Seeded growth of single-crystal black phosphorus nanoribbons.

Two-dimensional materials have emerged as an important research frontier for overcoming the challenges in nanoelectronics and for exploring new physics. Among them, black phosphorus, with a combination of a tunable bandgap and high mobility, is one of the most promising systems. In particular, black phosphorus nanoribbons show excellent electrostatic gate control, which can mitigate short-channel effects in nanoscale transistors. Controlled synthesis of black phosphorus nanoribbons, however, has remained an outstanding problem. Here we report large-area growth of black phosphorus nanoribbons directly on insulating substrates. We seed the chemical vapour transport growth with black phosphorus nanoparticles and obtain uniform, single-crystal nanoribbons oriented exclusively along the [100] crystal direction. With comprehensive structural calculations, we discover that self-passivation at the zigzag edges holds the key to the preferential one-dimensional growth. Field-effect transistors based on individual nanoribbons exhibit on/off ratios up to ~104, confirming the good semiconducting behaviour of the nanoribbons. These results demonstrate the potential of black phosphorus nanoribbons for nanoelectronic devices and also provide a platform for investigating the exotic physics in black phosphorus.

Direct experimental evidence of physical origin of electronic phase separation in manganites.

Electronic phase separation in complex oxides is the inhomogeneous spatial distribution of electronic phases, involving length scales much larger than those of structural defects or nonuniform distribution of chemical dopants. While experimental efforts focused on phase separation and established its correlation with nonlinear responses under external stimuli, it remains controversial whether phase separation requires quenched disorder for its realization. Early theory predicted that if perfectly "clean" samples could be grown, both phase separation and nonlinearities would be replaced by a bicritical-like phase diagram. Here, using a layer-by-layer superlattice growth technique we fabricate a fully chemically ordered "tricolor" manganite superlattice, and compare its properties with those of isovalent alloyed manganite films. Remarkably, the fully ordered manganite does not exhibit phase separation, while its presence is pronounced in the alloy. This suggests that chemical-doping-induced disorder is crucial to stabilize the potentially useful nonlinear responses of manganites, as theory predicted.

Cathodoluminescence visualisation of local thickness variations of GaAs/AlGaAs quantum-well tubes on nanowires.

We present spatially and spectrally resolved emission from nanowires with a thin radial layer of GaAs embedded in AlGaAs barriers, grown radially around taper-free GaAs cores. The GaAs layers are thin enough to show quantization, and are quantum wells. Due to their shape, they are referred to as quantum well tubes (QWTs). We have investigated three different nominal QWT thicknesses: 1.5, 2.0, and 6.0 nm. They all show average emission spectra from the QWT with an energy spread corresponding to a thickness variation of ±30%. We observe no thickness gradient along the length of the nanowires. Individual NWs show a number of peaks, corresponding to different QW thicknesses. Apart from the thinnest QWT, the integrated emission from the QWTs shows homogeneous emission intensity along the NW. The thinnest QWTs show patchy emission patterns due to the incomplete coverage of the QWT. We observe a few NWs with larger diameters. The QWTs in these NWs show spatially resolved variations across the NW. An increase in the local thickness of the QWT at the corners blocks the diffusion of carriers from facet to facet, thereby enabling us to visualise the thickness variations of the radial quantum wells.

Axicon Lens for Electrons Using a Magnetic Vortex: The Efficient Generation of a Bessel Beam.

We demonstrate experimentally an efficient electron axicon lens using a magnetic vortex. We show that naturally occurring magnetic vortices with circular magnetic moment distributions in a soft-magnetic thin film create conical phase shifts for fast electrons. Such radially symmetric linear phase ramps are equivalent to ideal light optical axicons. We apply this lens to generate efficient nondiffracting electron Bessel beams, which we observe experimentally in through-focus Lorentz images as well as in propagated off-axis electron holograms. This highlights the potential for using magnetic nanostructures as highly efficient and flexible phase plates for crafting desired electron beam shapes.

Quantum Confined Stark Effect in a GaAs/AlGaAs Nanowire Quantum Well Tube Device: Probing Exciton Localization.

In this Letter, we explore the nature of exciton localization in single GaAs/AlGaAs nanowire quantum well tube (QWT) devices using photocurrent (PC) spectroscopy combined with simultaneous photoluminescence (PL) and photoluminescence excitation (PLE) measurements. Excitons confined to GaAs quantum well tubes of 8 and 4 nm widths embedded into an AlGaAs barrier are seen to ionize at high bias levels. Spectroscopic signatures of the ground and excited states confined to the QWT seen in PL, PLE, and PC data are consistent with simple numerical calculations. The demonstration of good electrical contact with the QWTs enables the study of Stark effect shifts in the sharp emission lines of excitons localized to quantum dot-like states within the QWT. Atomic resolution cross-sectional TEM measurements and an analysis of the quantum confined Stark effect of these dots provide insights into the nature of the exciton localization in these nanostructures.

Emergence of localized states in narrow GaAs/AlGaAs nanowire quantum well tubes.

We use low-temperature photoluminescence, photoluminescence excitation, and photoluminescence imaging spectroscopy to explore the optical and electronic properties of GaAs/AlGaAs quantum well tube (QWT) heterostructured nanowires (NWs). We find that GaAs QWTs with widths >5 nm have electronic states which are delocalized and continuous along the length of the NW. As the NW QWT width decreases from 5 to 1.5 nm, only a single electron state is bound to the well, and no optical excitations to a confined excited state are present. Simultaneously, narrow emission lines (fwhm < 600 µeV) appear which are localized to single spatial points along the length of the NW. We find that these quantum-dot-like states broaden at higher temperatures and quench at temperatures above 80 K. The lifetimes of these localized states are observed to vary from dot to dot from 160 to 400 ps. The presence of delocalized states and then localized states as the QWTs become more confined suggests both opportunities and challenges for possible incorporation into quantum-confined device structures.

Investigation of (Fe,Co)NbB-Based Nanocrystalline Soft Magnetic Alloys by Lorentz Microscopy and Off-Axis Electron Holography.

The relationship between microstructure and magnetic properties of a (Fe,Co)NbB-based nanocrystalline soft magnetic alloy was investigated by analytical transmission electron microscopy (TEM). The microstructures of (Fe0.5Co0.5)80Nb4B13Ge2Cu1 nanocrystalline alloys annealed at different temperatures were characterized by TEM and electron diffraction. The magnetic structures were analyzed by Lorentz microscopy and off-axis electron holography, including quantitative measurement of domain wall width, induction, and in situ magnetic domain imaging. The results indicate that the magnetic domain structure and particularly the dynamical magnetization behavior of the alloys strongly depend on the microstructure of the nanocrystalline alloys. Smaller grain size and random orientation of the fine particles decrease the magneto-crystalline anisotropy and suggests better soft magnetic properties which may be explained by the anisotropy model of Herzer.

Fast imaging with inelastically scattered electrons by off-axis chromatic confocal electron microscopy.

We introduce off-axis chromatic scanning confocal electron microscopy, a technique for fast mapping of inelastically scattered electrons in a scanning transmission electron microscope without a spectrometer. The off-axis confocal mode enables the inelastically scattered electrons to be chromatically dispersed both parallel and perpendicular to the optic axis. This enables electrons with different energy losses to be separated and detected in the image plane, enabling efficient energy filtering in a confocal mode with an integrating detector. We describe the experimental configuration and demonstrate the method with nanoscale core-loss chemical mapping of silver (M4,5) in an aluminium-silver alloy and atomic scale imaging of the low intensity core-loss La (M4,5@840 eV) signal in LaB6. Scan rates up to 2 orders of magnitude faster than conventional methods were used, enabling a corresponding reduction in radiation dose and increase in the field of view. If coupled with the enhanced depth and lateral resolution of the incoherent confocal configuration, this offers an approach for nanoscale three-dimensional chemical mapping.

Polarity-driven 3-fold symmetry of GaAs/AlGaAs core multishell nanowires.

AlGaAs/GaAs quantum well heterostructures based on core-multishell nanowires exhibit excellent optical properties which are acutely sensitive to structure and morphology. We characterize these heterostructures and observe them to have 3-fold symmetry about the nanowire axis. Using aberration-corrected annular dark field scanning transmission electron microscopy (ADF-STEM), we measure directly the polarity of the crystal structure and correlate this with the shape and facet orientation of the GaAs core, quantum wells and cap, and the width of radial Al-rich bands. We discuss how the underlying polarity of the crystal structure drives the growth of these heterostructures with a 3-fold symmetry resulting in a nonuniform GaAs quantum well tube and AlGaAs shell. These observations suggest that the AlGaAs growth rate is faster along the [112] B compared to the [112] A directions and/or that there is a polarity driven surface reconstruction generating AlGaAs growth fronts inclined to the {110} planes. In contrast, the observations suggest that the opposite is true for the GaAs growth, with the preferred surface reconstruction plane being parallel to {110} and an apparent faster growth rate along the [112] A. This two-dimensional layer growth of the nanowire multishells strongly depends on the surface energies and surface reconstruction of the facets which are related to the crystal polarity and lead to the 3-fold symmetry observed here.

Optical, structural, and numerical investigations of GaAs/AlGaAs core-multishell nanowire quantum well tubes.

The electronic properties of thin, nanometer scale GaAs quantum well tubes embedded inside the AlGaAs shell of a GaAs core-multishell nanowire are investigated using optical spectroscopies. Using numerical simulations to model cylindrically and hexagonally symmetric systems, we correlate these electronic properties with structural characterization by aberration-corrected scanning transmission electron microscopy of nanowire cross sections. These tubular quantum wells exhibit extremely high quantum efficiency and intense emission for extremely low submicrowatt excitation powers in both photoluminescence and photoluminescence excitation measurements. Numerical calculations of the confined eigenstates suggest that the electrons and holes in their ground states are confined to extremely localized one-dimensional filaments at the corners of the hexagonal structure which extend along the length of the nanowire.

A simple coordinate transformation method for quickly locating the features of interest in TEM samples.

We developed a simple coordinate transformation method for quickly locating features of interest (FOIs) of samples in transmission electron microscope (TEM). The method is well suited for conducting sample searches in aberration-corrected scanning/transmission electron microscopes (S/TEM), where the survey can be very time-consuming because of the limited field of view imposed by the highly excited objective lens after fine-tuning the aberration correctors. For implementation, a digital image of the sample and the TEM holder was captured using a simple stereo-optical microscope. Naturally presented geometric patterns on the holder were referenced to construct a projective transformation between the electron and optical coordinate systems. The test results demonstrated that the method was accurate and required no electron microscope or specimen holder modifications. Additionally, it eliminated the need to mount the sample onto specific patterned TEM grids or deposit markers, resulting in universal applications for most TEM samples, holders and electron microscopes for fast FOI identification. Furthermore, we implemented the method into a Gatan script for graphical-user-interface-based step-by-step instructions. Through online communication, the script enabled real-time navigation and tracking of the motion of samples in TEM on enlarged optical images with a panoramic view.

Robust Tunability and Newly Emerged Q Resonance of Ba0.8Sr0.2TiO3-Based Microwave Capacitors under Gamma Irradiations.

The complex resonance of dielectric quality factor Q, combined with a capacitance tunability n higher than 3:1 without any dispersion, was achieved in the voltage-tunable interdigital capacitors (IDCs) based on epitaxial Ba0.8Sr0.2TiO3 ferroelectric thin films across the microwave L (1-2 GHz), S (2-4 GHz), and C (4-8 GHz) bands at room temperature. The resonant Q and n features were driven by the microwave responses of the ferroelectric nanodomains engineered in the films. To promote their application in space radiation environments, the evolutions of Q and n both as functions of frequency f (1-8 GHz) and applied electric field E (0-240 kV/cm) were systematically investigated under a series of gamma-ray irradiations up to 100 kGy. The robust capacitance tunability was accompanied by the emergence of an additional Q resonance at 2.3 GHz in most post-irradiated devices, which is ascribed to extra polar nanoregions of expanded surface lattices associated with oxygen vacancies induced by irradiations.

Synthesis of Rhenium-Doped Copper Twin Boundary for High-Turnover-Frequency Electrochemical Nitrogen Reduction.

The precise design and synthesis of active sites to improve catalyst's performance has emerged as a promising tactic for electrochemistry. However, it is challenging to combine different types of active sites and manipulate them simultaneously at atomic resolution. Here, we present a strategy to synthesize Re atom-doped Cu twin boundaries (TBs), through pulsed electrodeposition and boundary segregation. The Re-doped Cu TBs demonstrate a highly efficient nitrogen reduction reaction (NRR) performance. Re-doped Cu TBs showed a turnover frequency of ∼5889 s-1, ∼800 times higher than the pure Cu TB active centers (∼7 s-1). In addition to the "acceptance-donation" activation of N2 molecules, theoretical calculations also reveal that the Re-Re dimer on TB can boost the NRR and impede the hydrogen evolution reaction synchronously, rendering Re-doped Cu TB catalysts with high NRR activity and selectivity.

Hexagonal-Ge Nanostructures with Direct-Bandgap Emissions in a Si-Based Light-Emitting Metasurface.

Si-based emitters have been of great interest as an ideal light source for monolithic optical-electronic integrated circuits (MOEICs) on Si substrates. However, the general Si-based material is a diamond structure of cubic lattice with an indirect band gap, which cannot emit light efficiently. Here, hexagonal-Ge (H-Ge) nanostructures within a light-emitting metasurface consisting of a cubic-SiGe nanodisk array are reported. The H-Ge nanostructure is naturally formed within the cubic-Ge epitaxially grown on Si (001) substrates due to the strain-induced nanoscale crystal structure transformation assisted by far-from-equilibrium growth conditions. The direct-bandgap features of H-Ge nanostructures are observed and discussed, including a rather strong and linearly power-dependent photoluminescence (PL) peak around 1562 nm at room temperature and temperature-insensitive PL spectrum near room temperature. Given the direct-bandgap nature, the heterostructure of H-Ge/C-Ge, and the compatibility with the sophisticated Si technology, the H-Ge nanostructure has great potential for innovative light sources and other functional devices, particularly in Si-based MOEICs.

Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage.

Due to their uncontrollable assembly and crystallization process, the synthesis of mesoporous metal oxide single crystals remains a formidable challenge. Herein, we report the synthesis of single-crystal-like mesoporous Li2TiSiO5 by using soft micelles as templates. The key lies in the atomic-scale self-assembly and step-crystallization processes, which ensure the formation of single-crystal-like mesoporous Li2TiSiO5 microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon matrix. The mesoporous Li2TiSiO5 anode achieves a superior rate capability (148 mAh g-1 at 5.0 A g-1) and outstanding long-term cycling stability (138 mAh g-1 after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+ diffusion caused by penetrating mesochannels and nanosized crystal frameworks (5-10 nm). In comparison, bulk Li2TiSiO5 exhibits poor rate capability and cycle performance due to micron-scale diffusion lengths. This method is very simple and reproducible, heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

Spontaneous rotational symmetry breaking in KTaO3 heterointerface superconductors.

Broken symmetries play a fundamental role in superconductivity and influence many of its properties in a profound way. Understanding these symmetry breaking states is essential to elucidate the various exotic quantum behaviors in non-trivial superconductors. Here, we report an experimental observation of spontaneous rotational symmetry breaking of superconductivity at the heterointerface of amorphous (a)-YAlO3/KTaO3(111) with a superconducting transition temperature of 1.86 K. Both the magnetoresistance and superconducting critical field in an in-plane field manifest striking twofold symmetric oscillations deep inside the superconducting state, whereas the anisotropy vanishes in the normal state, demonstrating that it is an intrinsic property of the superconducting phase. We attribute this behavior to the mixed-parity superconducting state, which is an admixture of s-wave and p-wave pairing components induced by strong spin-orbit coupling inherent to inversion symmetry breaking at the heterointerface of a-YAlO3/KTaO3. Our work suggests an unconventional nature of the underlying pairing interaction in the KTaO3 heterointerface superconductors, and brings a new broad of perspective on understanding non-trivial superconducting properties at the artificial heterointerfaces.

Two-Dimensional Superconductivity at the Titanium Sesquioxide Heterointerface.

The study of exotic superconductivity in two dimensions has been a central theme in the solid state and materials research communities. Experimentally exploring and identifying exotic, fascinating interface superconductors with a high transition temperature (Tc) are challenging. Here, we report an experimental observation of intriguing two-dimensional superconductivity with a Tc of up to 3.8 K at the interface between a Mott insulator Ti2O3 and polar semiconductor GaN. At the verge of superconductivity, we also observe a striking quantum metallic-like state, demonstrating that it is a precursor to the two-dimensional superconductivity as the temperature is decreased. Our work shows an exciting opportunity to exploit the underlying, emergent quantum phenomena at the heterointerfaces via heterostructure engineering.

Electronically phase separated nano-network in antiferromagnetic insulating LaMnO3/PrMnO3/CaMnO3 tricolor superlattice.

Strongly correlated materials often exhibit an electronic phase separation (EPS) phenomena whose domain pattern is random in nature. The ability to control the spatial arrangement of the electronic phases at microscopic scales is highly desirable for tailoring their macroscopic properties and/or designing novel electronic devices. Here we report the formation of EPS nanoscale network in a mono-atomically stacked LaMnO3/CaMnO3/PrMnO3 superlattice grown on SrTiO3 (STO) (001) substrate, which is known to have an antiferromagnetic (AFM) insulating ground state. The EPS nano-network is a consequence of an internal strain relaxation triggered by the structural domain formation of the underlying STO substrate at low temperatures. The same nanoscale network pattern can be reproduced upon temperature cycling allowing us to employ different local imaging techniques to directly compare the magnetic and transport state of a single EPS domain. Our results confirm the one-to-one correspondence between ferromagnetic (AFM) to metallic (insulating) state in manganite. It also represents a significant step in a paradigm shift from passively characterizing EPS in strongly correlated systems to actively engaging in its manipulation.

Self-rolling of vanadium dioxide nanomembranes for enhanced multi-level solar modulation.

Thermochromic window develops as a competitive solution for carbon emissions due to comprehensive advantages of its passivity and effective utilization of energy. How to further enhance the solar modulation ([Formula: see text]) of thermochromic windows while ensuring high luminous transmittance ([Formula: see text]) becomes the latest challenge to touch the limit of energy efficiency. Here, we show a smart window combining mechanochromism with thermochromism by self-rolling of vanadium dioxide (VO2) nanomembranes to enhance multi-level solar modulation. The mechanochromism is introduced by the temperature-controlled regulation of curvature of rolled-up smart window, which benefits from effective strain adjustment in VO2 nanomembranes upon the phase transition. Under geometry design and optimization, the rolled-up smart window with high [Formula: see text] and [Formula: see text] is achieved for the modulation of indoor temperature self-adapted to seasons and climate. Furthermore, such rolled-up smart window enables high infrared reflectance after triggered phase transition and acts as a smart lens protective cover for strong radiation. This work supports the feasibility of self-rolling technology in smart windows and lens protection, which promises broad interest and practical applications of self-adapting devices and systems for smart building, intelligent sensors and actuators with the perspective of energy efficiency.