quasi-1D Systems Research Articles

Broken symmetries in quasi-2D charged systems via negative dielectric confinement

We report spontaneous symmetry breaking (SSB) phenomena in symmetrically charged binary particle systems under planar nanoconfinement with negative dielectric constants. The SSB is triggered solely via the dielectric confinement effect, without any external fields. The mechanism of SSB is found to be caused by the strong polarization field enhanced by nanoconfinement, giving rise to charge/field oscillations in the transverse directions. Interestingly, dielectric contrast can even determine the degree of SSB in transverse and longitudinal dimensions, forming charge-separated interfacial liquids and clusters on square lattices. Furthermore, we analytically show that the formed lattice constant is determined by the dielectric mismatch and the length scale of confinement, which is validated via molecular dynamics simulations. The novel broken symmetry mechanism may provide new insights into the study of quasi-2D systems and the design of future nanodevices.

Vortex splitting in two-dimensional fluids and non-neutral electron plasmas with smooth vorticity profiles

Initially, elliptical, quasi-two-dimensional (2D) fluid vortices can split into multiple pieces if the aspect ratio is sufficiently large due to the growth and saturation of perturbations known as Love modes on the vortex edge. Presented here are experiments and numerical simulations, showing that the aspect ratio threshold for vortex splitting is significantly higher for vortices with realistic, smooth edges than that predicted by a simple “vortex patch” model, where the vorticity is treated as piecewise constant inside a deformable boundary. The experiments are conducted by exploiting the E × B drift dynamics of collisionless, pure electron plasmas in a Penning–Malmberg trap, which closely model 2D vortex dynamics due to an isomorphism between the Drift–Poisson equations describing the plasmas and the Euler equations describing ideal fluids. The simulations use a particle-in-cell method to model the evolution of a set of point vortices. The aspect ratio splitting threshold ranges up to about twice as large as the vortex patch prediction and depends on the edge vorticity gradient. This is thought to be due to spatial Landau damping, which decreases the vortex aspect ratio over time and, thus, stabilizes the Love modes. Near the threshold, asymmetric splitting events are observed in which one of the split products contains much less circulation than the other. These results are relevant to a wide range of quasi-2D fluid systems, including geophysical fluids, astrophysical disks, and drift-wave eddies in tokamak plasmas.

Vertically Concentrated Quantum Wells Enabling Highly Efficient Deep-Blue Perovskite Light-Emitting Diodes.

Deep-blue perovskite light-emitting diodes (PeLEDs) based on quasi-two-dimensional (quasi-2D) systems exist heightened sensitivity to the domain distribution. The top-down crystallization mode will lead to a vertical gradient distribution of quantum well (QW) structure, which is unfavorable for deep-blue emission. Herein, a thermal gradient annealing treatment is proposed to address the polydispersity issue of vertical QWs in quasi-2D perovskites. The formation of large-n domains at the upper interface of the perovskite film can be effectively inhibited by introducing a low-temperature source in the annealing process. Combined with the utilization of NaBr to inhibit the undesirable n=1 domain, a vertically concentrated QW structure is ultimately attained. As a result, the fabricated device delivers a narrow and stable deep-blue emission at 458 nm with an impressive external quantum efficiency (EQE) of 5.82 %. Green and sky-blue PeLEDs with remarkable EQE of 21.83 % and 17.51 % are also successfully achieved, respectively, by using the same strategy. The findings provide a universal strategy across the entire quasi-2D perovskites, paving the way for future practical application of PeLEDs.

Unexpected Two-Dimensional Polarons Induced by Oxygen Vacancies in Layered Structure MoO3-x.

Unveiling the effects of oxygen vacancies on the structural stability of layered α-MoO3 is critical for optimizing its physical and chemical properties. Herein, we present experimental evidence regarding the phase stability of α-MoO3 with ∼2% oxygen vacancy concentrations. Interestingly, we report a previously ignored oxygen-deficient orthorhombic MoO3-x phase in space group Cmcm. Further density functional theory calculations reveal a detailed phase transition mechanism from α-MoO3 to MoO3-x. More importantly, we demonstrate that two-dimensional (2D) large polarons must exist to stabilize the MoO3-x crystal structure. 2D large polarons are suspected to exist in numerous quasi-2D systems but have never been found in layered α-MoO3 or other molybdenum oxides. Our work contributes to a basic understanding of the polaronic behavior in MoO3-x and may broaden the application realm of molybdenum oxides.

Bubble self-organization in pulsed annular gas-solid fluidized beds

Pulsating the gas flow in rectangular, quasi-2D fluidized beds can turn the chaotic bubble flow into a regular bubble pattern. Bubbles form a rising triangular lattice, leading to a scalable flow structure with controllable properties, such as narrow bubble size distribution, distance between bubbles, and residence time. This overcomes challenges encountered in conventional units, like flow maldistribution and non-uniform contact. In this work, we reproduced a similar, dynamically structured flow in a cylindrical annular geometry. Regular bubble patterns emerge along the circumference of the cylinder. The absence of lateral walls and strongly curved boundaries could cause instabilities. This study presents an operating window for creating spatiotemporally structured flows and compares the flow properties in quasi-2D rectangular and annular systems, quantifying the impact of curvature and, effectively, lateral walls on flow behavior. These insights offer new opportunities for modularization of fluidized bed operations.

Emergent quasi-two-dimensional metallic state derived from the Mott-insulator framework

Recent quasi-two-dimensional (quasi-2D) systems with judicious exploitation of the atomic monolayer or few-layer architecture exhibit unprecedented physical properties that challenge the conventional wisdom on condensed matter physics. Here we show that the infinite layer ${\mathrm{SrCuO}}_{2}$ (SCO), a topical cuprate Mott insulator in bulk form, can manifest an unexpected metallic state in the quasi-2D limit when SCO is grown on ${\mathrm{TiO}}_{2}$-terminated ${\mathrm{SrTiO}}_{3}$ (STO) substrates. The sheet resistance does not conform to Landau's Fermi liquid paradigm. Hard x-ray core-level photoemission spectra demonstrate a definitive Fermi level that resembles the hole doped metal. Soft x-ray absorption spectroscopy also reveals features analogous to those of a hole doped Mott insulator. Based on these results, we conclude that the hole doping does not occur at the interfaces between SCO and STO; instead, it comes from the transient layers between the chain-type and the planar-type structures within the SCO slab. The present work reveals a metallic state in the infinite layer SCO and invites further examination to elucidate the spatial extent of this state.

Symmetry-Guaranteed High Carrier Mobility in Quasi-2D Thermoelectric Semiconductors.

Quasi-2D semiconductors have garnered immense research interest for next-generation electronics and thermoelectrics due to their unique structural, mechanical, and transport properties. However, most quasi-2D semiconductors experimentally synthesized so far have relatively low carrier mobility, preventing the achievement of exceptional power output. To break through this obstacle, a route is proposed based on the crystal symmetry arguments to facilitate the charge transport of quasi-2D semiconductors, in which the horizontal mirror symmetry is found to vanish the electron-phonon coupling strength mediated by phonons with purely out-of-plane vibrational vectors. This is demonstrated in ZrBeSi-type quasi-2D systems, where the representative sample Ba1.01 AgSb shows a high room-temperature hole mobility of 344 cm2 V-1 S-1 , a record value among quasi-2D polycrystalline thermoelectrics. Accompanied by intrinsically low thermal conductivity, an excellent p-type zT of ≈1.3 is reached at 1012 K, which is the highest value in ZrBeSi-type compounds. This work uncovers the relation between electron-phonon coupling and crystal symmetry in quasi-2D systems, which broadens the horizon to develop high mobility semiconductors for electronic and energy conversion applications.

Realization of quasi-1D topological magnetism at the V-alloyed MoS2 zigzag edge.

Topological magnetism in quasi-1D systems can be interesting because of the significant quantum confinement. However, the realization is missing. In this letter, we propose the use of 3× periodicities related edge reconstructions of MoS2 zigzag edges to construct a topological quasi-1D spin chain. Specifically, a trimer Su-Schrieffer-Heeger model can be applied to illustrate the topological and spin order when the inter-cell hopping integral is larger than the intra-cell ones. As a result, topological ferromagnetic order is achieved for S-oriented edge states magnetized by V atoms and confirmed by first-principles calculations and Wannier functions analysis. Finally, gap opening and spin-polarized end states are realized.

The Third Dimension of Ferroelectric Domain Walls.

Ferroelectric domain walls are quasi-2D systems that show great promise for the development of nonvolatile memory, memristor technology, and electronic components with ultrasmall feature size. Electric fields, for example, can change the domain wall orientation relative to the spontaneous polarization and switch between resistive and conductive states, controlling the electrical current. Being embedded in a 3Dmaterial, however, the domain walls are not perfectly flat and can form networks, which leads to complex physical structures. In this work, the importance of the nanoscale structure for the emergent transport properties is demonstrated, studying electronic conduction in the 3D network of neutral and charged domain walls in ErMnO3 . By combining tomographic microscopy techniques and finite element modeling, the contribution of domain walls within the bulk is clarified and the significance of curvature effects for the local conduction is shown down to the nanoscale. The findings provide insights into the propagation of electrical currents in domain wall networks, reveal additional degrees of freedom for their control, and provide quantitative guidelines for the design of domain-wall-based technology.

Sensitive multi-element profiling with high depth resolution enabled by time-of-flight recoil detection in transmission using pulsed keV ion beams

The potential of time-of-flight recoil detection for sensitive multi-element profiling of thin membranes and quasi-2D systems in transmission geometry using pulsed keV ion beams is assessed. While the time-of-flight approach allows for simultaneous detection of multiple elements, to the largest extent irrespective of recoil charge states, the keV projectile energies guarantee high recoil-cross sections yielding high sensitivity at low dose. We demonstrate the capabilities of the approach using 22Ne and 40Ar as projectiles transmitted through thin carbon foils featuring optional LiF-coatings and single-crystalline silicon membranes for different sample preparation routines and crystal orientations.Using a large position-sensitive detector (0.13 sr), a depth resolution below 6 nm and sensitivity below 1014 atoms/cm2 was achieved for H in a 50 nm thick silicon membrane. For crystalline targets, we show how the probability of creation and detection of recoils and their observed angular distribution depend on sample orientation.

Identifying the Correlation between Structural Parameters and Anisotropic Magnetic Properties in IMnV Semiconductors: A Possible Room-Temperature Magnetism.

Layer-structured materials are of central importance in a wide range of research fields owing to their unique properties originating from their two dimensionality and anisotropy. Herein, quasi-2D layer-structured IMnV (I: alkali metals and V: pnictogen elements) compounds are investigated, which are potential antiferromagnetic (AFM) semiconductors. Single crystals of IMnV compounds are successfully grown using the self-flux method and their electronic and magnetic properties are analyzed in correlation with structural parameters. Combined with theoretical calculations, the structural analysis indicates that the variation in the bonding angle between VMnV is responsible for the change in the orbital hybridization of Mn and V, predominantly affecting their anisotropic semiconducting properties. Anisotropy in the magnetic properties is also found, where AFM ordering is expected to occur in the in-plane direction, as supported by spin-structure calculations. Furthermore, a possible ferromagnetic (FM) transition is discussed in relation to the vacancy defects. This study provides a candidate material group for AFM and FM spintronics and a basis for exploring magnetic semiconductors in quasi-2D layer-structured systems.

Spatiotemporal Distribution of Precipitates and Mineral Phase Transition During Biomineralization Affect Porosity–Permeability Relationships

Enzymatically induced calcium carbonate precipitation is a promising geotechnique with the potential, for example, to seal leakage pathways in the subsurface or to stabilize soils. Precipitation of calcium carbonate in a porous medium reduces the porosity and, consequently, the permeability. With pseudo-2D microfluidic experiments, including pressure monitoring and, for visualization, optical microscopy and X-ray computed tomography, pore-space alterations were reliably related to corresponding hydraulic responses. The study comprises six experiments with two different pore structures, a simple, quasi-1D structure, and a 2D structure. Using a continuous injection strategy with either constant or step-wise reduced flow rates, we identified key mechanisms that significantly influence the relationship between porosity and permeability. In the quasi-1D structure, the location of precipitates is more relevant to the hydraulic response (pressure gradients) than the overall porosity change. In the quasi-2D structure, this is different, because flow can bypass locally clogged regions, thus leading to steadier porosity–permeability relationships. Moreover, in quasi-2D systems, during continuous injection, preferential flow paths can evolve and remain open. Classical porosity–permeability power-law relationships with constant exponents cannot adequately describe this phenomenon. We furthermore observed coexistence and transformation of different polymorphs of calcium carbonate, namely amorphous calcium carbonate, vaterite, and calcite and discuss their influence on the observed development of preferential flow paths. This has so far not been accounted for in the state-of-the-art approaches for porosity–permeability relationships during calcium carbonate precipitation in porous media.

Are strongly confined colloids good models for two dimensional liquids?

Quasi-two-dimensional (quasi-2D) colloidal hard-sphere suspensions confined in a slit geometry are widely used as two-dimensional (2D) model systems in experiments that probe the glassy relaxation dynamics of 2D systems. However, the question to what extent these quasi-2D systems indeed represent 2D systems is rarely brought up. Here, we use computer simulations that take into account hydrodynamic interactions to show that dense quasi-2D colloidal bi-disperse hard-sphere suspensions exhibit much more rapid diffusion and relaxation than their 2D counterparts at the same area fraction. This difference is induced by the additional vertical space in the quasi-2D samples in which the small colloids can move out of the 2D plane, therefore allowing overlap between particles in the projected trajectories. Surprisingly, this difference in the dynamics can be accounted for if, instead of using the surface density, one characterizes the systems by means of a suitable structural quantity related to the radial distribution function. This implies that in the two geometries, the relevant physics for glass formation is essentially identical. Our results provide not only practical implications on 2D colloidal experiments but also interesting insights into the 3D-to-2D crossover in glass-forming systems.

Insights into the anisotropic spin- S Kitaev chain

Recently there has been a renewed interest in properties of the higher-spin Kitaev models, especially their low-dimensional analogues with additional interactions. These quasi-1D systems exhibit rich phase diagrams with symmetry-protected topological phases, Luttinger liquids, hidden order, and higher-rank magnetism. However, the nature of the pure spin-$S$ Kitaev chains are not yet fully understood. Earlier works found a unique ground state with short-ranged correlations for $S = 1$, and an intriguing double-peak structure in the heat capacity associated with an entropy plateau. To understand the low-energy excitations and thermodynamics for general $S$ we study the anisotropic spin-$S$ Kitaev chain. Starting from the dimerized limit we derive an effective low-energy Hamiltonian at finite anisotropy. For half-integer spins we find a trivial effective model, reflecting a non-local symmetry protecting the degeneracy, while for integer $S$ we find interactions among the flux degrees of freedom that select a unique ground state. The effective model for integer spins is used to predict the low-energy excitations and thermodynamics, and we make a comparison with the semiclassical limit through linear spin wave theory. Finally, we speculate on the nature of the isotropic limit.

Staggered Mesh Method for Correlation Energy Calculations of Solids: Random Phase Approximation in Direct Ring Coupled Cluster Doubles and Adiabatic Connection Formalisms

We propose a staggered mesh method for correlation energy calculations of periodic systems under the random phase approximation (RPA), which generalizes the recently developed staggered mesh method for periodic second order Møller-Plesset perturbation theory (MP2) calculations [Xing; Li; Lin J. Chem. Theory Comput. 2021]. Compared to standard RPA calculations, the staggered mesh method introduces negligible additional computational cost. It avoids a significant portion of the finite-size error and can be asymptotically advantageous for quasi-1D systems and certain quasi-2D and 3D systems with high symmetries. We demonstrate the applicability of the method using two different formalisms: the direct ring coupled cluster doubles (drCCD) theory, and the adiabatic-connection (AC) fluctuation-dissipation theory. In the drCCD formalism, the second order screened exchange (SOSEX) correction can also be readily obtained using the staggered mesh method. In the AC formalism, the staggered mesh method naturally avoids the need of performing "head/wing" corrections to the dielectric operator. The effectiveness of the staggered mesh method for insulating systems is theoretically justified by investigating the finite-size error of each individual perturbative term in the RPA correlation energy, expanded as an infinite series of terms associated with ring diagrams. As a side contribution, our analysis provides proof that the finite-size error of each perturbative term of standard RPA and SOSEX calculations scales as , where Nk is the number of grid points in a Monkhorst-Pack mesh.

Au adsorption on stepped Si(hhk)-Au surfaces

The impact of submonolayer gold adsorption on metallic atomic wires grown on terraced silicon substrates is modeled from first principles. Calculations within density functional theory predict Au adsorption at the Si step edge of the Si(553)-Au surface and moderate mobility of the Au adatoms. Although the Au adsorption at the Si step edge does not substantially modify its geometry, a large adsorbate-to-substrate electronic transfer is predicted, which causes a rearrangement of the electronic band structure. The electronic states related to the Si step edge are shifted below the Fermi energy, while an electronic gap opens between the Au-related electronic states. The gap opening leads to a strong enhancement of the Au-chain dimerization. The Au adsorption at the step edge thus modifies the surface morphology non-locally, as a consequence of the strong electronic correlation in quasi-1D systems. Au adsorption on the Si(775)-Au nanowire system occurs mainly at the Au chain, and then at the Si step edge, instead. Adsorption at the Au chain directly modifies its structure by the formation of a structural defect, while adsorption at the step edge has the same effect as in the case of the Si(553)-Au system.

Coupled harmonic oscillator models for correlated plasmons in one-dimensional and quasi-one-dimensional systems

A new phenomenon of correlated plasmons was first observed in the insulating phase of the Sr1−x Nb1−y O3+δ family (Asamara et al 2017 Nat. Commun. 8 15271). The correlated plasmons are tunable, have multiple plasmonic frequencies, and exhibit low loss—making them desirable in numerous plasmonic applications. However, their fundamental mechanism is yet to be explored. While conventional plasmons can be understood solely by considering long-range interactions, unconventional correlated plasmons arise in correlated electron systems and require consideration of the short-range interactions. Here, we report how the interplay of short-range and long-range interactions determines the correlated plasmon phenomena through a coupled harmonic oscillator model of both 1D and quasi-1D systems. In each system, the impact of various physical parameters like the number of oscillators, energy scale, free electron scattering parameter, quasi-particle concentration, charges, effective masses, and Coulomb interaction strengths are explored to gain an understanding of their impact on the complex dielectric function and loss function. We study both cases where the parameters are the same for all quasi-particles and where effective mass, Coulomb interaction strength, and charge are varied for individual quasi-particles. In an extended model of the quasi-1D system, we study both cases where the rung symmetry of all parameters is conserved and where it is broken. When rung symmetry is conserved, the overall trends in optical and plasmonic peaks are the same as the 1D model, though the peaks tend to shift to higher energies and amplitudes. When rung symmetry is broken, the quasi-1D behavior deviates significantly from the 1D model, including an increase in the maximum possible number of optical and plasmonic peaks. Overall, our results demonstrate the significance of the interplay of short-range and long-range interactions in determining the correlated plasmons and identifying how various parameters can be used to tune the resulting plasmons.

Spin liquid and ferroelectricity close to a quantum critical point in PbCuTe2O6

Geometrical frustration among interacting spins combined with strong quantum fluctuations destabilize long-range magnetic order in favor of more exotic states such as spin liquids. By following this guiding principle, a number of spin liquid candidate systems were identified in quasi-two-dimensional (quasi-2D) systems. For 3D, however, the situation is less favorable as quantum fluctuations are reduced and competing states become more relevant. Here we report a comprehensive study of thermodynamic, magnetic and dielectric properties on single crystalline and pressed-powder samples of PbCuTe2O6, a candidate material for a 3D frustrated quantum spin liquid featuring a hyperkagome lattice. Whereas the low-temperature properties of the powder samples are consistent with the recently proposed quantum spin liquid state, an even more exotic behavior is revealed for the single crystals. These crystals show ferroelectric order at TFE ≈ 1 K, accompanied by strong lattice distortions, and a modified magnetic response—still consistent with a quantum spin liquid—but with clear indications for quantum critical behavior.

InSbAs Two-Dimensional Electron Gases as a Platform for Topological Superconductivity.

Topological superconductivity can be engineered in semiconductors with strong spin-orbit interaction coupled to a superconductor. Experimental advances in this field have often been triggered by the development of new hybrid material systems. Among these, two-dimensional electron gases (2DEGs) are of particular interest due to their inherent design flexibility and scalability. Here, we discuss results on a 2D platform based on a ternary 2DEG (InSbAs) coupled to in situ grown aluminum. The spin-orbit coupling in these 2DEGs can be tuned with the As concentration, reaching values up to 400 meV Å, thus exceeding typical values measured in its binary constituents. In addition to a large Landé g-factor of ∼55 (comparable to that of InSb), we show that the clean superconductor-semiconductor interface leads to a hard induced superconducting gap. Using this new platform, we demonstrate the basic operation of phase-controllable Josephson junctions, superconducting islands, and quasi-1D systems, prototypical device geometries used to study Majorana zero modes.

Microscopic diffusion coefficients of dumbbell- and spherocylinder-shaped colloids and their application in simulations of crowded monolayers.

We explore the diffusion properties of colloidal particles with dumbbell and spherocylinder shapes using a hydrodynamic bead-shell approach and additional Brownian dynamics (BD) simulations. By applying the bead-shell method, we determine empirical formulas for the microscopic diffusion coefficients. A comparison of these formulas and established experimental and theoretical results shows remarkable agreement. For example, the maximum relative discrepancy found for dumbbells is less than 5%. As an application example of the empirical formulas, we perform two-dimensional (2D) BD simulations based on a single dumbbell or spherocylinder in a suspension of spheres and calculate the resulting effective long-time diffusion coefficients. The performed BD simulations can be compared to quasi-2D systems such as colloids confined at the interface of two fluids. We find that the effective diffusion coefficient of translation mostly depends on the sphere area fraction ϕ, while the effective diffusion coefficient of rotation is influenced by the aspect ratio and ϕ. Furthermore, the effective rotational diffusion constant seems to depend on the particle shape with the corresponding implementation of the interactions. In the resolution limit of our methods, the shape-dependent differences of the microscopic diffusion coefficients and the long-time diffusion constant of translation are negligible in the first approximation. The determined empirical formulas for the microscopic diffusion coefficients add to the knowledge of the diffusion of anisotropic particles, and they can be used in countless future studies.