Sublattice Structure Research Articles

In-Sublattice Carrier Transition Enabled Polarimetric Photodetectors with Reconfigurable Polarity Transition.

Miniaturized polarimetric photodetectors based on anisotropic two-dimensionalmaterials attract potential applications in ultra-compact polarimeters. However, these photodetectors are hindered by the small polarization ratio values and complicated artificial structures. Here, a novel polarization photodetector based on in-sublattice carrier transition in the CdSb2Se3Br2/WSe2 heterostructure, with a giant and reconfigurable PR value, is demonstrated. The unique periodic sublattice structure of CdSb2Se3Br2 features an in-sublattice carrier transition preferred along Sb2Se3 chains. Leveraging on the in-sublattice carrier transition in the CdSb2Se3Br2/WSe2 heterostructure, gate voltage has an anisotropic modulation effect on the band alignment of heterostructure along sublattice. Consequently, the heterostructure exhibits a polarization-tunable photo-induced threshold voltage shift, which provides reconfigurable PR values from positive (unipolar regime) to negative (bipolar regime), covering all possible numbers (1→+∞/-∞→-1). Using this anisotropic photovoltaic effect, gate-tunable polarimetric imaging is successfully implemented. This work provides a new platform for developing next-generation highly polarimetric optoelectronics.

Sublattice Structure and Topology in Spontaneously Crystallized Electronic States.

The prediction and realization of the quantum anomalous Hall effect are often intimately connected to honeycomb lattices in which the sublattice degree of freedom plays a central role in the nontrivial topology. Two-dimensional Wigner crystals, on the other hand, form triangular lattices without sublattice degrees of freedom, resulting in a topologically trivial state. Here, we discuss the possibility of spontaneously formed honeycomb-lattice crystals that exhibit the quantum anomalous Hall effect. Starting from a single-band system with nontrivial quantum geometry, we derive the mean-field energy functional of a class of crystal states and express it as a model of sublattice pseudospins in momentum space. We find that nontrivial quantum geometry leads to extra terms in the pseudospin model that break an effective "time-reversal symmetry" and favor a topologically nontrivial pseudospin texture. When the effects of these extra terms dominate over the ferromagnetic exchange coupling between pseudospins, the anomalous Hall crystal state becomes energetically favorable over the trivial Wigner crystal state.

Cu1.94S-ZnS-CdS ternary heteronanoplates with efficient carrier transfer for enhanced photocatalytic hydrogen evolution

Incorporating precise morphology control and efficient carrier separation into single-nanoparticle heterojunctions to achieve high photocatalytic efficiency remains a significant challenge. Here, we synthesized Cu1.94S-ZnS-CdS ternary heteronanoplates (HNPs) with a continuous sublattice structure using cation exchange reactions. Femtosecond transient absorption spectroscopy (TAS) confirms that ternary heterojunction enhances carrier separation efficiency, demonstrating both rapid separation (∼0.2 ps) and an extended lifetime (∼1512 ps). The synergistic combination results in a significantly enhanced hydrogen evolution rate of 2.012 mmol·g−1·h−1, which is 17 times and 183 times higher than that achieved by pure CdS and ZnS, respectively. Furthermore, there is no significant decrease in the activity of Cu1.94S-ZnS-CdS in photocatalytic hydrogen evolution after 288 days of placement. Our work offers an alternative approach for designing noble-metal-free photocatalysts with precisely defined materials and interfaces, aiming to enhance both photocatalytic hydrogen evolution efficiency and stability.

Exploring the low-temperature polarization and the multifield-manipulated dielectric tunability behavior of NiMn2O4

Manganese oxides with spinel structure could exhibit abundant physical effects due to the complex sublattice structure, variable valence states and the intricate roles of manganese cations in magnetic interaction. In this work, NiMn2O4 ceramic with space group of Fd3‾m is synthesized. The low-temperature polarization behavior is investigated accompanied by revealing the multi-stage dielectric relaxation. Moreover, the relaxation mechanism is confirmed through microstructure characterization, multiple-condition pyroelectric measurement and the dielectric tunability properties under electric/magnetic fields. With increasing measuring temperature, different relaxation phenomena are respectively induced by lattice distortion because of the competition among magnetic coupling interactions (below ∼135 K), electron hopping relating to the coexistence of different valence states of manganese ions (∼135–230 K), and the synergistic contribution of oxygen vacancies and domain wall effect (above ∼230 K). These results provide additional evidence for comprehensive understanding the low-temperature polarization in NiMn2O4, guiding the method design for exploring the physical origin within a wide temperature range.

Planar triangular lattice of the LuMgGaO4: Clustered site-occupancy and the upconversion luminescence of the co-doped Er,Yb ions

The ordered and stable structure of inorganic lattice is the basis of constructing high-efficiency rare earth activated fluorescence, solid-state laser or other optical materials. The mixed sensitized and activated rare earth ions usually keeps a uniform space-occupying and the energy transfer depends much on the doping concentration, while the aggregation of rare earth dopants in order is rare. In this work, a series of LuMgGaO4 phosphors were synthesized and the detail lattice parameters are analyzed through Vietveld refinement and the new CIF file is provided. The site-occupancy of Er3+, Yb3+ shows clustered features and the Er–Yb sublattice structure with various Yb/Er ratios were constructed on the basis of planar triangular lattice. The long-distance excitation energy migration to lattice or defects can be effectively inhibited in case of the hexagonal circle Er-6Yb sublattice, in which the most intense green/red UCL was obtained. All the results demonstrate the novelty of regulating ordered site-occupancy of rare earth ions on a compact planar triangular lattice with higher efficiency of energy migration, which will pave a way for developing phosphor-converted materials or laser materials with better performance.

Study on the rapid synthesis of high-entropy carbonitride powder and its remarkable hardening effects on cemented carbide tool materials

As a novel high-entropy ceramic material with a multi-cation and multi-anion sublattice structure, high-entropy carbonitride ceramics (HECNs) have exhibited outstanding comprehensive properties and attracted increasing attention. In this study, a new WC-based cemented carbide material reinforced by high-entropy carbonitride (Ti0.2W0.2Mo0.2V0.2Nb0.2)(C0.7N0.3) (marked as HECN) was successfully fabricated by vacuum hot-pressed sintering. The mutual constraints between hardness and fracture toughness in extant WC-Co cemented carbide tool materials and their deficient high-temperature mechanical properties were effectively addressed. Moreover, for the low efficiency of the traditional carbothermal reduction nitridation, a novel method for rapidly preparing HECN powder was firstly proposed, namely the microwave-assisted carbothermal reduction nitridation, which could accelerate the heating rate and shorten the holding time. Single-phase HECN powder was successfully synthesized by this method, and the impacts of varying HECN content on the room and high-temperature mechanical properties of WC-based cemented carbide were investigated combined with the microstructure analysis by XRD\\SEM. The results revealed that HECN effectively inhibited the grain growth of WC in cemented carbide, and the refined WC grains provided a high-volume fraction of grain boundaries, which prevented dislocation movement and increased the hardness. With the optimized HECN content of 10 wt%, the Vickers hardness and fracture toughness of WC-HECN-Co composite reached 21.58 ± 0.36 GPa and 12.27 ± 1.17 MPa∙m1/2 respectively. Furthermore, WC-10HECN-10Co composites possessed outstanding high-temperature hardness and maintained a high hardness value of 13.16 ± 0.30 GPa at 800 °C, 37% higher than that of WC-10Co. The findings of this research hold significant practical implications for applying cemented carbide cutting tools in high-speed dry cutting.

Pt-CsPbBr3 Perovskite Nanocrystal Heterostructures: All Epitaxial.

Designing heterostructures of soft ionic nanocrystals with metallic or covalent nanostructures having epitaxial junctions in solution poses several fundamental challenges. Hence, in spite of large successes in developing lead halide perovskite nanocrystals, the chemistry of formation of their facet-directive epitaxial growth of noble metals cannot be explored yet. To address this, herein, epitaxial heterostructures of orthorhombic CsPbBr3 and cubic Pt in multiple directional approaches are reported. Appropriate facets of perovskite nanocrystals and high-temperature reaction are the key parameters for obtaining such nanocrystal heterostructures. Interfacial planes at the junctions having ideal lattice matching helped in establishing the epitaxial relations of (110) of orthorhombic (space group Pbnm) CsPbBr3 with {020} of cubic Pt and again (011) of CsPbBr3 with {111} of Pt. These results provided strong fundamental insights that ionic halide perovskite nanostructures and materials having different crystal phases can be placed in a single building block with continuous sublattice structures.

Improvement on cyclic stability of AB4-type La–Mg–Ni-based hydrogen storage alloys via merging Y element for nickel-metal hydride batteries

The newly discovered AB4-type superlattice structure of rare earth–Mg–Ni-based (RE–Mg–Ni) alloys have extended cycle life and power performance, which are a promising anode material for nickel-metal hydride (Ni/MH) battery. However, the cycling stability still needs to be enhanced to meet the requirement of utilization. Herein, we design low cost single-phase AB4-type alloys and clarify the effect of merging Y on Mg on the electrochemical performance. Studies show that the cycling stability of the alloy is significantly enhanced after partial replacement of Y on Mg, where the discharge capacity of the La0.65Sm0.12Y0.10Mg0.13Ni3.60Al0.15 alloy maintains 234.5 mAh g−1 after cycling 500 times with a capacity retention of 61.8%, in contrast to 191.6 mAh g−1 with 50.6% of the La0.65Sm0.12Mg0.23Ni3.60Al0.15 alloy. The prolonged cycling life relates to the reduction of pulverization due to the increased matching degree of the sublattice structure, and the prevention of oxidation in terms of the oxide film of Y. Whereas, the discharge ability at high rates and low temperatures of the alloy are deteriorated after Y replacement. The results pave the way to the component design of the RE–Mg–Ni-based alloys for long-life Ni/MH batteries.

The phase diagram of the next-neighbour Ising model of the face-centred cubic lattice

We use Monte Carlo simulation to determine the stable structures in the second-neighbour Ising model on the face-centred cubic lattice. Those structures are for strongly antiferromagnetic second-neighbour interactions and for ferromagnetic and weakly antiferromagnetic second neighbours. We find a third stable “intermediate” antiferromagnetic phase with symmetry, and calculate the paramagnetic transition temperature for each. The transition temperature depends strongly on second-neighbour interactions which are not frustrated. We determine a sublattice structure suitable for solving this problem with mean-field theory.

Spin-current generation from local spin polarization induced by current through local inversion asymmetry: Double quantum well structure

The current-induced spin polarization (CISP) in a system without the inversion symmetry is known to efficiently generate the spin current. In this paper we propose another approach, generating the spin current from the CISP locally arising in a system with the inversion symmetry in the form of the antiparallel CISP in sublattice structure. In this approach the local CISP is extracted from one of sublattices by a selective contact between the sublattice and an electrode. As the simplest system with such antiparallel CISP, we consider a symmetric double-quantum-well structure (DQWS) and calculate the antiparallel CISP and the spin current to a metallic layer in parallel contact with one well of the DQWS using the Boltzmann equation in the relaxation time approximation. When the Fermi energy is large enough that the first-excited sub-band is occupied, the magnitude of the spin current, which is proportional to that of the antiparallel CISP, increases with the interwell tunnel coupling and reaches twice the value of the decoupled quantum well with the broken inversion symmetry. Such an estimate suggests that inversion-symmetric systems can be useful in generating the spin current if the inversion symmetry is locally broken.

Nanoionics from a quantum mechanics point of view: Mathematical modeling and numerical simulation

Solid nano-structures exhibiting fast ion transport (cations moving in anionic crystal structures) are becoming increasingly relevant in industrial applications. However, it is challenging to model their mechanics due to the presence of electromagnetic couplings. In this paper, a mathematical, physical, and computational framework is introduced, for a cation particle moving through an anion sub-lattice structure in the presence of two electromagnetic fields: an external electromagnetic field; and a self-induced electromagnetic field coming from back-reaction phenomena caused by the relative movement of cations with respect to the mentioned structure. Our approach seeks to incorporate magnetic effects, such as magnetic induction and spin of cations, which are not incorporated in other models, mainly due to the intrinsic difficulty of 3D effects. We propose a quantum mechanical formalism based on a Schrödinger-type equation, where a wave function models the behavior of a cation in presence of an external electromagnetic potential, coupled with transient and self-induced electromagnetic effects. To solve the model, a space–time coupled numerical scheme is presented, which allows the possibility of time-evolving electromagnetic effects. The technique uses finite-elements in space and time-marching schemes in time. While a time-explicit marching scheme is used to update the magnetic and electric-potential fields, a time-implicit marching scheme is used to solve the coupled Schrödinger equation. This strategy allows us to update the electromagnetic contributions and wave functions at each time-step. Numerical examples in one and two spatial dimensions (and evolving in time) have been implemented for some meaningful models obtained from nanoionics literature.

Hidden Zeeman-type spin polarization in bulk crystals

Exploring hidden effects that have been overlooked given the nominal global crystal symmetry but are indeed visible in solid-state materials has been a fascinating subject of research recently. Here, we introduce a novel hidden Zeeman-type spin polarization (HZSP) in nonmagnetic bulk crystals with sublattice structures. In the momentum space of these crystals, the doubly degenerate bands formed in a certain plane can exhibit a uniform spin configuration with opposite spin orientations perpendicular to this plane, whereas such degenerate states are spatially separated in a pair of real-space sectors. Interestingly, we find that HZSP can manifest itself in both centrosymmetric and non-centrosymmetric materials. We further demonstrate the important role of nonsymmorphic twofold screw-rotational symmetry played in the formation of HZSP. Moreover, two representative material examples, i.e., centrosymmetric WSe$_2$ and noncentrosymmetric BaBi$_4$O$_7$, are identified to show HZSP via first-principles calculations. Our finding thus not only opens new perspectives for hidden spin polarization research but also significantly broadens the range of materials towards spintronics applications.

Unlocking AlN Piezoelectric Performance with Earth‐Abundant Dopants

AbstractThe increasing demand for high‐performance piezoelectric materials and toxicity and thermal stability issues of the widely used lead zirconate titanates (PZT) have spurred a search for better alternatives in electronic devices. In comparison to PZT, group III nitrides such as aluminum nitride (AlN), are only weakly piezoelectric, but doping AlN with scandium (Sc) improves the piezoelectric response by nearly 500%. Relative to PZT, doped‐AlN piezoelectric materials are advantageous because they are far more compatible with complementary metal–oxide–semiconductor (CMOS) materials, and they maintain both piezoelectric and thermodynamic stability up to very high temperatures. Unfortunately, rare‐earth metals are notoriously expensive, and fabricating stable films with rare‐earth dopants is also challenging, limiting their use in industrial applications. In this work, ab initio calculations are combined with targeted fabrication and experimentation to identify alternative earth‐abundant dopants for AlN from the periodic table d‐block. Amongst the 23 elements screened, it is found that group IVB metals, titanium, zirconium, and hafnium induce large piezoelectric enhancements comparable to Sc. This improvement is traced to shifts in the atomic sublattice structure and changes in the local charge states. In demonstrating a highly accessible and affordable path for technological adaptation of AlN‐based piezoelectrics, this work provides the foundation for sustainable, next‐generation electronics.

Formation of CuO$_2$ sublattices by suppression of interlattice correlations in tetragonal CuO

We investigate the tetragonal phase of the binary transition metal oxide CuO (t-CuO) within the context of cellular dynamical mean-field theory. Due to its strong antiferromagnetic correlations and simple structure, analysing the physics of t-CuO is of high interest as it may pave the way towards a more complete understanding of high-temperature superconductivity in hole-doped antiferromagnets. In this work we give a formal justification for the weak-coupling assumption that has previously been made for the interconnected sublattices within a single layer of t-CuO by studying the non-local self-energies of the system. We compute momentum-resolved spectral functions using a Matrix Product State (MPS)-based impurity solver directly on the real axis, which does not require any numerically ill-conditioned analytic continuation. The agreement with photoemission spectroscopy indicates that a single-band Hubbard model is sufficient to capture the material’s low energy physics. We perform calculations on a range of different temperatures, finding two magnetic regimes, for which we identify the driving mechanism behind their respective insulating state. Finally, we show that in the hole-doped regime the sublattice structure of t-CuO has interesting consequences on the symmetry of the superconducting state.

Lithium-rich diamond-like solid electrolytes for lithium batteries

Materials with diamond-like structure possess large cavity sites for excess lithium ions, making them have good lithium-ion transport properties. In this work, first-principles calculations are applied to study the structurally thermal stability, electrochemical stability, and lithium-ion migration kinetics of this class of materials. Our calculation results screen out four very promising solid state electrolytes Li15Zn0.5Ge4S16, Li15Zn0.5Ge4Se16, Li15Zn0.5Sn4Se16 and Li14ZnSn4S16, which are all three-dimension conductors of lithium ions and exhibit superior ionic conductivities of 4.682, 6.032, 22.963 and 13.077 mS/cm at 300 K respectively. Among them, sulfides Li15Zn0.5Ge4S16 and Li14ZnSn4S16 exhibit properties comparable to Li10GeP2S10, and selenides Li15Zn0.5Ge4Se16 and Li15Zn0.5Sn4Se16 can be well applied to Li-Se all-solid-state batteries because of their oxidation products including Se and other Selenides as well as the great interface stability with Selenide cathode. In addition, all these materials have the hcp anionic sublattice structure, meaning that the selection range of super lithium-ion conductor is expanded. Our study develops a new class of promising materials as solid state electrolytes for lithium batteries.

Engineering Floquet dynamical quantum phase transitions

Floquet dynamical quantum phase transitions (FDQPTs) are signified by recurrent nonanalytic behaviors of observables in time. In this work, we introduce a quench-free and generic approach to engineer and control FDQPTs for both pure and mixed Floquet states. By applying time-periodic modulations with two commensurate driving frequencies to a general class of spin chain model, we find multiple FDQPTs within each driving period. The nonanalytic cusps of return probability form sublattice structures in time domain. Notably, the number and time-locations of these cusps can be flexibly controlled by tuning the Hamiltonian parameter and the higher frequency of the drive. We further employ the dynamical topological order parameter (DTOP), which shows a quantized jump whenever a DQPT happens, to identify the topological feature of FDQPTs. Our findings reveal the advantage of engineering nonequilibrium phase transitions with multi-frequency driving fields.

Dipolar Bose-Hubbard model in finite-size real-space cylindrical lattices

Recent experimental progress in magnetic atoms and polar molecules has created the prospect of simulating dipolar Hubbard models with off-site interactions. When applied to real-space cylindrical optical lattices, these anisotropic dipole-dipole interactions acquire a tunable spatially-dependent component while they remain translationally-invariant in the axial direction, creating a sublattice structure in the azimuthal direction. We numerically study how the coexistence of these classes of interactions affects the ground state of hardcore dipolar bosons at half-filling in a finite-size cylindrical optical lattice with octagonal rings. When these two interaction classes cooperate, we find a solid state where the density order is determined by the azimuthal sublattice structure and builds smoothly as the interaction strength increases. For dipole polarisations where the axial interactions are sufficiently repulsive, the repulsion competes with the sublattice structure, significantly increasing entanglement and creating two distinct ordered density patterns. The spatially-varying interactions cause the emergence of these ordered states in small lattices as a function of interaction strength to be staggered according to the azimuthal sublattices.

Bound states at partial dislocation defects in multipole higher-order topological insulators

The bulk-boundary correspondence, which links a bulk topological property of a material to the existence of robust boundary states, is a hallmark of topological insulators. However, in crystalline topological materials the presence of boundary states in the insulating gap is not always necessary since they can be hidden in the bulk energy bands, obscured by boundary artifacts of non-topological origin, or, in the case of higher-order topology, they can be gapped altogether. Recently, exotic defects of translation symmetry called partial dislocations have been proposed to trap gapless topological modes in some materials. Here we present experimental observations of partial-dislocation-induced topological modes in 2D and 3D insulators. We particularly focus on multipole higher-order topological insulators built from circuit-based resonator arrays, since crucially they are not sensitive to full dislocation defects, and they have a sublattice structure allowing for stacking faults and partial dislocations.

Tight-binding studies of uniaxial strain in T-graphene nanoribbons

The role of uniaxial strain in armchair, T-graphene nanoribbons (ATGNRs) with symmetric and asymmetric structures is investigated using a nearest-neighbour, tight-binding (TB) model. ATGNRs with structural symmetry and two a sub-lattice structure exhibit Dirac points at zero strain. Application of uniaxial strain to these systems induces multiple Dirac points under compression (up to −20% strain), with the number of these points commensurate with the number of tetra-carbon base-units along the width of the unit cell, accounting also for the mirror symmetry of the structure. Under tensile, uniaxial strain (up to 20% extension), the induced asymmetry in the carbon tetrabond results in the number of Dirac points being reduced, although a minimum number are preserved due to the fundamental mirror-symmetry of the symmetric ATGNR. Asymmetric ATGNRs, which are semiconductors, are shown to have tunable band-gaps that decrease as a function of increasing ribbon width and uniaxial strain. Uniaxial strain induces a single Dirac point at the band edge of these systems under high compression (16%), with the closing of the band gap linked to symmetry-induced perturbations in the structure that override the symmetry-breaking, gap-opening mechanisms. In summary, the TB model shows ATGNRs to have suitable device features for flexible electronics applications, such as band-gap tuning, and for the strain engineering of relativistic properties.

Decoding the conductance of disordered nanostructures: a quantum inverse problem

Obtaining conductance spectra for a concentration of disordered impurities distributed over a nanoscale device with sensing capabilities is a well-defined problem. However, to do this inversely, i.e., extracting information about the scatters from the conductance spectrum alone, is not an easy task. In the presence of impurities, even advanced techniques of inversion can become particularly challenging. This article extends the applicability of a methodology we proposed capable of extracting composition information about a nanoscale sensing device using the conductance spectrum. The inversion tool decodes the conductance spectrum to yield the concentration and nature of the disorders responsible for conductance fluctuations in the spectra. We present the method for simple one-dimensional systems like an electron gas with randomly distributed delta functions and a linear chain of atoms. We prove the generality and robustness of the method using materials with complex electronic structures like hexagonal boron nitride, graphene nanoribbons, and carbon nanotubes. We also go on to probe distribution of disorders on the sublattice structure of the materials using the proposed inversion tool.