Graphene nanoribbons (GNRs), quasi-one-dimensional graphene strips, have shown great potential for nanoscale electronics, optoelectronics, and photonics. Atomically precise GNRs can be "bottom-up" synthesized by surface-assisted assembly of molecular building blocks under ultra-high-vacuum conditions. However, large-scale and efficient synthesis of such GNRs at low cost remains a significant challenge. Here we report an efficient "bottom-up" chemical vapor deposition (CVD) process for inexpensive and high-throughput growth of structurally defined GNRs with varying structures under ambient-pressure conditions. The high quality of our CVD-grown GNRs is validated by a combination of different spectroscopic and microscopic characterizations. Facile, large-area transfer of GNRs onto insulating substrates and subsequent device fabrication demonstrate their promising potential as semiconducting materials, exhibiting high current on/off ratios up to 6000 in field-effect transistor devices. This value is 3 orders of magnitude higher than values reported so far for other thin-film transistors of structurally defined GNRs. Notably, on-surface mass spectrometry analyses of polymer precursors provide unprecedented evidence for the chemical structures of the resulting GNRs, especially the heteroatom doping and heterojunctions. These results pave the way toward the scalable and controllable growth of GNRs for future applications.
wafer-scale, with good crystallinity and with contamination levels compatible with large-scale back-end-of-line (BEOL) integration. At present, chemical vapor deposition (CVD) on catalytic copper (Cu) substrates is widely recognized as the most promising route to obtain scalable monolayer graphene for electronic and optoelectronic applications. [1][2][3][4] However, significant hurdles are limiting the actual integration of CVD graphene grown on Cu for most applications. In the first instance, the unavoidable transfer process over wafer-scale is rather cumbersome and introduces contamination, unintentional doping, and mechanical stress, [5][6][7] which adversely impact the physical integrity and electrical performance [8] of the graphene layer. The significant challenge involved in carrying out this seemingly straightforward task is reflected by the vast literature on large-scale transfer processes. Second, metallic contamination levels in transferred CVD graphene grown on Cu are typically well-above the specifications requested for BEOL integration. [6] Clearly, asThe adoption of graphene in electronics, optoelectronics, and photonics is hindered by the difficulty in obtaining high-quality material on technologically relevant substrates, over wafer-scale sizes, and with metal contamination levels compatible with industrial requirements. To date, the direct growth of graphene on insulating substrates has proved to be challenging, usually requiring metal-catalysts or yielding defective graphene. In this work, a metal-free approach implemented in commercially available reactors to obtain high-quality monolayer graphene on c-plane sapphire substrates via chemical vapor deposition is demonstrated. Low energy electron diffraction, low energy electron microscopy, and scanning tunneling microscopy measurements identify the Al-rich reconstruction9° of sapphire to be crucial for obtaining epitaxial graphene. Raman spectroscopy and electrical transport measurements reveal high-quality graphene with mobilities consistently above 2000 cm 2 V −1 s −1 . The process is scaled up to 4 and 6 in. wafers sizes and metal contamination levels are retrieved to be within the limits for back-end-ofline integration. The growth process introduced here establishes a method for the synthesis of wafer-scale graphene films on a technologically viable basis.
Graphene nanoribbons (GNRs) are a novel and intriguing class of materials in the field of nanoelectronics, since their properties, solely defined by their width and edge type, are controllable with high precision directly from synthesis. Here we study the correlation between the GNR structure and the corresponding device electrical properties. We investigated a series of field effect devices consisting of a film of armchair GNRs with different structures (namely width and/or length) as the transistor channel, contacted with narrowly spaced graphene sheets as the source-drain electrodes. By analyzing several tens of junctions for each individual GNR type, we observe that the values of the output current display a width-dependent behavior, indicating electronic bandgaps in good agreement with the predicted theoretical values. These results provide insights into the link between the ribbon structure and the device properties, which are fundamental for the development of GNR-based electronics.
We report compact, scalable, high-performance, waveguide integrated graphene-based photodetectors (GPDs) for telecom and datacom applications, not affected by dark current. To exploit the photothermoelectric (PTE) effect, our devices rely on a graphene/polymer/graphene stack with static top split gates. The polymeric dielectric, poly(vinyl alcohol) (PVA), allows us to preserve graphene quality and to generate a controllable p−n junction. Both graphene layers are fabricated using aligned single-crystal graphene arrays grown by chemical vapor deposition. The use of PVA yields a low charge inhomogeneity ∼8 × 10 10 cm −2 at the charge neutrality point, and a large Seebeck coefficient ∼140 μV K −1 , enhancing the PTE effect. Our devices are the fastest GPDs operating with zero dark current, showing a flat frequency response up to 67 GHz without roll-off. This performance is achieved on a passive, low-cost, photonic platform, and does not rely on nanoscale plasmonic structures. This, combined with scalability and ease of integration, makes our GPDs a promising building block for next-generation optical communication devices.
Out of the different structural phases of molybdenum ditelluride (MoTe 2 ), the distorted octahedral 1T′ possesses great interest for fundamental physics and is a promising candidate for the implementation of innovative devices such as topological transistors. Indeed, 1T′-MoTe 2 is a semimetal with superconductivity, which has been predicted to be a Weyl semimetal and a quantum spin Hall insulator in bulk and monolayer form, respectively. Large instability of monolayer 1T′-MoTe 2 in environmental conditions, however, has made its investigation extremely challenging so far. In this work, we demonstrate homogeneous growth of large single-crystal (up to 500 μm) monolayer 1T′-MoTe 2 via chemical vapor deposition (CVD) and its stabilization in air with a scalable encapsulation approach. The encapsulant is obtained by electrochemically delaminating CVD hexagonal boron nitride (hBN) from copper foil, and it is applied on the freshly grown 1T′-MoTe 2 via a top-down dry lamination step. The structural and electrical properties of encapsulated 1T′-MoTe 2 have been monitored over several months to assess the degree of degradation of the material. We find that when encapsulated with hBN, the lifetime of monolayer 1T′-MoTe 2 successfully increases from a few minutes to more than a month. Furthermore, the encapsulated monolayer can be subjected to transfer, device processing, and heating and cooling cycles without degradation of its properties. The potential of this scalable heterostack is confirmed by the observation of signatures of low-temperature phase transition in monolayer 1T′-MoTe 2 by both Raman spectroscopy and electrical measurements. The growth and encapsulation methods reported in this work can be employed for further fundamental studies of this enticing material as well as facilitate the technological development of monolayer 1T′-MoTe 2 .
Ultra-narrow graphene nanoribbons (GNRs) with atomically precise structures are considered a promising class of materials for the realization of optoelectronic and photonic devices with improved functionalities. Here we report the opto-electronic characterization of a field effect transistor devices made of a layer of bottom-up synthesized GNRs contacted with multilayer graphene electrodes, showing high photoresponsivity of 5 × 10 5 A/W for small incident power in the visible-UV range. Our results show that combining the properties of intrinsic graphene with that of semiconducting GNRs is a viable route to realize novel devices for optoelectronic and sensing applications.
2-step chemical cleaning allows enhanced removal of polymeric residues from the surface of graphene, leading to significantly improved electrical and morphological properties.
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