Electrical Pumping of Perovskite Diodes: Toward Stimulated Emission.

The success of metal halide perovskites in photovoltaic and light-emitting diodes (LEDs) motivates their application as a solid-state thin-film laser. Various perovskites have shown optically pumped stimulated emission of lasing and amplified spontaneous emission (ASE), yet the ultimate goal of electrically pumped stimulated emission has not been achieved. As an essential step toward this goal, here, a perovskite diode structure that simultaneously exhibits stable operation at high current density (≈1 kA cm-2 ) and optically excited ASE (with a threshold of 180 µJ cm-2 ) is reported. This diode structure achieves an electroluminescence quantum efficiency of 0.8% at 850 A cm-2 , which is estimated to be ≈3% of the charge carrier population required to reach ASE in the same device. It is shown that the formation of a large angle waveguide mode and the reduction of parasitic absorption losses are two major design principles for diodes to obtain a positive gain for stimulated emission. In addition to its prospect as a perovskite laser, a new application of electrically pumped ASE is proposed as an ideal perovskite LED architecture allowing 100% external radiation efficiency.

Matching p-i-n-junctions and optical modes enables fast and ultra-small silicon modulators.

In this article a new method is presented that allows for low loss implementation of fast carrier transport structures in diffraction limited photonic crystal resonators. We utilize a 'node-matched doping' process in which precise silicon doping results in comb-like shaped, highly-doped diode areas that are matched to the spatial field distribution of the optical modes of a Fabry-Pérot resonator. While the doping is only applied to areas with low optical field strength, the intrinsic diode region overlaps with an optical field maximum. The presented node-matched diode-modulators, combining small size, high-speed, thermal stability and energy-efficient switching could become the centerpiece for monolithically integrated transceivers.

Rapid surface oxidation as a source of surface degradation factor for Bi2Se3.

Bismuth selenide (Bi(2)Se(3)) is a topological insulator with metallic surface states (SS) residing in a large bulk bandgap. In experiments, synthesized Bi(2)Se(3) is often heavily n-type doped due to selenium vacancies. Furthermore, it is discovered from experiments on bulk single crystals that Bi(2)Se(3) gets additional n-type doping after exposure to the atmosphere, thereby reducing the relative contribution of SS in total conductivity. In this article, transport measurements on Bi(2)Se(3) nanoribbons provide additional evidence of such environmental doping process. Systematic surface composition analyses by X-ray photoelectron spectroscopy reveal fast formation and continuous growth of native oxide on Bi(2)Se(3) under ambient conditions. In addition to n-type doping at the surface, such surface oxidation is likely the material origin of the degradation of topological SS. Appropriate surface passivation or encapsulation may be required to probe topological SS of Bi(2)Se(3) by transport measurements.

Operation of a Raman laser in bulk silicon.

A Raman laser based on a bulk silicon single crystal with 1.127 µm emission wavelength is demonstrated. The Si crystal with 30 mm length was placed into an external cavity and pumped by a Q-switched Nd:YAG master oscillator power amplifier system. Strong defocusing of the pump and Raman laser beam by free carriers was compensated by an intracavity lens. Raman laser operation with a pulse duration of 2.5 ns was identified by a Raman laser threshold significantly lower than the single-pass stimulated Raman-scattering threshold. Linear absorption losses of the 1.06415 µm pump radiation are strongly reduced by cooling the Si crystal to a temperature of 10 K.

In situ transmission electron microscopy observation of nanostructural changes in phase-change memory.

Phase-change memory (PCM) has been researched extensively as a promising alternative to flash memory. Important studies have focused on its scalability, switching speed, endurance, and new materials. Still, reliability issues and inconsistent switching in PCM devices motivate the need to further study its fundamental properties. However, many investigations treat PCM cells as black boxes; nanostructural changes inside the devices remain hidden. Here, using in situ transmission electron microscopy, we observe real-time nanostructural changes in lateral Ge(2)Sb(2)Te(5) (GST) PCM bridges during switching. We find that PCM devices with similar resistances can exhibit distinct threshold switching behaviors due to the different initial distribution of nanocrystalline and amorphous domains, explaining variability of switching behaviors of PCM cells in the literature. Our findings show a direct correlation between nanostructure and switching behavior, providing important guidelines in the design and operation of future PCM devices with improved endurance and lower variability.

Ultrathin topological insulator Bi2Se3 nanoribbons exfoliated by atomic force microscopy.

Ultrathin topological insulator nanostructures, in which coupling between top and bottom surface states takes place, are of great intellectual and practical importance. Due to the weak van der Waals interaction between adjacent quintuple layers (QLs), the layered bismuth selenide (Bi(2)Se(3)), a single Dirac-cone topological insulator with a large bulk gap, can be exfoliated down to a few QLs. In this paper, we report the first controlled mechanical exfoliation of Bi(2)Se(3) nanoribbons (>50 QLs) by an atomic force microscope (AFM) tip down to a single QL. Microwave impedance microscopy is employed to map out the local conductivity of such ultrathin nanoribbons, showing drastic difference in sheet resistance between 1-2 QLs and 4-5 QLs. Transport measurement carried out on an exfoliated (50 QLs) ribbons. These AFM-exfoliated thin nanoribbons afford interesting candidates for studying the transition from quantum spin Hall surface to edge states.

Few-layer nanoplates of Bi 2 Se 3 and Bi 2 Te 3 with highly tunable chemical potential.

A topological insulator (TI) represents an unconventional quantum phase of matter with insulating bulk band gap and metallic surface states. Recent theoretical calculations and photoemission spectroscopy measurements show that group V-VI materials Bi(2)Se(3), Bi(2)Te(3), and Sb(2)Te(3) are TIs with a single Dirac cone on the surface. These materials have anisotropic, layered structures, in which five atomic layers are covalently bonded to form a quintuple layer, and quintuple layers interact weakly through van der Waals interaction to form the crystal. A few quintuple layers of these materials are predicted to exhibit interesting surface properties. Different from our previous nanoribbon study, here we report the synthesis and characterizations of ultrathin Bi(2)Te(3) and Bi(2)Se(3) nanoplates with thickness down to 3 nm (3 quintuple layers), via catalyst-free vapor-solid (VS) growth mechanism. Optical images reveal thickness-dependent color and contrast for nanoplates grown on oxidized silicon (300 nm SiO(2)/Si). As a new member of TI nanomaterials, ultrathin TI nanoplates have an extremely large surface-to-volume ratio and can be electrically gated more effectively than the bulk form, potentially enhancing surface state effects in transport measurements. Low-temperature transport measurements of a single nanoplate device, with a high-k dielectric top gate, show decrease in carrier concentration by several times and large tuning of chemical potential.

Magnetic doping and kondo effect in bi(2)se(3) nanoribbons.

A simple surface band structure and a large bulk band gap have allowed Bi2Se3 to become a reference material for the newly discovered three-dimensional topological insulators, which exhibit topologically protected conducting surface states that reside inside the bulk band gap. Studying topological insulators such as Bi2Se3 in nanostructures is advantageous because of the high surface-to-volume ratio, which enhances effects from the surface states; recently reported Aharonov-Bohm oscillation in topological insulator nanoribbons by some of us is a good example. Theoretically, introducing magnetic impurities in topological insulators is predicted to open a small gap in the surface states by breaking time-reversal symmetry. Here, we present synthesis of magnetically doped Bi2Se3 nanoribbons by vapor-liquid-solid growth using magnetic metal thin films as catalysts. Although the doping concentration is less than approximately 2%, low-temperature transport measurements of the Fe-doped Bi2Se3 nanoribbon devices show a clear Kondo effect at temperatures below 30 K, confirming the presence of magnetic impurities in the Bi2Se3 nanoribbons. The capability to dope topological insulator nanostructures magnetically opens up exciting opportunities for spintronics.

Aharonov-Bohm interference in topological insulator nanoribbons.

Topological insulators represent unusual phases of quantum matter with an insulating bulk gap and gapless edges or surface states. The two-dimensional topological insulator phase was predicted in HgTe quantum wells and confirmed by transport measurements. Recently, Bi(2)Se(3) and related materials have been proposed as three-dimensional topological insulators with a single Dirac cone on the surface, protected by time-reversal symmetry. The topological surface states have been observed by angle-resolved photoemission spectroscopy experiments. However, few transport measurements in this context have been reported, presumably owing to the predominance of bulk carriers from crystal defects or thermal excitations. Here we show unambiguous transport evidence of topological surface states through periodic quantum interference effects in layered single-crystalline Bi(2)Se(3) nanoribbons, which have larger surface-to-volume ratios than bulk materials and can therefore manifest surface effects. Pronounced Aharonov-Bohm oscillations in the magnetoresistance clearly demonstrate the coherent propagation of two-dimensional electrons around the perimeter of the nanoribbon surface, as expected from the topological nature of the surface states. The dominance of the primary h/e oscillation, where h is Planck's constant and e is the electron charge, and its temperature dependence demonstrate the robustness of these states. Our results suggest that topological insulator nanoribbons afford promising materials for future spintronic devices at room temperature.

Topological insulator nanowires and nanoribbons.

Recent theoretical calculations and photoemission spectroscopy measurements on the bulk Bi(2)Se(3) material show that it is a three-dimensional topological insulator possessing conductive surface states with nondegenerate spins, attractive for dissipationless electronics and spintronics applications. Nanoscale topological insulator materials have a large surface-to-volume ratio that can manifest the conductive surface states and are promising candidates for devices. Here we report the synthesis and characterization of high quality single crystalline Bi(2)Se(3) nanomaterials with a variety of morphologies. The synthesis of Bi(2)Se(3) nanowires and nanoribbons employs Au-catalyzed vapor-liquid-solid (VLS) mechanism. Nanowires, which exhibit rough surfaces, are formed by stacking nanoplatelets along the axial direction of the wires. Nanoribbons are grown along [1120] direction with a rectangular cross-section and have diverse morphologies, including quasi-one-dimensional, sheetlike, zigzag and sawtooth shapes. Scanning tunneling microscopy (STM) studies on nanoribbons show atomically smooth surfaces with approximately 1 nm step edges, indicating single Se-Bi-Se-Bi-Se quintuple layers. STM measurements reveal a honeycomb atomic lattice, suggesting that the STM tip couples not only to the top Se atomic layer, but also to the Bi atomic layer underneath, which opens up the possibility to investigate the contribution of different atomic orbitals to the topological surface states. Transport measurements of a single nanoribbon device (four terminal resistance and Hall resistance) show great promise for nanoribbons as candidates to study topological surface states.

Nanoscale Electronic Inhomogeneity in In2Se3 Nanoribbons Revealed by Microwave Impedance Microscopy.

Driven by interactions due to the charge, spin, orbital, and lattice degrees of freedom, nanoscale inhomogeneity has emerged as a new theme for materials with novel properties near multiphase boundaries. As vividly demonstrated in complex metal oxides (see refs 1-5) and chalcogenides (see refs 6 and 7), these microscopic phases are of great scientific and technological importance for research in high-temperature superconductors (see refs 1 and 2), colossal magnetoresistance effect (see ref 4), phase-change memories (see refs 5 and 6), and domain switching operations (see refs 7-9). Direct imaging on dielectric properties of these local phases, however, presents a big challenge for existing scanning probe techniques. Here, we report the observation of electronic inhomogeneity in indium selenide (In(2)Se(3)) nanoribbons (see ref 10) by near-field scanning microwave impedance microscopy (see refs 11-13). Multiple phases with local resistivity spanning 6 orders of magnitude are identified as the coexistence of superlattice, simple hexagonal lattice and amorphous structures with approximately 100 nm inhomogeneous length scale, consistent with high-resolution transmission electron microscope studies. The atomic-force-microscope-compatible microwave probe is able to perform a quantitative subsurface electrical study in a noninvasive manner. Finally, the phase change memory function in In(2)Se(3) nanoribbon devices can be locally recorded with big signals of opposite signs.

Void formation induced electrical switching in phase-change nanowires.

Solid-state structural transformation coupled with an electronic property change is an important mechanism for nonvolatile information storage technologies, such as phase-change memories. Here we exploit phase-change GeTe single-nanowire devices combined with ex situ and in situ transmission electron microscopy to correlate directly nanoscale structural transformations with electrical switching and discover surprising results. Instead of crystalline-amorphous transformation, the dominant switching mechanism during multiple cycling appears to be the opening and closing of voids in the nanowires due to material migration, which offers a new mechanism for memory. During switching, composition change and the formation of banded structural defects are observed in addition to the expected crystal-amorphous transformation. Our method and results are important to phase-change memories specifically, but also to any device whose operation relies on a small scale structural transformation.

Morphology control of layer-structured gallium selenide nanowires.

Layer-structured group III chalcogenides have highly anisotropic properties and are attractive materials for stable photocathodes and battery electrodes. We report the controlled synthesis and characterization of layer-structured GaSe nanowires via a catalyst-assisted vapor-liquid-solid (VLS) growth mechanism during GaSe powder evaporation. GaSe nanowires consist of Se-Ga-Ga-Se layers stacked together via van der Waals interactions to form belt-shaped nanowires with a growth direction along the [11-20], width along the [1-100], and height along the [0001] direction. Nanobelts exhibit a variety of morphologies including straight, zigzag, and saw-tooth shapes. These morphologies are realized by controlling the growth temperature and time so that the actual catalysts have a chemical composition of Au, Au-Ga alloy, or Ga. The participation of Ga in the VLS catalyst is important for achieving different morphologies of GaSe. In addition, GaSe nanotubes are also prepared by a slow growth process.

Synthesis and characterization of phase-change nanowires.

Phase-change memory materials have stimulated a great deal of interest although the size-dependent behaviors have not been well studied due to the lack of method for producing their nanoscale structures. We report the synthesis and characterization of GeTe and Sb(2)Te(3) phase-change nanowires via a vapor-liquid-solid growth mechanism. The as-grown GeTe nanowires have three different types of morphologies: single-crystalline straight and helical rhombohedral GeTe nanowires and amorphous curly GeO(2) nanowires. All the Sb(2)Te(3) nanowires are single-crystalline.