Lack Of Inversion Symmetry Research Articles

Bulk Photovoltaic Effect in 2D Materials for Solar‐Power Harvesting

AbstractIt is highly desirable for exploring and discovering new materials and outcome‐based approaches to exceed the Shockley–Queisser limit for single‐junction photovoltaic cells. Low‐dimensional piezoelectric materials have the potential to generate the optoelectronic phenomenon called the bulk photovoltaic effect, which is not limited by the theoretical limit for solar radiation into electricity conversion. The recent development of 2D materials has demonstrated that by using the bulk photovoltaic effect (BPVE) for crystals lacking inversion symmetry, it is possible to overcome this limit. So far, the exploration of p–n junction designs has been addressed in several review articles. However, the mechanism of BPVE differs from traditional p–n junction‐based photovoltaics in 2D materials. In this focused review, various concepts regarding the shift‐current response are explored, both from theoretical and experimental points of view, which are generated in the framework of deformed 2D materials. Finally, prospective approaches for building BPVE‐based next‐generation solar cells using ultrathin 2D materials are presented. These materials are expected to work better than current methods of turning energy into electricity.

Large Spin-To-Charge Conversion at the Two-Dimensional Interface of Transition-Metal Dichalcogenides and Permalloy.

Spin-to-charge conversion is an essential requirement for the implementation of spintronic devices. Recently, monolayers (MLs) of semiconducting transition-metal dichalcogenides (TMDs) have attracted considerable interest for spin-to-charge conversion due to their high spin-orbit coupling and lack of inversion symmetry in their crystal structure. However, reports of direct measurement of spin-to-charge conversion at TMD-based interfaces are very much limited. Here, we report on the room-temperature observation of a large spin-to-charge conversion arising from the interface of Ni80Fe20 (Py) and four distinct large-area (∼5 × 2 mm2) ML TMDs, namely, MoS2, MoSe2, WS2, and WSe2. We show that both spin mixing conductance and the Rashba efficiency parameter (λIREE) scale with the spin-orbit coupling strength of the ML TMD layers. The λIREE parameter is found to range between -0.54 and -0.76 nm for the four ML TMDs, demonstrating a large spin-to-charge conversion. Our findings reveal that the TMD/ferromagnet interface can be used for efficient generation and detection of spin current, opening new opportunities for novel spintronic devices.

Tunable Spin and Orbital Edelstein Effect at (111) LaAlO3/SrTiO3 Interface.

Converting charge current into spin current is one of the main mechanisms exploited in spintronics. One prominent example is the Edelstein effect, namely, the generation of a magnetization in response to an external electric field, which can be realized in systems with lack of inversion symmetry. If a system has electrons with an orbital angular momentum character, an orbital magnetization can be generated by the applied electric field, giving rise to the so-called orbital Edelstein effect. Oxide heterostructures are the ideal platform for these effects due to the strong spin–orbit coupling and the lack of inversion symmetries. Beyond a gate-tunable spin Edelstein effect, we predict an orbital Edelstein effect an order of magnitude larger then the spin one at the (111) LaAlO/SrTiO interface for very low and high fillings. We model the material as a bilayer of orbitals using a tight-binding approach, whereas transport properties are obtained in the Boltzmann approach. We give an effective model at low filling, which explains the non-trivial behaviour of the Edelstein response, showing that the hybridization between the electronic bands crucially impacts the Edelstein susceptibility.

Observation of Néel-type skyrmions in acentric self-intercalated Cr1+δTe2

Transition-metal dichalcogenides intercalated with 3d-transition metals within the van der Waals (vdW) gaps have been the focus of intense investigations owing to their fascinating structural and magnetic properties. At certain concentrations the intercalated atoms form ordered superstructures that exhibit ferromagnetic or anti-ferromagnetic ordering. Here we show that the self-intercalated compound Cr1+δTe2 with δ ≈ 0.3 exhibits a new, so far unseen, three-dimensionally ordered (2×2×2) superstructure. Furthermore, high resolution X-ray diffraction reveals that there is an asymmetric occupation of the two inequivalent vdW gaps in the unit cell. The structure thus lacks inversion symmetry, which, thereby, allows for chiral non-collinear magnetic nanostructures. Indeed, Néel-type skyrmions are directly observed using Lorentz transmission electron microscopy. The skyrmions are stable within the accessible temperature range (100–200 K) as well as in zero magnetic field. The diameter of the Néel skyrmions increases with lamella thickness and varies with applied magnetic field, indicating the role of long-range dipole fields. Our studies show that self-intercalation in vdW materials is a novel route to the formation of synthetic non-collinear spin textures.

Ising and XY paramagnons in two-dimensional 2H−NbSe2

Paramagnons are the collective modes that govern the spin response of nearly magnetic conductors. In some cases they mediate electron pairing leading to superconductivity. This scenario may occur in 2H-NbSe$_2$ monolayers, that feature spin-valley coupling on account of spin-orbit interactions and their lack of inversion symmetry. Here we explore spin anisotropy of paramagnons both for non-centrosymmetric Kane-Mele-Hubbard models for 2H-NbSe$_2$ monolayers described with a DFT-derived tight-binding model. In the infinite wavelength limit we find spatially uniform paramagnons with energies around $1$~meV that feature a colossal off-plane uniaxial magnetic anisotropy, with quenched transversal spin response. At finite wave vectors, longitudinal and transverse channels reverse roles: XY fluctuations dominate within a significant portion of the Brillouin zone. Our results show that 2H-NbSe$_2$ is close to a Coulomb-driven in-plane (XY) spin density wave instability.

Colossal Orbital Edelstein Effect in Noncentrosymmetric Superconductors.

In superconductors that lack inversion symmetry, the flow of supercurrent can induce a nonvanishing magnetization, a phenomenon which is at the heart of nondissipative magnetoelectric effects, also known as Edelstein effects. For electrons carrying spin and orbital moments, a question of fundamental relevance deals with the orbital nature of magnetoelectric effects in conventional spin-singlet superconductors with Rashba coupling. Remarkably, we find that the supercurrent-induced orbital magnetization is more than 1 order of magnitude greater than that due to the spin, giving rise to a colossal magnetoelectric effect. The induced orbital magnetization is shown to be sign tunable, with the sign change occurring for the Fermi level lying in proximity of avoiding crossing points in the Brillouin zone. In the presence of superconducting phase inhomogeneities, a modulation of the Edelstein signal on the scale of the superconducting coherence length appears, leading to domains with opposite orbital moment orientations. These hallmarks are robust to real-space self-consistent treatment of the superconducting order parameter. The orbital-dominated magnetoelectric phenomena, hence, have clear-cut marks for detection both in the bulk and at the edge of the system and are expected to be a general feature of multiorbital superconductors with inversion symmetry breaking.

Optical second-harmonic generation of Janus MoSSe monolayer

The transition metal dichalcogenides (TMD) monolayers have shown strong second-harmonic generation (SHG) owing to their lack of inversion symmetry. These ultrathin layers then serve as the frequency converters that can be intergraded on a chip. Here, taking MoSSe as an example, we report the first detailed experimental study of the SHG of Janus TMD monolayer, in which the transition metal layer is sandwiched by the two distinct chalcogen layers. It is shown that the SHG effectively arises from an in-plane second-harmonic polarization under paraxial focusing and detection. Based on this, the orientation-resolved SHG spectroscopy is realized to readily determine the zigzag and armchair axes of the Janus crystal with an accuracy better than ±0.6°. Moreover, the SHG intensity is wavelength-dependent and can be greatly enhanced (∼ 60 times) when the two-photon transition is resonant with the C-exciton state. Our findings uncover the SHG properties of Janus MoSSe monolayer, therefore lay the basis for its integrated frequency-doubling applications.

Role of Shift Vector in High-Harmonic Generation from Noncentrosymmetric Topological Insulators under Strong Laser Fields

As a promising avenue to obtain new extreme ultraviolet light source and detect electronic properties, high-harmonic generation (HHG) has been actively developed in both theory and experiment. In solids lacking inversion symmetry, when electrons undergo a nonadiabatic transition, a directional charge shift occurs and is characterized by shift vector, which measures the real-space shift of the photoexcited electron and hole. For the first time, we have revealed that shift vector plays prominent roles in the real-space tunneling mechanism of three-step model for electrons under strong laser fields. Since shift vector is determined by the topological properties of related wave functions, we expect HHG with its contribution can provide direct knowledge on the band topology in noncentrosymmetric topological insulators (TIs). In both Kane-Mele model and realistic material BiTeI, we have found that the shift vector reverses when band inversion happens during the topological phase transition between normal and topological insulators. Under oscillating strong laser fields, the reversal of shift vector leads to completely opposite radiation time of high-order harmonics. This makes HHG a feasible all-optical strong-field method to directly identify the band inversion in non-centrosymmetric TIs.

Nanoampere‐Level Piezoelectric Energy Harvesting Performance of Lithography‐Free Centimeter‐Scale MoS2 Monolayer Film Generators

2D transition-metal dichalcogenides have been reported to possess piezoelectricity due to their lack of inversion symmetry; thus, they are potentially applicable as electromechanical energy harvesters. Herein, the authors propose a lithography-free piezoelectric energy harvester composed of centimeter-scale MoS2 monolayer films with an interdigitated electrode pattern that is enabled only by the large scale of the film. High-quality large-scale synthesis of the monolayer films is conducted by low-pressure chemical vapor deposition with the assistance of an unprecedented Na2 S promoter. The extra sulfur supplied by Na2 S critically passivates the sulfur vacancies. The energy harvester having a large active area of ≈18.3mm2 demonstrates an unexpectedly high piezoelectric energy harvesting performance of ≈400.4mV and ≈40.7nA under a bending strain of 0.57%, with the careful adjustment of side electrodes along the zigzag atomic arrays in the two dominant domain structure. Nanoampere-level harvesting has not yet been reported with any 2D material-based harvester.

Generation of pure spin-valley beams at controllable angles by gate voltage in monolayer molybdenum disulfide

Strong spin–orbit coupling and lack of inversion symmetry in monolayer transition metal dechalcogenides has made these materials as a promising candidate for both spintronic and valleytronic applications. We investigate the effect of adjustable parameters on quantum transmission of electrons through a magnetic barrier on MoS2 monolayer and introduce selection rules for generation of perfectly polarized spin-valley beams in various directions. These selection rules provide an efficient tool for versatile electrical manipulation of spin-valley beams in two-dimensional structures.

Spin-triplet superconductivity in Weyl nodal-line semimetals

Topological semimetals are three dimensional materials with symmetry-protected massless bulk excitations. As a special case, Weyl nodal-line semimetals are realized in materials having either no inversion or broken time-reversal symmetry and feature bulk nodal lines. The 111-family, including LaNiSi, LaPtSi and LaPtGe materials (all lacking inversion symmetry), belongs to this class. Here, by combining muon-spin rotation and relaxation with thermodynamic measurements, we find that these materials exhibit a fully-gapped superconducting ground state, while spontaneously breaking time-reversal symmetry at the superconducting transition. Since time-reversal symmetry is essential for protecting the normal-state topology, its breaking upon entering the superconducting state should remarkably result in a topological phase transition. By developing a minimal model for the normal-state band structure and assuming a purely spin-triplet pairing, we show that the superconducting properties across this family can be described accurately. Our results demonstrate that the 111 materials reported here provide an ideal test-bed for investigating the rich interplay between the exotic properties of Weyl nodal-line fermions and unconventional superconductivity.

Breaking Transmission Symmetry Without Breaking Reciprocity in Linear All-Dielectric Polarization-Preserving Metagratings

Transmission asymmetry in reciprocal systems offers an appealing alternative to bulkier nonreciprocal implementations for certain applications. Common reciprocal routes to transmission asymmetry of linearly polarized light involve a rotation of its polarization. Here, we explore a different route with a linear all-dielectric metagrating that preserves polarization, while lacking inversion symmetry along the surface-normal direction. Our all-angle transmission calculations reveal an abrupt transition from a symmetric to an asymmetric transmission response that traces the Bragg critical wavelength of higher-order beam emergence as a function of the incident angle. By adopting an analogy between scattering from a multiport network and the metagrating paradigm we establish why the only necessary condition for transmission symmetry breaking in this class of systems is the emergence of any higher-order Bragg diffracted beam. We further show how such a transmission symmetry breaking is consistent with reciprocity and also demonstrate the underpinning symmetry-breaking mechanism with a first-principles numerical experiment. Finally, we shed light on some previous misconceptions regarding transmission symmetry breaking related to the role of the substrate or need for change of diffraction order number at each interface. Our proposed metagrating can exhibit a strong transmission asymmetry, with contrast that can be as high as approximately 75%, thus underlining its potential as a blueprint for passive asymmetric or nonlinear self-biasing nonreciprocal metasurfaces relevant to integrated and active photonics.

Crossover between Bulk and Interface Photovoltaic Mechanisms in a Ferroelectric Vertical Heterostructure

The bulk photovoltaic (BPVE) effect in crystals lacking inversion symmetry offers great potential for optoelectronic applications due to its unique properties, such as above-band-gap photovoltage and switchable photocurrent. Because of their large spontaneous polarizations, ferroelectric materials are ideal platforms for studying the BPVE. However, identifying the origin of an experimentally observed photovoltaic response is often challenging due to the entanglement between bulk and interface effects, leading to much debate in the field. This issue is particularly pronounced in vertical heterostructures, where the two effects are comparable. Here, we report crossover between bulk- and interface-dominant responses in vertical ${\mathrm{Bi}\mathrm{Fe}\mathrm{O}}_{3}$ heterostructures when changing the photon energy. We show that well-above-band-gap excitation leads to a bulk photovoltaic response, but band-edge excitation requires interface band bending to separate the photocarriers. Our findings not only help to clarify contradicting reports in the literature, but also lay the foundation for a deeper understanding of the ferroelectric photovoltaic effect and its applications in various devices.

Trigonal-to-monoclinic structural transition in TiSe2 due to a combined condensation of q=(12,0,0) and (12,0,12) phonon instabilities

I present first principles calculations of the phonon dispersions of TiSe$_2$ in the $P\overline{3}c1$ phase, which is the currently accepted low-temperature structure of this material. They show weak instabilities in the acoustic branches in the out-of-plane direction, suggesting that this phase may not be the true ground state. To find the lowest energy structure, I study the energetics of all possible distorted structures corresponding to the isotropy subgroups of $P\overline{3}m1$ for the $M_1^-$ and $L_1^-$ phonon instabilities present in this high-temperature phase at $q = (\frac{1}{2},0,0)$ and $(\frac{1}{2},0,\frac{1}{2})$, respectively. I was able to stabilize 10 different structures that are lower in energy relative to the parent $P\overline{3}m1$ phase, including two monoclinic structures more energetically stable than the $P\overline{3}c1$ phase. The lowest energy structure has the space group $C2$ with the order parameter $M_1^- (a,0,0) + L_1^- (0,b,b)$. This structure lacks inversion symmetry, and its primitive unit cell has 12 atoms.

Electrical transport properties of atomically thin WSe2 using perpendicular magnetic anisotropy metal contacts

Tungsten diselenide, WSe2, shows excellent properties and becomes a very promising material among two-dimensional semiconductors. Wide bandgap and large spin–orbit coupling along with naturally lacking inversion symmetry in the monolayer WSe2 make it an efficient material for spintronics, optoelectronics, and valleytronics applications. In this work, we report electrical transport properties of a monolayer WSe2 based field effect transistor with most needed multilayer Co/Pt ferromagnetic electrodes exhibiting perpendicular magnetic anisotropy. We studied contact behavior by performing I-V curve measurements and estimating Schottky barrier heights (SBHs). SBHs estimated from experimental data are found to be comparatively small without using any tunnel barrier. This work expands the current understanding of WSe2 based devices and gives insight into the electrical behavior of Co/Pt metal contacts, which can open great possibilities for spintronic/valleytronic applications.

The role of nonlocal response in second harmonic generation at metasurfaces with triangular metaatoms

Metasurface consisting of square array of obtuse isosceles triangle metaatoms is found to exhibit much more efficient second harmonic generation (SHG) compared to that of split ring resonators and its heptagonal modification, experimentally as well as numerically. All of them are designed to lack inversion symmetry in horizontal direction but to have vertical symmetry, and to meet the double resonance condition for vertically-polarized fundamental and horizontally-polarized SHG waves. SHG efficiencies were estimated numerically for each structure by evaluating an overlap integral of second order nonlinear polarization and field distribution at the SHG wavelength. The large overlap integral for the triangle metasurface is ascribed to the nonlocal response at the SHG wavelength. Current induced at the center of the triangle near the obtuse angle by horizontally polarized light at SHG wavelength flows toward two corners of acute angles. As a result, polarization charges oscillate in time at the surfaces of two acute corners, which results in strong field oscillation away from the center where the electric field is applied to majority of free electrons. Experimentally observed wavelength dependence of SHG efficiencies for the three metasurfaces are reasonably reproduced by a numerical estimation.

Extreme in-plane upper critical magnetic fields of heavily doped quasi-two-dimensional transition metal dichalcogenides

Extreme in-plane upper critical magnetic fields $B_{c2//ab}$ strongly violating the Pauli paramagnetic limit have been observed in the misfit layer $(LaSe)_{1.14}(NbSe_2)$ and $(LaSe)_{1.14}(NbSe_2)_2$ single crystals with $T_c$ = 1.23 K and 5.7 K, respectively. The crystals show a two-dimensional to three-dimensional transition at temperatures slightly below $T_c$ with an upturn in the temperature dependence of $B_{c2//ab}$, a temperature dependent huge superconducting anisotropy and a cusplike behavior of the angular dependence of $B_{c2}$. Both misfits are characterized by a strong charge transfer from LaSe to $NbSe_2$. As shown in our previous work, $(LaSe)_{1.14}(NbSe_2)$ is electronically equivalent to the highly doped $NbSe_2$ monolayers. Then, the strong upper critical field can be attributed to the Ising coupling recently discovered in atomically thin transition metal dichalcogenides with strong spin-orbit coupling and a lack of inversion symmetry. A very similar behavior is found in $(LaSe)_{1.14}(NbSe_2)_2$, where the charge transfer is nominally twice as big, which could eventually lead to complete filling of the $NbSe_2$ conduction band and opening superconductivity in LaSe. Whatever the particular superconducting mechanism would be, a common denominator in both misfits is that they behave as a stack of almost decoupled superconducting atomic layers, proving that Ising superconductivity can also exist in bulk materials.

Resonant nonlinear response of a nanomechanical system with broken symmetry

We study the response of a weakly damped vibrational mode of a nanostring resonator to a moderately strong resonant driving force. Because of the geometry of the experiment, the studied flexural vibrations lack inversion symmetry. As we show, this leads to a nontrivial dependence of the vibration amplitude on the force parameters. For a comparatively weak force, the response has the familiar Duffing form, but for a somewhat stronger force, it becomes significantly different. Concurrently there emerge vibrations at twice the drive frequency, a signature of the broken symmetry. Their amplitude and phase allow us to establish the cubic nonlinearity of the potential of the mode as the mechanism responsible for both observations. The developed theory goes beyond the standard rotating-wave approximation. It quantitatively describes the experiment and allows us to determine the nonlinearity parameters.

Unconventional supercurrent phase in Ising superconductor Josephson junction with atomically thin magnetic insulator

In two-dimensional (2D) NbSe2 crystal, which lacks inversion symmetry, strong spin-orbit coupling aligns the spins of Cooper pairs to the orbital valleys, forming Ising Cooper pairs (ICPs). The unusual spin texture of ICPs can be further modulated by introducing magnetic exchange. Here, we report unconventional supercurrent phase in van der Waals heterostructure Josephson junctions (JJs) that couples NbSe2 ICPs across an atomically thin magnetic insulator (MI) Cr2Ge2Te6. By constructing a superconducting quantum interference device (SQUID), we measure the phase of the transferred Cooper pairs in the MI JJ. We demonstrate a doubly degenerate nontrivial JJ phase (ϕ), formed by momentum-conserving tunneling of ICPs across magnetic domains in the barrier. The doubly degenerate ground states in MI JJs provide a two-level quantum system that can be utilized as a new dissipationless component for superconducting quantum devices. Our work boosts the study of various superconducting states with spin-orbit coupling, opening up an avenue to designing new superconducting phase-controlled quantum electronic devices.

Light localization in one-dimensional photonic crystal heterostructures

Effects of both metamaterial inclusion and lack of inversion symmetry on the localized modes in one-dimensional photonic heterostructures under normal incidence are investigated. Each structure consists of two semi-infinite photonic crystals separated by an interface or by several layers. A general condition for light localization between semi-infinite crystals is given by parallelism between two-dimensional vectors in the electromagnetic (H, E) space. The case of a defective photonic crystal is recovered by joining crystals having the same unit cell. The defect modes display leftward and rightward damped oscillations with the same ratio, even when the unit cell lacks inversion symmetry. Their frequencies are found in good agreement with peaks of the transmittance through truncated structures. In heterostructures including metamaterials, an anomalous exponential decay of the magnetic field is found near one edge of the zero-〈n〉 gap.