Imposing additional confinement in two-dimensional (2D) materials can yield further control over the associated electronic, optical, and topological properties. However, synthesis of ultra-narrow nanoribbons (NRs) remains a challenge, particularly for the transition metal dichalcogenides (TMDs), and synthesizing TMD NRs narrower than 50 nm has remained elusive. Here, we report the vapor-phase synthesis of ultra-narrow TaS2 NRs. The NRs are grown within the hollow cavity of carbon nanotubes, thereby limiting their lateral dimensions and layer number, while simultaneously stabilizing them against the environment. The NRs reach the monolayer (ML) limit and exhibit widths as low as 2.5 nm. Atomic-resolution scanning transmission electron microscopy (STEM) reveals the detailed atomic structure of the ultra-narrow NRs and we observe a hitherto unseen atomic structure supermodulation phenomenon of ordered defect arrays within the NRs. First-principles calculations based on density functional theory (DFT) show the presence of flat bands, as well as edge- and boundary-localized states, and help identify the atomic configuration of the supermodulation. Nanotube-templated synthesis represents a unique, transferable, and broadly deployable route toward ultra-narrow TMD NR growth.
It is a challenge to synthesize graphene nanoribbons (GNRs) with narrow widths and smooth edges in large scale. Our first principles study on the hydrogenation of GNRs shows that the hydrogenation starts from the edges of GNRs and proceeds gradually toward the middle of the GNRs so as to maximize the number of carbon-carbon $π$-$π$ bonds. Furthermore, the partially hydrogenated wide GNRs have similar electronic and magnetic properties as those of narrow GNRs. Therefore, it is not necessary to directly produce narrow GNRs for realistic applications because partial hydrogenation could make wide …
Graphene nanoribbons present diverse electronic properties ranging from semiconducting to half-metallic, depending on their geometry, dimensions and chemical composition. Here we present a route to control these properties via externally applied mechanical deformations. Using state-of-the-art density functional theory calculations combined with classical elasticity theory considerations, we find a remarkable Young's modulus value of ~7 TPa for ultra-narrow graphene strips and a pronounced electromechanical response towards bending and torsional deformations. Given the current advances in the s…
A topological insulator is a new state of matter, possessing gapless spin-locking surface states across the bulk band gap which has created new opportunities from novel electronics to energy conversion. However, the large concentration of bulk residual carriers has been a major challenge for revealing the property of the topological surface state via electron transport measurement. Here we report surface state dominated transport in Sb-doped Bi2Se3 nanoribbons with very low bulk electron concentrations. In the nanoribbons with sub-10nm thickness protected by a ZnO layer, we demonstrate complet…
Edge states in narrow quasi two-dimensional nanostructures determine, to a large extent, their electric, thermoelectric and magnetic properties. Non-magnetic edge states may quite often lead to topological insulator type behavior. However another scenario develops when the zigzag edges are magnetic and the time reversal symmetry is broken. In this work we report on the electronic band structure modifications, electrical conductance and thermoelectric properties of narrow zigzag nanoribbons with spontaneously magnetized edges. Theoretical studies based on the Kane-Mele- Hubbard tight-binding mo…
We investigate the influence of low-dimensionality and disorder in phonon transport in ultra-narrow armchair graphene nanoribbons (GNRs) using non-equilibrium Greens function (NEGF) simulation techniques. We specifically focus on how different parts of the phonon spectrum are influenced by geometrical confinement and line edge roughness. With the introduction of line edge roughness, the phonon transmission is reduced, but non-uniformly throughout the spectrum. We identify four distinct behaviors within the phonon spectrum in the presence of disorder: i) the low-energy, low-wavevector acoustic …
The thermal conductivity of low-dimensional materials and graphene nanoribbons in particular, is limited by the strength of line-edge-roughness scattering. One way to characterize the roughness strength is the dependency of the thermal conductivity on the channel width in the form W^β. Although in the case of electronic transport this dependency is very well studied, resulting in W^6 for nanowires and quantum wells and W^4 for nanoribbons, in the case of phonon transport it is not yet clear what this dependence is. In this work, using lattice dynamics and Non-Equilibrium Greens Function simula…
Here we present a combined experimental and theoretical study of graphene nanoribbons (GNRs), where detailed multi-wavelength Raman measurements are integrated by accurate ab initio simulations. Our study covers several ultra-narrow GNRs, obtained by means of solution-based bottom-up synthetic approach, allowing to rationalize the effect of edge morphology, position and type of functional groups as well as the length on the GNR Raman spectrum. We show that the low-energy region, especially in presence of bulky functional groups is populated by several modes, and a single radial breathing-like …
The electronic, optical and magnetic properties of graphene nanoribbons (GNRs) can be engineered by controlling their edge structure and width with atomic precision through bottom-up fabrication based on molecular precursors. This approach offers a unique platform for all-carbon electronic devices but requires careful optimization of the growth conditions to match structural requirements for successful device integration, with GNR length being the most critical parameter. In this work, we study the growth, characterization, and device integration of 5-atom wide armchair GNRs (5-AGNRs), which a…
Graphene nanoribbons have attracted attention for their novel electronic and spin transport properties1-6, and because nanoribbons less than 10 nm wide have a band gap that can be used to make field effect transistors. However, producing nanoribbons of very high quality, or in high volumes, remains a challenge. Here, we show that pristine few-layer nanoribbons can be produced by unzipping mildly gas-phase oxidized multiwalled carbon nanotube using mechanical sonication in an organic solvent. The nanoribbons exhibit very high quality, with smooth edges (as seen by high-resolution transmission e…
Aligned graphene nanoribbon (GNR) arrays were made by unzipping of aligned single-walled and few-walled carbon nanotube (CNT) arrays. Nanotube unzipping was achieved by a polymer-protected Ar plasma etching method, and the resulting nanoribbon array was transferred onto any substrates. Atomic force microscope (AFM) imaging and Raman mapping on the same CNTs before and after unzipping confirmed that ~80% of CNTs were opened up to form single layer sub-10 nm GNRs. Electrical devices made from the GNRs (after annealing in H2 at high temperature) showed on/off current (Ion/Ioff) ratios up to 103 a…
Three typical one-dimensional (1D)/quasi-1D nanocarbons, linear carbon chains, carbon nanotubes, and graphene nanoribbons have been proven to grow inside single-wall carbon nanotubes. This gives rise to three types of hybrid materials whose behaviour and properties compared among each other are far from understood. After proving successful the synthesis of these nanostructured materials in recently published work, we have now been able to study their oxidation stability systematically by using resonance Raman spectroscopy. Surprisingly, the linear carbon chains, which have been theoretically p…
Elemental phosphorus nanostructures are notorious for a large number of allotropes, which limits their usefulness as semiconductors. To limit this structural diversity, we synthesize selectively quasi-1D phosphorus nanostructures inside carbon nanotubes (CNTs) that act both as stable templates and nanoreactors. Whereas zigzag phosphorus nanoribbons form preferably in CNTs with an inner diameter exceeding 1.4 nm, a previously unknown square columnar structure of phosphorus is observed to form inside narrower nanotubes. Our findings are supported by electron microscopy and Raman spectroscopy obs…
We present the successful synthesis of single-atom-thick borophene nanoribbons (BNRs) by self-assembly of boron on Ag(110) surface. The scanning tunneling microscopy (STM) studies reveal high quality BNRs: all the ribbons are along the [-110] direction of Ag(110), and can run across the steps on the surface. The width of ribbons is distributed in a narrow range around 10.3 nm. High resolution STM images revealed four ordered surface structures in BNRs. Combined with DFT calculations, we found that all the four structures of boron nanoribbons consist of the boron chains with different width, se…
Ultra-high vacuum Raman platform for in situ characterization of graphene nanoribbons
Department of Information Technology and Electrical Engineering, ETH Zürich - Swiss Federal Institute of Technology Zürich（苏黎世联邦理工学院信息与电气工程系）；Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院）；Max Planck Institute for Polymer Research（马克斯·普朗克聚合物研究所）；Faculty of Chemistry and Food Chemistry & Center for Advanced Electronics Dresden, TUD - Dresden University of Technology（德累斯顿工业大学化学与食品化学学院及先进电子中心）；Max Planck Institute of Microstructure Physics（马克斯·普朗克微观结构物理研究所）
