥ 0.45. The observed polarization is comparable to that for a prototypical ferroelectric BaTiO(3). We further demonstrate that the magnetic order suppresses the ferroelectric lattice dilation by ～70% and increases the soft-phonon energy by ～50%, indicating the largest magnetoelectric effects yet attained.     

Landau theory of ferroelectric transition in long cylindrical nanoparticles

Using a phenomenological Landau theory, the size dependence on ferroelectric transition for free-standing long cylindrical nanoparticles is discussed. We derive the size dependence of the transition temperature, polarization profile as well as the static susceptibility. The transition temperature vanishes below a critical size where the static susceptibility shows divergence obeying Curie-Weiss law. In order to make this result compared with experiments, the average polarization and the susceptibility is computed with a Gaussian particle size distribution. The average polarization in such a case shows smearing with respect to the particle size whereas the divergence in the susceptibilty gets rounded. This might correspond to a size dependent soft mode which can be observed in Raman measurement.