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A topological insulator (TI) interfaced with an s-wave superconductor has been predicted to host an unusual form of superconductivity known as topological superconductivity (TSC). Molecular beam epitaxy (MBE) has been the primary approach in the scalable synthesis of the TI/superconductor heterostructures. Although the growth of epitaxial TI films on s-wave superconductors has been achieved, it remains an outstanding challenge for synthesizing atomically thin TI/superconductor heterostructures, which are critical for engineering the TSC phase. Here, we used MBE to grow Bi2Se3 films with the controlled thickness on monolayer NbSe2 and performed in-situ angle-resolved photoemission spectroscopy and ex-situ magneto-transport measurements on these Bi2Se3/monolayer NbSe2 heterostructures. We found that the emergence of Rashba-type bulk quantum well bands and spin-nondegenerate surface states coincides with a marked suppression of the in-plane upper critical magnetic field of the superconductivity in Bi2Se3/monolayer NbSe2 heterostructures. This is the signature of a crossover from Ising- to Rashba-type superconducting pairings, induced by altering Bi2Se3 film thickness. Our work opens a new route for exploring a robust TSC phase in TI/Ising superconductor heterostructures., 27 pages, 4 pages, comments are welcome

Realization of wafer-scale single-crystal films of transition metal dichalcogenides (TMDs) such as WS2 requires epitaxial growth and coalescence of oriented domains to form a continuous monolayer. The domains must be oriented in the same crystallographic direction on the substrate to inhibit the formation of inversion domain boundaries (IDBs), which are a common feature of layered chalcogenides. Here we demonstrate fully coalesced unidirectional WS2 monolayers on 2 in. diameter c-plane sapphire by metalorganic chemical vapor deposition using a multistep growth process to achieve epitaxial WS2 monolayers with low in-plane rotational twist (0.09°). Transmission electron microscopy analysis reveals that the WS2 monolayers are largely free of IDBs but instead have translational boundaries that arise when WS2 domains with slightly offset lattices merge together. By regulating the monolayer growth rate, the density of translational boundaries and bilayer coverage were significantly reduced. The unidirectional orientation of domains is attributed to the presence of steps on the sapphire surface coupled with growth conditions that promote surface diffusion, lateral domain growth, and coalescence while preserving the aligned domain structure. The transferred WS2 monolayers show neutral and charged exciton emission at 80 K with negligible defect-related luminescence. Back-gated WS2 field effect transistors exhibited an ION/OFF of ∼107 and mobility of 16 cm2/(V s). The results demonstrate the potential of achieving wafer-scale TMD monolayers free of inversion domains with properties approaching those of exfoliated flakes.

Atomistic simulation techniques have become an indispensable tool to acquire a fundamental understanding of growth and structural characteristics of two-dimensional (2D) materials of interest, ther...

The introduction of superconductivity to the Dirac surface states of a topological insulator leads to a topological superconductor, which may support topological quantum computing through Majorana zero modes. The development of a scalable material platform is key to the realization of topological quantum computing. Here we report on the growth and properties of high-quality (Bi,Sb)2Te3/graphene/gallium heterostructures. Our synthetic approach enables atomically sharp layers at both hetero-interfaces, which in turn promotes proximity-induced superconductivity that originates in the gallium film. A lithography-free, van der Waals tunnel junction is developed to perform transport tunneling spectroscopy. We find a robust, proximity-induced superconducting gap formed in the Dirac surface states in 5-10 quintuple-layer (Bi,Sb)2Te3/graphene/gallium heterostructures. The presence of a single Abrikosov vortex, where the Majorana zero modes are expected to reside, manifests in discrete conductance changes. The present material platform opens up opportunities for understanding and harnessing the application potential of topological superconductivity., 19 pages, 4 figures, with a Supplemental Information. Comments are welcome

Magnetic insulator-topological insulator heterostructures have been studied in search of chiral edge states via proximity induced magnetism in the topological insulator, but these states have been elusive. We identified MgAl_{0.5}Fe_{1.5}O_{4}/Bi_{2}Se_{3} bilayers for a possible magnetic proximity effect. Electrical transport and polarized neutron reflectometry suggest a proximity effect, but structural data indicate a disordered interface as the origin of the magnetic response. Our results provide a strategy via correlation of microstructure with magnetic data to confirm a magnetic proximity effect.

Sustainable technologies will be essential for meeting future energy demands. Therefore, it is critical to be exploring the fundamental science of materials for photovoltaics and catalysis. For these applications, nanomaterials hold great promise due to their unique, size-dependent properties, tunability, and solution processability. Additionally, nanomaterials offer an effective testbed to understand structural transformations in bulk materials, and to take advantage of effects related to having a high surface area to volume ratio. Transmission electron microscopy (TEM) allows a unique window into the atomic structures of nanomaterials by enabling high-resolution imaging, electron diffraction, and compositional analysis. Specifically, this work explores local structural and compositional transformations by examining how colloidal nanocrystals transform under in situ conditions during imaging. Focusing on halide perovskite nanocrystals for photovoltaic applications and metal nanocrystals for catalytic applications, the roles of size, shape, and composition will be explored, as well as the impact of atomic defects. The degradation of halide perovskites is a major issue facing the field and can be mitigated by an in-depth understanding of the structural changes that occur during degradation processes. For instance, the relative stability of different compositions and dissimilar geometries can provide insights into which factors could improve the longevity of photovoltaic devices. Similarly, metallic nanocrystals for heterogeneous catalysis rely on reactive surfaces, which can be identified, examined, and transformed during in situ TEM experiments. This presentation will describe progress toward understanding transformation mechanisms in these two classes of nanocrystals, and it will provide comparative insights across the systems.

Engineering atomic-scale defects is crucial for realizing wafer-scale, single-crystalline transition metal dichalcogenide monolayers for electronic devices. However, connecting atomic-scale defects to larger morphologies poses a significant challenge. Using electron microscopy and ReaxFF reactive force field-based molecular dynamics simulations, we provide insights into WS

Realization of wafer-scale single-crystal films of transition metal dichalcogenides (TMDs) such as WS

A two-dimensional electron system placed in a magnetic field develops Landau levels, where strong Coulomb interactions lead to the appearance of many-body correlated ground states. Quantum numbers similar to the electron spin enable the understanding and control of complex ground state order and collective excitations. Owing to its spin, valley and orbital degrees of freedom, Bernal-stacked bilayer graphene offers a rich platform to pursue correlated phenomena in two dimensions. In this work, we fabricate dual-gated Bernal-stacked bilayer graphene devices and demonstrate unprecedented fine control over its valley isospin degrees of freedom using a perpendicular electric field. Higher sample quality enables us to probe regimes obscured by disorder in previous studies. We present evidence for a new even-denominator fractional quantum Hall state at filling factor {\nu} = 5/2. The 5/2 state is found to be spontaneously valley polarized in the limit of vanishing valley Zeeman splitting, consistent with a theoretical prediction made regarding the spin polarization of the Moore-Read state. In the vicinity of the even-denominator fractional quantum Hall states, we observe the appearance of the predicted Levin-Halperin daughter states of the Moore-Read Pfaffian wave function at {\nu}= 3/2, 7/2 and of the anti-Pfaffian at {\nu}= 5/2 and -1/2. These observations suggest the breaking of particle-hole symmetry in bilayer graphene. We construct a comprehensive valley polarization phase diagram for the Jain sequence fractional states surrounding filling factor 3/2. These results are well explained by a two-component composite fermion model, further demonstrating the SU(2) nature of the valley isospin in bilayer graphene. Our experiment paves the path for future efforts of manipulating the valley isospin in bilayer graphene to engineer exotic topological orders and quantum information processes., Comment: 24 pages, 14 figures. The changes reported in the erratum are included in the latest version

The spin-orbit torque (SOT) arising from materials with large spin-orbit coupling promises a path for ultra-low power and fast magnetic-based storage and computational devices. We investigated the SOT from magnetron-sputtered BixSe(1-x) thin films in BixSe(1-x)/CoFeB heterostructures by using a dc planar Hall method. Remarkably, the spin Hall angle (SHA) was found to be as large as 18.83, which is the largest ever reported at room temperature (RT). Moreover, switching of a perpendicular CoFeB multilayer using SOT from the BixSe(1-x) has been observed with the lowest-ever switching current density reported in a bilayer system: 2.3 * 105 A/cm2 at RT. The giant SHA, smooth surface, ease of growth of the films on silicon substrate, successful growth and switching of a perpendicular CoFeB multilayer on BixSe(1-x) film opens a path for use of BixSe(1-x) topological insulator (TI) material as a spin-current generator in SOT-based memory and logic devices.

Characterization efforts of core/shell and core/multishell nanocrystals have struggled to quantitatively evaluate the interface width between the core and shell materials despite its importance in their optoelectronic properties. Here, we demonstrate a scanning transmission electron microscopy (STEM) method for measuring the radial elemental composition of two spherical core/shell nanocrystal systems, Ge/Si core/shell and CdSe/CdS/ZnS core/double-shell nanocrystals. By fitting model-based radial distributions of elements to measured STEM–energy-dispersive X-ray (EDX) maps, this method yields reliable and accurate measurements of interface broadening as well as core and shell sizes, surface roughness, and the fraction of core material in the shell. The direct evaluation of the structural parameters is an important step toward improving the synthesis of core/shell nanocrystals and optimizing their optoelectronic properties.

Patterned polymeric coatings are broadly relevant for all areas of bioengineering: anti-biofouling, controlled protein adsorption, guided cell growth, and many more. This contribution describes a robust topographical and chemical patterning platform that combines an LED digital light projector with oxygen-tolerant light-mediated polymerization to design advanced surfaces on the micron scale and in mild ambient conditions. The user-friendly nature of this approach is targeted towards bringing complex chemical patterning abilities based on surface-tethered polymers into the hands of non-experts and enabling both fundamental and applied studies related to patterned surfaces in bioengineering.

Topological insulator (TI) materials are exciting candidates for integration into next-generation memory and logic devices because of their potential for efficient, low-energy-consumption switching of magnetization. Specifically, the family of bismuth chalcogenides offers efficient spin-to-charge conversion because of its large spin-orbit coupling and spin-momentum locking of surface states. However, a major obstacle to realizing the promise of TIs is the thin-film materials' quality, which lags behind that of epitaxially grown semiconductors. In contrast to the latter systems, the Bi-chalcogenides form by van der Waals epitaxy, which allows them to successfully grow onto substrates with various degrees of lattice mismatch. This flexibility enables the integration of TIs into heterostructures with emerging materials, including two-dimensional materials. However, understanding and controlling local features and defects within the TI films is critical to achieving breakthrough device performance. Here, we report observations and modeling of large-scale structural defects in (Bi,Sb)$_2$Te$_3$ films grown onto hexagonal BN, highlighting unexpected symmetry-breaking rotations within the films and the coexistence of a second phase along grain boundaries. Using first-principles calculations, we show that these defects could have consequential impacts on the devices that rely on these TI films, and therefore they cannot be ignored.

Engineering atomic-scale defects is crucial for realizing wafer-scale, single-crystalline transition metal dichalcogenide monolayers for electronic devices. However, connecting atomic-scale defects to larger morphologies poses a significant challenge. Using electron microscopy and atomistic simulations, we provide insights into WS2 crystal growth mechanisms, providing a direct link between synthetic conditions and the microstructure. Dark-field TEM imaging of coalesced monolayer WS2 films illuminates defect arrays that atomic-resolution STEM imaging identifies as translational grain boundaries. Imaging reveals the films to have nearly a single orientation with imperfectly stitched domains. Through atomic-resolution imaging and ReaxFF reactive force field-based molecular dynamics simulations, we observe two types of translational mismatch and discuss their atomic structures and origin. Our results indicate that the mismatch results from relatively fast growth rates. Through statistical analysis of >1300 facets, we demonstrate that the macrostructural features are constructed from nanometer-scale building blocks, describing the system across sub-{\AA}ngstrom to multi-micrometer length scales., Comment: 20 pages, 4 figures

Whereas thin films of topological insulators grown by molecular beam epitaxy often display regular, triangular features, $\mathrm{B}{\mathrm{i}}_{2}\mathrm{S}{\mathrm{e}}_{3}$ films grown onto yttrium iron garnet (YIG) display much greater disorder. Here, we present observations of various types of disorder present in these films using atomic force microscopy and scanning transmission electron microscopy. The investigation reveals the presence of an amorphous metal oxide layer between the substrate and the film, which appears to smooth out the nanometer-scale undulations in the YIG surface. It also shows the existence of quasiordered arrays of heavy atoms in some interfacial regions, as well as rotations and tilting between adjacent grains and basal twinning at various heights in the film. Using density functional theory, we explore the impact of these prominent basal twins on the electronic structure of the film.

The emulsion-based self-assembly of nanoparticles into low-dimensional superparticles of hollow vesicle-like assemblies is reported. Evaporation of the oil phase at relatively low temperatures from nanoparticle-containing oil-in-water emulsion droplets leads to the formation of stable and uniform sub-micrometer vesicle-like assembly structures in water. This result is in contrast with those from many previously reported emulsion-based self-assembly methods, which produce solid spherical assemblies. It is found that extra surfactants in both the oil and water phases play a key role in stabilizing nanoscale emulsion droplets and capturing hollow assembly structures. Systematic investigation into what controls the morphology in emulsion self-assembly is carried out, and the approach is extended to fabricate more complex rattle-like structures and 2D plates. These results demonstrate that the emulsion-based assembly is not limited to typical thermodynamic spherical assembly structures and can be used to fabricate various types of interesting low-dimensional assembly structures.

Defects have a profound impact on the electronic and physical properties of crystals. For two-dimensional (2D) materials, many intrinsic point defects have been reported, but much remains to be understood about their origin. Using scanning transmission electron microscopy imaging, this study discovers various linear arrays of W-vacancy defects that are explained in the context of the crystal growth of coalesced, monolayer WS2. Atomistic-scale simulations show that vacancy arrays can result from steric hindrance of bulky gas-phase precursors at narrowly separated growth edges, and that increasing the edge separation leads to various intact and defective growth modes, which are driven by competition between the catalytic effects of the sapphire substrate and neighboring growth edge. Therefore, we hypothesize that the arrays result from combined growth modes, which directly result from film coalescence. The connections drawn here will guide future synthetic and processing strategies to harness the engineering potential of defects in 2D monolayers.

We have developed a generalized seeded-growth methodology for the synthesis of monodisperse metal-doped plasmonic oxide heterodimer nanocrystals (NCs) with a near-unity morphological yield. Using indium-doped cadmium oxide (ICO) as an example, we show that a wide variety of preformed metal NCs (Au, Pt, Pd, FePt, etc.) can serve as the seeds for the tailored synthesis of metal-ICO heterodimers with exquisite size, shape, and composition control, facilitated by the delayed nucleation mechanism of the CdO phase. The metal-ICO heterodimers exhibit broadly tunable near-infrared localized surface plasmon resonances, and dual plasmonic bands are observed for Au-ICO heterodimers. We further demonstrate that the oxide domain of the Au-ICO heterodimers can be selectively and controllably transformed into a series of partially and completely hollow cadmium chalcogenide nanoarchitectures with unprecedented structural complexity, leaving the metal domain intact. Our work not only represents an exciting addition to the rapidly expanding library of chemical reactions that produce colloidal hybrid NCs, but it also provides a general route for the bottom-up chemical design of multicomponent metal-oxide-semiconductor NCs in a rational and sequential manner.

We report the observation of ferromagnetic resonance-driven spin pumping signals at room temperature in three-dimensional topological insulator thin films-Bi_{2}Se_{3} and (Bi,Sb)_{2}Te_{3}-deposited by molecular beam epitaxy on Y_{3}Fe_{5}O_{12} thin films. By systematically varying the Bi_{2}Se_{3} film thickness, we show that the spin-charge conversion efficiency, characterized by the inverse Rashba-Edelstein effect length (λ_{IREE}), increases dramatically as the film thickness is increased from two quintuple layers, saturating above six quintuple layers. This suggests a dominant role of surface states in spin and charge interconversion in topological-insulator-ferromagnet heterostructures. Our conclusion is further corroborated by studying a series of Y_{3}Fe_{5}O_{12}/(Bi,Sb)_{2}Te_{3} heterostructures. Finally, we use the ferromagnetic resonance linewidth broadening and the inverse Rashba-Edelstein signals to determine the effective interfacial spin mixing conductance and λ_{IREE}.

We studied the tunnel magnetoresistance (TMR) of L10-FePd perpendicular magnetic tunnel junctions (p-MTJs) with an FePd free layer and an inserted diffusion barrier. The diffusion barriers studied here (Ta and W) were shown to enhance the TMR ratio of the p-MTJs formed using high-temperature annealing, which are necessary for the formation of high quality L10-FePd films and MgO barriers. The L10-FePd p-MTJ stack was developed with an FePd free layer with a stack of FePd/X/Co20Fe60B20, where X is the diffusion barrier, and patterned into micron-sized MTJ pillars. The addition of the diffusion barrier was found to greatly enhance the magneto-transport behavior of the L10-FePd p-MTJ pillars such that those without a diffusion barrier exhibited negligible TMR ratios (

We report electrical measurements of the current-induced spin polarization of the surface current in topological insulator devices where contributions from bulk and surface conduction can be disentangled by electrical gating. The devices use a ferromagnetic tunnel junction (permalloy/$\mathrm{Al}{}_{2}{\mathrm{O}}_{3}$) as a spin detector on a back-gated ${(\mathrm{Bi},\mathrm{Sb})}_{2}{\mathrm{Te}}_{3}$ channel. We observe hysteretic voltage signals as the magnetization of the detector ferromagnet is switched parallel or antiparallel to the spin polarization of the surface current. The amplitude of the detected voltage change is linearly proportional to the applied dc bias current in the ${(\mathrm{Bi},\mathrm{Sb})}_{2}{\mathrm{Te}}_{3}$ channel. As the chemical potential is tuned from the bulk bands into the surface state band, we observe an enhancement of the spin-dependent voltages up to 300% within the range of the electrostatic gating. Using a simple model, we extract the spin polarization near charge neutrality (i.e., the Dirac point).