Broken Inversion Symmetry Research Articles

Picosecond Spin Current Generation from Vicinal Metal-Antiferromagnetic Insulator Interfaces.

We report the picosecond spin current generation from the interface between a heavy metal and a vicinal antiferromagnet insulator Cr_{2}O_{3} by laser pulses at room temperature and zero magnetic field. It is converted into a detectable terahertz emission in the heavy metal via the inverse spin Hall effect. The vicinal interfaces are apparently the source of the picosecond spin current, as evidenced by the proportional terahertz signals to the vicinal angle. We attribute the origin of the spin current to the transient magnetic moment generated by an interfacial nonlinear magnetic-dipole difference-frequency generation. We propose a model based on the in-plane inversion symmetry breaking to quantitatively explain the terahertz intensity with respect to the angles of the laser polarization and the film azimuth. Our work opens new opportunities in antiferromagnetic and ultrafast spintronics by considering symmetry breaking.

Alloying Driven Antiferromagnetic Skyrmions on NiPS3 Monolayer: A First-Principles Calculation.

Topological magnetic states are promising information carriers for ultrahigh-density and high-efficiency magnetic storage. Recent advances in two-dimensional (2D) magnets provide powerful platforms for stabilizing various nanometer-size topological spin textures within a wide range of magnetic field and temperature. However, non-centrosymmetric 2D magnets with broken inversion symmetry are scarce in nature, making direct observations of the chiral spin structure difficult, especially for antiferromagnetic (AFM) skyrmions. In this work, it is theoretically predicted that intrinsic AFM skyrmions can be easily triggered in XY-type honeycomb magnet NiPS3 monolayer by alloying of Cr atoms, due to the presence of a sizable Dzyaloshinskii-Moriya interaction. More interestingly, the diameter of the AFM skyrmions in Ni3/4Cr1/4PS3 decreases from 12 to 4.4nm as the external magnetic field increases and the skyrmion phases remain stable up to an external magnetic field of 4 T. These results highlight an effective strategy to generate and modulate the topological spin texture in 2D magnets by alloying with magnetic element.

Frustrated Extended Bose-Hubbard Model and Deconfined Quantum Critical Points with Optical Lattices at the Antimagic Wavelength.

The study of geometrically frustrated many-body quantum systems is of central importance to uncover novel quantum mechanical effects. We design a scheme where ultracold bosons trapped in a one-dimensional state-dependent optical lattice are modeled by a frustrated Bose-Hubbard Hamiltonian. A derivation of the Hamiltonian parameters based on Cesium atoms, further show large tunability of contact and nearest-neighbor interactions. For pure contact repulsion, we discover the presence of two phases peculiar to frustrated quantum magnets: the bond-order-wave insulator with broken inversion symmetry and a chiral superfluid. When the nearest-neighbor repulsion becomes sizable, a further density-wave insulator with broken translational symmetry can appear. We show that the phase transition between the two spontaneously symmetry-broken phases is continuous, thus representing a one-dimensional deconfined quantum critical point not captured by the Landau-Ginzburg-Wilson symmetry-breaking paradigm. Our results provide a solid ground to unveil the novel quantum physics induced by the interplay of nonlocal interactions, geometrical frustration, and quantum fluctuations.

Skyrmion lattice in centrosymmetric magnets with local Dzyaloshinsky–Moriya interaction

It is common for the local inversion symmetry to break in crystals, even though the whole crystal has global inversion symmetry. This local inversion symmetry breaking allows for a local Dzyaloshinsky–Moriya interaction (DMI) in magnetic crystals. Here we show that the local DMI can stabilize a skyrmion as a metastable excitation or as a skyrmion crystal in equilibrium. We consider the crystal structure with layered structure as an example, where local inversion is violated in each layer but a global inversion center exists in the middle of the two layers. These skyrmions come in pairs that are related by inversion symmetry. The two skyrmions with opposite helicity in a pair form a bound state. We study the properties of a skyrmion pair in the ferromagnetic background and determine the equilibrium phase diagram, where a robust lattice of skyrmion pairs is stabilized. Our results point to a new direction to search for the skyrmion lattice in centrosymmetric magnets.

Topological Kerr effects in two-dimensional magnets with broken inversion symmetry

Topological Kerr effects in two-dimensional magnets with broken inversion symmetry

Reversible non-volatile electronic switching in a near-room-temperature van der Waals ferromagnet

Non-volatile phase-change memory devices utilize local heating to toggle between crystalline and amorphous states with distinct electrical properties. Expanding on this kind of switching to two topologically distinct phases requires controlled non-volatile switching between two crystalline phases with distinct symmetries. Here, we report the observation of reversible and non-volatile switching between two stable and closely related crystal structures, with remarkably distinct electronic structures, in the near-room-temperature van der Waals ferromagnet Fe5−δGeTe2. We show that the switching is enabled by the ordering and disordering of Fe site vacancies that results in distinct crystalline symmetries of the two phases, which can be controlled by a thermal annealing and quenching method. The two phases are distinguished by the presence of topological nodal lines due to the preserved global inversion symmetry in the site-disordered phase, flat bands resulting from quantum destructive interference on a bipartite lattice, and broken inversion symmetry in the site-ordered phase.

Structure-Guided Approaches for Enhanced Spin-Splitting in Chiral Perovskite.

Hybrid organic-inorganic perovskites with diverse lattice structures and chemical composition provide an ideal material platform for novel functionalization, including chirality transfer. Chiral perovskites combine organic and inorganic sublattices, therefore encoding the structural asymmetry into the electronic structures and giving rise to the spin-splitting effect. From a structural chemistry perspective, the magnitude of the spin-splitting effect crucially depends on the noncovalent and electrostatic interaction within the chiral perovskite, which induces the local site and long-range bulk inversion symmetry breaking. In this regard, we systematically retrospect the structure-property relationships in chiral perovskite. Insight into the rational design of chiral perovskites based on molecular configuration, dimensionality, and chemical composition along with their effects on spin-splitting manifestation is presented. Lastly, challenges in purposeful material design and further integration into chiral perovskite-based spintronic devices are outlined. With an understanding of fundamental chemistry and physics, we believe that this Perspective will propel the application of multifunctional spintronic devices.

Rashba spin-splitting and spin Hall effect in Janus monolayers Sb2XSX’ (X, X’= S, Se, or Te; X ≠ X’)

The combined influence of spin–orbit coupling and spatial inversion asymmetry leads to an enhancement of electronic properties, including Rashba spin-splittings as well as spin Hall effect. Recent research has shown the possibility to create two-dimensional Janus materials with inherent structural asymmetry. In this work, the structural stability, piezoelectricity, electronic properties, and intrinsic spin Hall conductivity of quintuple-layer atomic Janus Sb2XSX’ (X, X’ = S, Se, Te; X ≠ X’) monolayers are investigated using first-principles calculations within the framework of density functional theory. They demonstrate relatively high in-plane piezoelectric coefficients (d22) and also possess out-of-plane piezoelectric coefficients (d31), which is due to the breaking of inversion symmetry in the crystal structure with the space group P3m1. Large Rashba parameters are obtained in Janus Sb2XSX’ monolayers, especially high for Sb2S2Te (1.62 eV Å) and Sb2SeSTe (1.33 eV Å) due to strong spin–orbit coupling. Moreover, Rashba-like spin-splitting is also observed in the edge-states as well, which is highest for Sb2SeSTe with 2.17 eV Å. Furthermore, Sb2S2Te and Sb2SeSTe monolayers reveal a significantly high Berry curvature (65.59 and 61.05 Bohr2), spin Berry curvature (−118.4 and −120.6 Bohr2), and spin Hall conductivity (1.8 and 1.6 e2/h). Our results suggest that Janus Sb2S2Te and Sb2SeSTe monolayers could be an excellent platform for multifunctional electronic applications.

Large nonlinear optical magnetoelectric response in a noncentrosymmetric magnetic Weyl semimetal

Weyl semimetals resulting from either inversion (P) or time-reversal (T) symmetry breaking have been revealed to show the record-breaking large optical response due to intense Berry curvature of Weyl-node pairs. Different classes of Weyl semimetals with both P and T symmetry breaking potentially exhibit optical magnetoelectric (ME) responses, which are essentially distinct from the previously observed optical responses in conventional Weyl semimetals, leading to the versatile functions such as directional dependence for light propagation and gyrotropic effects. However, such optical ME phenomena of (semi)metallic systems have remained elusive so far. Here, we show the large nonlinear optical ME response in noncentrosymmetric magnetic Weyl semimetal PrAlGe, in which the polar structural asymmetry and ferromagnetic ordering break P and T symmetry. We observe the giant second harmonic generation (SHG) arising from the P symmetry breaking in the paramagnetic phase, being comparable to the largest SHG response reported in Weyl semimetal TaAs. In the ferromagnetically ordered phase, it is found that interference between this nonmagnetic SHG and the magnetically induced SHG emerging due to both P and T symmetry breaking results in the magnetic field switching of SHG intensity. Furthermore, such an interference effect critically depends on the light-propagating direction. The corresponding magnetically induced nonlinear susceptibility is significantly larger than the prototypical ME material, manifesting the existence of the strong nonlinear dynamical ME coupling. The present findings establish the unique optical functionality of P- and T-symmetry broken ME topological semimetals.

Anomalous layer-dependent photoluminescence spectra of supertwisted spiral WS2.

Twisted stacking of two-dimensional materials with broken inversion symmetry, such as spiral MoTe2 nanopyramids and supertwisted spiral WS2, emerge extremely strong second- and third-harmonic generation. Unlike well-studied nonlinear optical effects in these newly synthesized layered materials, photoluminescence (PL) spectra and exciton information involving their optoelectronic applications remain unknown. Here, we report layer- and power-dependent PL spectra of the supertwisted spiral WS2. The anomalous layer-dependent PL evolutions that PL intensity almost linearly increases with the rise of layer thickness have been determined. Furthermore, from the power-dependent spectra, we find the power exponents of the supertwisted spiral WS2 are smaller than 1, while those of the conventional multilayer WS2 are bigger than 1. These two abnormal phenomena indicate the enlarged interlayer spacing and the decoupling interlayer interaction in the supertwisted spiral WS2. These observations provide insight into PL features in the supertwisted spiral materials and may pave the way for further optoelectronic devices based on the twisted stacking materials.

Gate-tunable circular phonon dichroism effect in bilayer graphene

Circular phonon dichroism effect has been proposed in two-dimensional materials; however, the lack of tunability hinders the exploration of the effect. Here, we investigate the role of dual-gating-induced inversion symmetry breaking in the circular phonon dichroism effect in bilayer graphene. We find that the introduction of inversion symmetry breaking modifies the response in the layer-symmetric and layer-antisymmetric channels, and results in the occurrence of phonon dichroism in the cross-channel. In the layer representation, the inversion symmetry breaking breaks the equality of intralayer circular phonon dichroism and enhances the interlayer response. Our results suggest that layer degree of freedom provides possibilities to tune phonon dynamics, which paves a way toward different physics and applications of two-dimensional acoustoelectronics and layertronics.

On the local aspect of valley magnetic moments

Valley magnetic moments play a crucial role in valleytronics in 2D hexagonal materials. Traditionally, insights drawn from the study of quantum states in homogeneous bulks have led to a widespread belief that only materials with broken structural inversion symmetry can exhibit nonvanishing valley magnetic moments. This belief, however, limits the scope of relevant applications, especially for materials with inversion symmetry, such as gapless monolayer graphene, despite its advantage in routine growth and production. This work revisits valley-derived magnetic moments in a broad context covering inhomogeneous structures as well. It generalizes the notion of a valley magnetic moment for a state from an integrated quantity to the local field called the “local valley magnetic moment” with space-varying distribution. It explores the local magnetic moment analytically both within the Dirac model and through a symmetry argument. Numerical investigations are conducted within the tight-binding model. Overall, we demonstrate that the breaking of inversion symmetry in the electron probability distribution leads to nonvanishing local magnetic moments. This probability-based breaking can occur in both structural inversion symmetric and symmetry-broken structures. In suitable inversion-symmetric structures with inhomogeneity, e.g., zigzag nanoribbons of gapless monolayer graphene, it is shown that the local moment of a state can be nonvanishing while the corresponding integrated moment is subject to the broken symmetry constraint. Moreover, it is demonstrated that the local moment can interact with space-dependent magnetic fields, resulting in field effects such as valley Zeeman splitting. Such effects can be exploited for local valley control as a conduit for the implementation of valleytronics.

Symmetry and magnetic direction dependent spin/valley splitting and anomalous Hall conductivity of antiferromagnetic monolayer MnPTe3

Due to the time reversal symmetry breaking or spin-valley coupling, there are intrinsic valley splittings in two-dimensional magnetic materials, which are closely related to the symmetry and magnetic order. Based on MnPTe3 monolayers with different symmetries, we present an understanding of direction dependent spin/valley splitting and anomalous Hall conductivity from the perspective of orbital interactions. Unlike T-MnPTe3 with central inversion symmetry, in-plane magnetization leads to further non-degeneracy of valley electrons of H–MnPTe3, and the splitted valley states are spin polarized, which is perpendicular to the in-plane magnetization direction. The model and first-principle calculations consistently indicate that the splitting of the valley states is almost proportional to sinθxz, which originates from the difference in spin-up and spin-down interactions introduced by the breaking of spatial inversion symmetry. Regardless of spin degeneracy, non-zero anomalous Hall conductivity occurs with out-of-plane magnetization, and this direction dependent anomalous Hall effect is caused by mirror symmetry breaking from the neighboring Te atoms and spin-orbit coupling. Magnetization direction is an important means of regulating valley/spin splittings and anomalous Hall effect, which has certain significance for realizing spin or valley polarized Hall effect and the research of spintronic or valleytronic devices.

Coexistence of Ferromagnetism and Ferroelectricity in Cu-Intercalated Bilayer CrI3.

Design of two-dimensional (2D) multiferroic materials with two or more ferroic orders in one structure is highly desired in view of the development of next-generation electronic devices. Unfortunately, experimental or theoretical discovery of 2D intrinsic multiferroic materials is rare. Using first-principles calculation methods, we report the realization of multiferroics that couple ferromagnetism and ferroelectricity by intercalating Cu atoms in bilayer CrI3, Cux@bi-CrI3 (x = 0.03, 0.06, and 0.25). Our results show that the intercalation of Cu atoms leads to the inversion symmetry breaking of bilayer CrI3 and produces intercalation density-dependent out-of-plane electric polarization, around 18.84-90.31 pC·cm-2. Moreover, the switch barriers of Cux@bi-CrI3 in both polarization states are small, ranging from 0.31 to 0.69 eV. Furthermore, the magnetoelectric coupling properties of Cux@bi-CrI3 can be modulated via varying the metal ion intercalation density, and half-metal to semiconductor transition can be occurred by decreasing the intercalation density of metal ions. Our work paves a practical path for 2D magnetoelectron coupling devices.

Effects of Rashba and Dresselhaus spin-orbit couplings on the critical temperature and paramagnetic limiting field of superconductors with broken inversion symmetry

Transition temperature (Tc) and paramagnetic limiting of a superconductor without spatial inversion symmetry in the presence of both Rashba and Dresselhaus antisymmetric spin-orbit couplings is studied. The critical temperature is derived for anisotropy of the superconducting order parameter, ranging from isotropic s-wave to any pairing state with nonzero angular momentum and mixed parity singlet-triplet states emerge due to spin-orbit coupling (SOC). It will be shown that for unprotected odd parity pairing, pure Rashba and Dresselhaus SOCs have similar effects on the reduction of Tc and for combined effects of the two spin-orbit couplings at fixed SOC, Tc reduced by increasing Dresselhaus component and decreased down to its minimum value in the equal-Rashba-Dresselhaus case. The paramagnetic limiting is also analyzed for spin-singlet pairing and it is shown that the low temperature divergence behavior of paramagnetic limiting is less affected by both Rashba and Dresselhaus SOCs but for fixed SOC strength by increasing Dresselhaus component the paramagnetic limiting field is increased.

Nonlinear Valley Hall Effect.

The valley Hall effect arises from valley-contrasting Berry curvature and requires inversion symmetry breaking. Here, we propose a nonlinear mechanism to generate a valley Hall current in systems with both inversion and time-reversal symmetry, where the linear and second-order charge Hall currents vanish along with the linear valley Hall current. We show that a second-order valley Hall signal emerges from the electric field correction to the Berry curvature, provided a valley-contrasting anisotropic dispersion is engineered. We demonstrate the nonlinear valley Hall effect in tilted massless Dirac fermions in strained graphene and organic semiconductors. Our Letter opens up the possibility of controlling the valley degree of freedom in inversion symmetric systems via nonlinear valleytronics.

Light-induced switching between singlet and triplet superconducting states

While the search for topological triplet-pairing superconductivity has remained a challenge, recent developments in optically stabilizing metastable superconducting states suggest a new route to realizing this elusive phase. Here, we devise a testable theory of competing superconducting orders that permits ultrafast switching to an opposite-parity superconducting phase in centrosymmetric crystals with strong spin-orbit coupling. Using both microscopic and phenomenological models, we show that dynamical inversion symmetry breaking with a tailored light pulse can induce odd-parity (spin triplet) order parameter oscillations in a conventional even-parity (spin singlet) superconductor, which when driven strongly can send the system to a competing minimum in its free energy landscape. Our results provide new guiding principles for engineering unconventional electronic phases using light, suggesting a fundamentally non-equilibrium route toward realizing topological superconductivity.

Chiral Magnetic Phases in Moire Bilayers of Magnetic Dipoles

AbstractIn magnetic insulators, the sense of rotation of the magnetization is associated with novel phases of matter and exotic transport phenomena. Aimed to find new sources of chiral magnetism rooted in intrinsic fields and geometry, twisted square bilayers of magnetic dipoles with easy plane anisotropy are studied. For no twist, each lattice settles in the zig‐zag magnetic state and orders antiferromagnetically to the other layer. The moire patterns that result from the mutual rotation of the two square lattices influence such zig‐zag order, giving rise to several phases that depict non‐collinear magnetic textures with chiral motifs that break both time and inversion symmetry. For certain moire angles, helical and toroidal magnetic orders arise. Changing the vertical distance between layers can further manipulate these novel phases. It is shown that the dipolar interlayer interaction induces an emergent twist‐dependent chiral magnetic field orthogonal to the direction of the zig‐zag chains, which is responsible for the internal torques conjugated to the toroidal orders.

Altermagnetic lifting of Kramers spin degeneracy

Lifted Kramers spin degeneracy (LKSD) has been among the central topics of condensed-matter physics since the dawn of the band theory of solids1,2. It underpins established practical applications as well as current frontier research, ranging from magnetic-memory technology3–7 to topological quantum matter8–14. Traditionally, LKSD has been considered to originate from two possible internal symmetry-breaking mechanisms. The first refers to time-reversal symmetry breaking by magnetization of ferromagnets and tends to be strong because of the non-relativistic exchange origin15. The second applies to crystals with broken inversion symmetry and tends to be comparatively weaker, as it originates from the relativistic spin–orbit coupling (SOC)16–19. A recent theory work based on spin-symmetry classification has identified an unconventional magnetic phase, dubbed altermagnetic20,21, that allows for LKSD without net magnetization and inversion-symmetry breaking. Here we provide the confirmation using photoemission spectroscopy and ab initio calculations. We identify two distinct unconventional mechanisms of LKSD generated by the altermagnetic phase of centrosymmetric MnTe with vanishing net magnetization20–23. Our observation of the altermagnetic LKSD can have broad consequences in magnetism. It motivates exploration and exploitation of the unconventional nature of this magnetic phase in an extended family of materials, ranging from insulators and semiconductors to metals and superconductors20,21, that have been either identified recently or perceived for many decades as conventional antiferromagnets21,24,25.

Directing valley-polarized emission of 3 L WS2 by photonic crystal with directional circular dichroism.

The valley degree of freedom that results from broken inversion symmetry in two-dimensional (2D) transition-metal dichalcogenides (TMDCs) has sparked a lot of interest due to its huge potential in information processing. In this experimental work, to optically address the valley-polarized emission from three-layer (3 L) thick WS2 at room temperature, we employ a SiN photonic crystal slab that has two sets of holes in a square lattice that supports directional circular dichroism engendered by delocalized guided mode resonances. By perturbatively breaking the inversion symmetry of the photonic crystal slab, we can simultaneously manipulate s and p components of the radiating field so that these resonances correspond to circularly polarized emission. The emission of excitons from distinct valleys is coupled into different radiative channels and hence separated in the farfield. This directional exciton emission from selective valleys provides a potential route for valley-polarized light emitters, which lays the groundwork for future valleytronic devices.