Erratum: Phonon-Mediated Interlayer Conductance in Twisted Graphene Bilayers [Phys. Rev. Lett. 109, 236604 (2012)].

This corrects the article DOI: 10.1103/PhysRevLett.109.236604.

Interface dynamics and crystal phase switching in GaAs nanowires.

Controlled formation of non-equilibrium crystal structures is one of the most important challenges in crystal growth. Catalytically grown nanowires are ideal systems for studying the fundamental physics of phase selection, and could lead to new electronic applications based on the engineering of crystal phases. Here we image gallium arsenide (GaAs) nanowires during growth as they switch between phases as a result of varying growth conditions. We find clear differences between the growth dynamics of the phases, including differences in interface morphology, step flow and catalyst geometry. We explain these differences, and the phase selection, using a model that relates the catalyst volume, the contact angle at the trijunction (the point at which solid, liquid and vapour meet) and the nucleation site of each new layer of GaAs. This model allows us to predict the conditions under which each phase should be observed, and use these predictions to design GaAs heterostructures. These results could apply to phase selection in other nanowire systems.

Band Structure and Contact Resistance of Carbon Nanotubes Deformed by a Metal Contact.

Capillary and van der Waals forces cause nanotubes to deform or even collapse under metal contacts. Using ab initio band structure calculations, we find that these deformations reduce the band gap by as much as 30%, while fully collapsed nanotubes become metallic. Moreover, degeneracy lifting due to the broken axial symmetry, and wave functions mismatch between the fully collapsed and the round portions of a CNT, lead to a 3 times higher contact resistance. The latter we demonstrate by contact resistance calculations within the tight-binding approach.

Coherent Plasmon and Phonon-Plasmon Resonances in Carbon Nanotubes.

Carbon nanotubes provide a rare access point into the plasmon physics of one-dimensional electronic systems. By assembling purified nanotubes into uniformly sized arrays, we show that they support coherent plasmon resonances, that these plasmons couple to nanotube and substrate phonons, and that the resulting phonon-plasmon resonances have quality factors as high as 10. Because nanotube plasmons intensely strengthen electromagnetic fields and light-matter interactions, they provide a compelling platform for surface-enhanced spectroscopy and tunable optical devices at deep-subwavelength scales.

Vapor-Liquid-Solid Etch of Semiconductor Surface Channels by Running Gold Nanodroplets.

We show that Au nanoparticles spontaneously move across the (001) surface of InP, InAs, and GaP when heated in the presence of water vapor. As they move, the particles etch crystallographically aligned grooves into the surface. We show that this process is a negative analogue of the vapor-liquid-solid (VLS) growth of semiconductor nanowires: the semiconductor dissolves into the catalyst and reacts with water vapor at the catalyst surface to create volatile oxides, depleting the dissolved cations and anions and thus sustaining the dissolution process. This VLS etching process provides a new tool for directed assembly of structures with sublithographic dimensions, as small as a few nanometers in diameter. Au particles above 100 nm in size do not exhibit this process but remain stationary, with oxide accumulating around the particles.

Carbon nanotube complementary wrap-gate transistors.

Among the challenges hindering the integration of carbon nanotube (CNT) transistors in digital technology are the lack of a scalable self-aligned gate and complementary n- and p-type devices. We report CNT transistors with self-aligned gates scaled down to 20 nm in the ideal gate-all-around geometry. Uniformity of the gate wrapping the nanotube channels is confirmed, and the process is shown not to damage the CNTs. Further, both n- and p-type transistors were realized by using the appropriate gate dielectric-HfO2 yielded n-type and Al2O3 yielded p-type-with quantum simulations used to explore the impact of important device parameters on performance. These discoveries not only provide a promising platform for further research into gate-all-around CNT devices but also demonstrate that scalable digital switches with realistic technological potential can be achieved with carbon nanotubes.

Structure and electronic transport in graphene wrinkles.

Wrinkling is a ubiquitous phenomenon in two-dimensional membranes. In particular, in the large-scale growth of graphene on metallic substrates, high densities of wrinkles are commonly observed. Despite their prevalence and potential impact on large-scale graphene electronics, relatively little is known about their structural morphology and electronic properties. Surveying the graphene landscape using atomic force microscopy, we found that wrinkles reach a certain maximum height before folding over. Calculations of the energetics explain the morphological transition and indicate that the tall ripples are collapsed into narrow standing wrinkles by van der Waals forces, analogous to large-diameter nanotubes. Quantum transport calculations show that conductance through these "collapsed wrinkle" structures is limited mainly by a density-of-states bottleneck and by interlayer tunneling across the collapsed bilayer region. Also through systematic measurements across large numbers of devices with wide "folded wrinkles", we find a distinct anisotropy in their electrical resistivity, consistent with our transport simulations. These results highlight the coupling between morphology and electronic properties, which has important practical implications for large-scale high-speed graphene electronics.

Correction to "Reversible Decomposition of Single-Crystal Methylammonium Lead Iodide Perovskite Nanorods".

[This corrects the article DOI: 10.1021/acscentsci.0c00385.].

Chip-Scale Droop-Free Fin Light-Emitting Diodes Using Facet-Selective Contacts.

Sub-micron-size light sources are currently extremely dim, achieving nanowatt output powers due to the current density and temperature droop. Recently, we reported a droop-free fin light-emitting diode (LED) pixel that at high current densities becomes a laser with record output power in the microwatt range. Here, we show a scalable method for selectively metallizing fins via their nonpolar side facet that allows electrical injection to sub-200 nm wide n-ZnO fins on p-GaN with at least 0.8 µm2 active area. Electrically addressable fin LEDs are fabricated in a linear array format using standard 2 µm resolution photolithography. Electroluminescence analysis across different pixels shows that the fin acts as the active region of the LED and generates a narrow-band ultraviolet emission between ≈368 and ≈390 nm. Investigating fins at high current densities, ranging from 100 to 2000 kA/cm2, shows that their emission increases without any decline even as the junction temperature reaches a range of 200-340 °C. The absence of electron leakage to p-GaN at high injection levels and an undetectable electron-hole escape from the fin at high temperatures indicate that the fin shape is highly efficient in controlling the nonradiative recombination pathways such as Auger recombination. The fin LED geometry is expected to enable the realization of high-brightness arrays of light sources at sub-micron-size regimes suitable for operation at high temperatures and high current densities.

Tuning the Doping of Epitaxial Graphene on a Conventional Semiconductor via Substrate Surface Reconstruction.

Combining scanning tunneling microscopy and angle-resolved photoemission spectroscopy, we demonstrate how to tune the doping of epitaxial graphene from p to n by exploiting the structural changes that occur spontaneously on the Ge surface upon thermal annealing. Furthermore, using first-principle calculations, we build a model that successfully reproduces the experimental observations. Since the ability to modify graphene electronic properties is of fundamental importance when it comes to applications, our results provide an important contribution toward the integration of graphene with conventional semiconductors.

Reversible Decomposition of Single-Crystal Methylammonium Lead Iodide Perovskite Nanorods.

Perovskite solar cells offer remarkable performance, but further advances will require deeper understanding and control of the materials and processing. Here, we fabricate the first single crystal nanorods of intermediate phase (MAI-PbI2-DMSO), allowing us to directly observe the phase evolution while annealing in situ in a high-vacuum transmission electron microscope, which lets up separate thermal effects from other environmental conditions such as oxygen and moisture. We attain the first full determination of the crystal structures and orientations of the intermediate phase, evolving perovskite, precipitating PbI2, and e-beam induced PbI2 during phase conversion and decomposition. Surprisingly, the perovskite decomposition to PbI2 is reversible upon cooling, critical for long-term device endurance due to the formation of MAI-rich MAPbI3 and PbI2 upon heating. Quantitative measurements with a thermodynamic model suggest the decomposition is entropically driven. The single crystal MAPbI3 nanorods obtained via thermal cycling exhibit excellent mobility and trap density, with full reversibility up to 100 °C (above the maximum temperature for solar cell operation) under high vacuum, offering unique potential for high-performance flexible solar cells.

High-brightness lasing at submicrometer enabled by droop-free fin light-emitting diodes (LEDs).

"Efficiency droop," i.e., a decline in brightness of light-emitting diodes (LEDs) at high electrical currents, limits the performance of all commercial LEDs and has limited the output power of submicrometer LEDs and lasers to nanowatts. We present a fin p-n junction LED pixel that eliminates efficiency droop, allowing LED brightness to increase linearly with current. With record current densities of 1000 kA/cm2, the LEDs transition to lasing, with brightness over 20 µW. Despite a light extraction efficiency of only 15%, these devices exceed the output power of any previous electrically driven submicrometer LED or laser pixel by 100 to 1000 times while showing comparable external quantum efficiencies. Modeling suggests that spreading of the electron-hole recombination region in fin LEDs at high injection levels suppresses the nonradiative Auger recombination processes. Further refinement of this design is expected to enable a new generation of high-brightness LED and laser pixels for macro- and microscale applications.

Surface Crystallization of Liquid Au-Si and Its Impact on Catalysis.

In situ transmission electron microscopy reveals that an atomically thin crystalline phase at the surface of liquid Au-Si is stable over an unexpectedly wide range of conditions. By measuring the surface structure as a function of liquid temperature and composition, a simple thermodynamic model is developed to explain the stability of the ordered phase. The presence of surface ordering plays a key role in the pathway by which the Au-Si eutectic solidifies and also dramatically affects the catalytic properties of the liquid, explaining the anomalously slow growth kinetics of Si nanowires at low temperature. A strategy to control the presence of the surface phase is discussed, using it as a tool in designing strategies for nanostructure growth.

Strain distributions and their influence on electronic structures of WSe2-MoS2 laterally strained heterojunctions.

Monolayer transition metal dichalcogenide heterojunctions, including vertical and lateral p-n junctions, have attracted considerable attention due to their potential applications in electronics and optoelectronics. Lattice-misfit strain in atomically abrupt lateral heterojunctions, such as WSe2-MoS2, offers a new band-engineering strategy for tailoring their electronic properties. However, this approach requires an understanding of the strain distribution and its effect on band alignment. Here, we study a WSe2-MoS2 lateral heterojunction using scanning tunnelling microscopy and image its moiré pattern to map the full two-dimensional strain tensor with high spatial resolution. Using scanning tunnelling spectroscopy, we measure both the strain and the band alignment of the WSe2-MoS2 lateral heterojunction. We find that the misfit strain induces type II to type I band alignment transformation. Scanning transmission electron microscopy reveals the dislocations at the interface that partially relieve the strain. Finally, we observe a distinctive electronic structure at the interface due to hetero-bonding.

Carbon nanotube transistors scaled to a 40-nanometer footprint.

The International Technology Roadmap for Semiconductors challenges the device research community to reduce the transistor footprint containing all components to 40 nanometers within the next decade. We report on a p-channel transistor scaled to such an extremely small dimension. Built on one semiconducting carbon nanotube, it occupies less than half the space of leading silicon technologies, while delivering a significantly higher pitch-normalized current density-above 0.9 milliampere per micrometer at a low supply voltage of 0.5 volts with a subthreshold swing of 85 millivolts per decade. Furthermore, we show transistors with the same small footprint built on actual high-density arrays of such nanotubes that deliver higher current than that of the best-competing silicon devices under the same overdrive, without any normalization. We achieve this using low-resistance end-bonded contacts, a high-purity semiconducting carbon nanotube source, and self-assembly to pack nanotubes into full surface-coverage aligned arrays.

Self-assembly of ordered graphene nanodot arrays.

The ability to fabricate nanoscale domains of uniform size in two-dimensional materials could potentially enable new applications in nanoelectronics and the development of innovative metamaterials. However, achieving even minimal control over the growth of two-dimensional lateral heterostructures at such extreme dimensions has proven exceptionally challenging. Here we show the spontaneous formation of ordered arrays of graphene nano-domains (dots), epitaxially embedded in a two-dimensional boron-carbon-nitrogen alloy. These dots exhibit a strikingly uniform size of 1.6 ± 0.2 nm and strong ordering, and the array periodicity can be tuned by adjusting the growth conditions. We explain this behaviour with a model incorporating dot-boundary energy, a moiré-modulated substrate interaction and a long-range repulsion between dots. This new two-dimensional material, which theory predicts to be an ordered composite of uniform-size semiconducting graphene quantum dots laterally integrated within a larger-bandgap matrix, holds promise for novel electronic and optoelectronic properties, with a variety of potential device applications.The nanoscale patterning of two-dimensional materials offers the possibility of novel optoelectronic properties; however, it remains challenging. Here, Camilli et al. show the self-assembly of large arrays of highly-uniform graphene dots imbedded in a BCN matrix, enabling novel devices.

Erratum: Self-assembly of ordered graphene nanodot arrays.

Change History: A correction to this article has been published and is linked from the HTML version of this article.

Visualizing band offsets and edge states in bilayer-monolayer transition metal dichalcogenides lateral heterojunction.

Semiconductor heterostructures are fundamental building blocks for many important device applications. The emergence of two-dimensional semiconductors opens up a new realm for creating heterostructures. As the bandgaps of transition metal dichalcogenides thin films have sensitive layer dependence, it is natural to create lateral heterojunctions (HJs) using the same materials with different thicknesses. Here we show the real space image of electronic structures across the bilayer-monolayer interface in MoSe2 and WSe2, using scanning tunnelling microscopy and spectroscopy. Most bilayer-monolayer HJs are found to have a zig-zag-orientated interface, and the band alignment of such atomically sharp HJs is of type-I with a well-defined interface mode that acts as a narrower-gap quantum wire. The ability to utilize such commonly existing thickness terraces as lateral HJs is a crucial addition to the tool set for device applications based on atomically thin transition metal dichalcogenides, with the advantage of easy and flexible implementation.

Approaching the ideal elastic strain limit in silicon nanowires.

Achieving high elasticity for silicon (Si) nanowires, one of the most important and versatile building blocks in nanoelectronics, would enable their application in flexible electronics and bio-nano interfaces. We show that vapor-liquid-solid-grown single-crystalline Si nanowires with diameters of ~100 nm can be repeatedly stretched above 10% elastic strain at room temperature, approaching the theoretical elastic limit of silicon (17 to 20%). A few samples even reached ~16% tensile strain, with estimated fracture stress up to ~20 GPa. The deformations were fully reversible and hysteresis-free under loading-unloading tests with varied strain rates, and the failures still occurred in brittle fracture, with no visible sign of plasticity. The ability to achieve this "deep ultra-strength" for Si nanowires can be attributed mainly to their pristine, defect-scarce, nanosized single-crystalline structure and atomically smooth surfaces. This result indicates that semiconductor nanowires could have ultra-large elasticity with tunable band structures for promising "elastic strain engineering" applications.

End-bonded contacts for carbon nanotube transistors with low, size-independent resistance.

Moving beyond the limits of silicon transistors requires both a high-performance channel and high-quality electrical contacts. Carbon nanotubes provide high-performance channels below 10 nanometers, but as with silicon, the increase in contact resistance with decreasing size becomes a major performance roadblock. We report a single-walled carbon nanotube (SWNT) transistor technology with an end-bonded contact scheme that leads to size-independent contact resistance to overcome the scaling limits of conventional side-bonded or planar contact schemes. A high-performance SWNT transistor was fabricated with a sub-10-nanometer contact length, showing a device resistance below 36 kilohms and on-current above 15 microampere per tube. The p-type end-bonded contact, formed through the reaction of molybdenum with the SWNT to form carbide, also exhibited no Schottky barrier. This strategy promises high-performance SWNT transistors, enabling future ultimately scaled device technologies.