Stacking Symmetry Research Articles

Revisiting the metal-to-metal transition in 2H-AgNiO2

The layered delafossite compound AgNiO2 with stacking symmetry undergoes a structural metal-to-metal transition at . It has been described in the past as a charge-ordering transition, where local S = 1 spins are formed on part of the Ni sites. By means of first-principles many-body calculations, we show that the transition is in fact a site-selective Mott transition on the Ni sublattice with only minor charge differentiation. Key to this finding is the uncovering of ligand-hole physics, rendering a Ni2+ instead of a formal Ni3+ oxidation state, in conjunction with strong local Coulomb repulsions.

Full-Volume 3D Fluid Flow Reconstruction With Light Field PIV.

Particle Imaging Velocimetry (PIV) is a classical method that estimates fluid flow by analyzing the motion of injected particles. To reconstruct and track the swirling particles is a difficult computer vision problem, as the particles are dense in the fluid volume and have similar appearances. Further, tracking a large number of particles is particularly challenging due to heavy occlusion. Here we present a low-cost PIV solution that uses compact lenslet-based light field cameras as imaging device. We develop novel optimization algorithms for dense particle 3D reconstruction and tracking. As a single light field camera has limited capacity in resolving depth (z-dimension measurement), the resolution of 3D reconstruction on the x-y plane is much higher than along the z-axis. To compensate for the imbalanced resolution in 3D, we use two light field cameras positioned at an orthogonal angle to capture particle images. In this way, we can achieve high-resolution 3D particle reconstruction in the full fluid volume. For each time frame, we first estimate particle depths under a single viewpoint by exploiting the focal stack symmetry of light field. We then fuse the recovered 3D particles in two views by solving a linear assignment problem (LAP). Specifically, we propose an anisotropic point-to-ray distance as matching cost to handle the resolution mismatch. Finally, given a sequence of 3D particle reconstructions over time, we recover the full-volume 3D fluid flow with a physically-constrained optical flow, which enforces local motion rigidity and fluid incompressibility. We perform comprehensive experiments on synthetic and real data for ablation and evaluation. We show that our method recovers full-volume 3D fluid flows of various types. Two-view reconstruction results achieves higher accuracy than those with one view only.

Controlling interlayer magnetic coupling in the two-dimensional magnet Fe3GeTe2

Interlayer magnetic coupling in emerging two-dimensional layered magnets holds great potential for manipulating layered magnetic structures for cross-layer transport or tunneling phenomena. In this paper, we employed first-principles calculations to show enhanced ferromagnetic (FM) interlayer exchange coupling for ${\mathrm{Fe}}_{3}{\mathrm{GeTe}}_{2}$ by reducing stacking symmetry or reducing the layer number. Electronic structure analysis reveals that the former is mainly due to low-symmetry enhanced interlayer orbital hopping, and the latter originates from reduced Pauli potential for out-of-plane metallic electrons with respect to thicker layers. Interlayer FM coupling could also be weakened by substrates due to the screened Coulomb interactions, simulated by reducing the onsite Coulomb repulsion for Fe $d$ electrons. In this paper, we provide guidance to rationally control interlayer magnetic coupling via engineering stacking configuration and dielectric environment.

Tuning interfacial Dzyaloshinskii-Moriya interactions in thin amorphous ferrimagnetic alloys

Skyrmions can be stabilized in magnetic systems with broken inversion symmetry and chiral interactions, such as Dzyaloshinskii-Moriya interactions (DMI). Further, compensation of magnetic moments in ferrimagnetic materials can significantly reduce magnetic dipolar interactions, which tend to favor large skyrmions. Tuning DMI is essential to control skyrmion properties, with symmetry breaking at interfaces offering the greatest flexibility. However, in contrast to the ferromagnet case, few studies have investigated interfacial DMI in ferrimagnets. Here we present a systematic study of DMI in ferrimagnetic CoGd films by Brillouin light scattering. We demonstrate the ability to control DMI by the CoGd cap layer composition, the stack symmetry and the ferrimagnetic layer thickness. The DMI thickness dependence confirms its interfacial nature. In addition, magnetic force microscopy reveals the ability to tune DMI in a range that stabilizes sub-100 nm skyrmions at room temperature in zero field. Our work opens new paths for controlling interfacial DMI in ferrimagnets to nucleate and manipulate skyrmions.

Symmetry-Controlled Reversible Photovoltaic Current Flow in Ultrathin All 2D Vertically Stacked Graphene/MoS2/WS2/Graphene Devices.

Atomically thin vertical heterostructures are promising candidates for optoelectronic applications, especially for flexible and transparent technologies. Here, we show how ultrathin all two-dimensional vertical-stacked type-II heterostructure devices can be assembled using only materials grown by chemical vapor deposition, with graphene (Gr) as top and bottom electrodes and MoS2/WS2 as the active semiconductor layers in the middle. Furthermore, we show that the stack symmetry, which dictates the type-II directionality, is the dominant factor in controlling the photocurrent direction upon light irradiation, whereas in homobilayers, photocurrent direction cannot be easily controlled because the tunnel barrier is determined by the doping levels of the graphene, which appears fixed for top and bottom graphene layers due to their dielectric environments. Therefore, the ability to direct photovoltaic current flow is demonstrated to be only possible using heterobilayers (HBs) and not homobilayers. We study the photovoltaic effects in more than 40 devices, which allows for statistical verification of performance and comparative behavior. The photovoltage in the graphene/transition-metal dichalcogenide-heterobilayer/graphene (Gr/TMD-HB (MoS2/WS2)/Gr) increases up to 10 times that generated in the monolayer TMD devices under the same optical illumination power, due to efficient charge transfer between WS2 and MoS2 and extraction to graphene electrodes. By applying external gate voltages ( Vg), the band alignment can be tuned, which in turn controls the photovoltaic effect in the vertical heterostructures. The tunneling-assisted interlayer charge recombination also plays a significant role in modulating the photovoltaic effect in the Gr/TMD-HB/Gr. These results provide important insights into how layer symmetry in vertical-stacked graphene/TMD/graphene ultrathin optoelectronics can be used to control electron flow directions during photoexcitation and open up opportunities for tandem cell assembly.

Different threshold and bipolar resistive switching mechanisms in reactively sputtered amorphous undoped and Cr-doped vanadium oxide thin films

This study investigates resistive switching in amorphous undoped and Cr-doped vanadium oxide thin films synthesized by sputtering deposition at low oxygen partial pressure. Two different volatile threshold switching characteristics can occur as well as a non-volatile bipolar switching mechanism, depending on device stack symmetry and Cr-doping. The two threshold switching types are associated with different crystalline phases in the conduction filament created during an initial forming step. The first kind of threshold switching, observed for undoped vanadium oxide films, was, by its temperature dependence, proven to be associated with a thermally triggered insulator-to-metal transition in a crystalline VO2 phase, whereas the threshold switch observed in chromium doped films is stable up to 90 °C and shows characteristics of an electronically induced Mott transition. This different behaviour for undoped versus doped films has been attributed to an increased stability of V3+ due to the Cr3+ doping (as evidenced by X-ray photoelectron spectroscopy analysis), probably favouring the creation of a crystalline Cr-doped V2O3 phase (rather than a Cr-doped VO2 phase) during the energetic forming step. The symmetric Pt/a-(VCr)Ox/Pt device showing high temperature stable threshold switching may find interesting applications as a possible new selector device for resistive switching memory (ReRAM) crossbar arrays.

Symmetry forbidden morphologies and domain boundaries in nanoscale graphene islands

The synthesis of graphene nanoislands with tailored quantum properties requires an atomic control of the morphology and crystal structure. As one reduces their size down to the nanometer scale, domain boundary and edge energetics, as well as nucleation and growth mechanisms impose different stability and kinetic landscape from that at the microscale. This offers the possibility to synthesize structures that are exclusive to the nanoscale, but also calls for fundamental growth studies in order to control them.By employing high-resolution scanning tunneling microscopy we elucidate the atomic stacking configurations, domain boundaries, and edge structure of graphene nanoislands grown on Ni(1 1 1) by CVD and post-annealed at different temperatures. We find a non-conventional multistep mechanism that separates the thermal regimes for growth, edge reconstruction, and final stacking configuration, leading to nanoisland morphologies that are incompatible with their stacking symmetry. Whole islands shift their stacking configuration during cooling down, and others present continuous transitions at the edges. A statistical analysis of the domain structures obtained at different annealing temperatures reveals how polycrystalline, ill-defined structures heal into shape-selected islands of a single predominant stacking. The high crystallinity and the control on morphology and edge structure makes these graphene nanoislands ideal for their application in optoelectronics and spintronics.

First-Principles Quantum Dynamics of Singlet Fission: Coherent versus Thermally Activated Mechanisms Governed by Molecular π Stacking.

Singlet excitons in π-stacked molecular crystals can split into two triplet excitons in a process called singlet fission that opens a route to carrier multiplication in photovoltaics. To resolve controversies about the mechanism of singlet fission, we have developed a first principles nonadiabatic quantum dynamical model that reveals the critical role of molecular stacking symmetry and provides a unified picture of coherent versus thermally activated singlet fission mechanisms in different acenes. The slip-stacked equilibrium packing structure of pentacene derivatives is found to enhance ultrafast singlet fission mediated by a coherent superexchange mechanism via higher-lying charge transfer states. By contrast, the electronic couplings for singlet fission strictly vanish at the C(2h) symmetric equilibrium π stacking of rubrene. In this case, singlet fission is driven by excitations of symmetry-breaking intermolecular vibrations, rationalizing the experimentally observed temperature dependence. Design rules for optimal singlet fission materials therefore need to account for the interplay of molecular π-stacking symmetry and phonon-induced coherent or thermally activated mechanisms.

Electronic Thermal Property of Graphite

The interlayer atomic interactions determine the low-lying band structure of graphite and thus the electronic specific heat. Simple hexagonal graphite presents the greatest specific heat and exhibits a linear temperature-dependence due to the nearly constant density of states. Bernal graphite deviates from the linear \(T\)-dependence as temperature is above 100 K. Rhombohedral graphite shows the linear dependence only in the low temperature range, and is revealed to have the lowest specific heat. In addition, monolayer graphene has a \(T\)-square dependence. These significant differences in thermal property originate from the stacking symmetry.

Optical transitions between Landau levels: AA-stacked bilayer graphene

The magneto-optical absorption spectra of AA-stacked bilayer graphene (AABG) exhibit two kinds of absorption peaks resulting from two groups of Landau levels (LLs). Only intragroup excitations that follow a single selection rule take place. The excitation channels are altered as the field strength approaches a critical strength. These optical properties can be comprehended by the characteristics of the LL wave functions. A comparison of AABG and AB-stacked bilayer graphene (BBG) demonstrates that the optical properties are dominated by the stacking symmetry. The presented results could offer a way to distinguish AABG from BBG and monolayer graphene.

Multilayer epitaxial graphene grown on the surface; structure and electronic properties

We review the progress towards developing epitaxial graphene as a material for carbon electronics. In particular, we discuss improvements in epitaxial graphene growth, interface control and the understanding of multilayer epitaxial graphene's (MEG's) electronic properties. Although graphene grown on both polar faces of SiC will be discussed, our discussions will focus on graphene grown on the C-face of SiC. The unique properties of C-face MEG have become apparent. These films behave electronically like a stack of nearly independent graphene sheets rather than a thin Bernal stacked graphite sample. The origins of multilayer graphene's electronic behaviour are its unique highly ordered stacking of non-Bernal rotated graphene planes. While these rotations do not significantly affect the inter-layer interactions, they do break the stacking symmetry of graphite. It is this broken symmetry that leads to each sheet behaving like isolated graphene planes.