Protocols and tools to enable reproducibility in 2D materials research

The layered two-dimensional (2D) materials, e.g., the well-known graphene, transition metal dichalcogenides, and topological insulators, have attracted great interest of researchers from fundamental research as well as industries owing to their intriguing properties in a number of aspects. In practical applications, the efficient modification of the features of 2D materials is compelling and essential to achieve desired functionalities. Ion implantation has been successfully applied to synthesize graphene. The most exotic advantage of ion beam technology is that it offers distinct options of energetic beams, which has recently shown the unique capability to modify and tailor the properties of versatile 2D materials. To name a few, the energetic ion beams could implement the surface morphology or layer-to-layer structural engineering of 2D materials. At the microcosmic level, the introduction of ion beam induced defects and intentional doping of specific ions are the basis of tailoring properties of 2D materials. By manipulating the parameters of ion beams (energies, species, fluences, incident angles, etc.), the modified 2D materials may possess novel properties, which are unprecedented in pristine ones. Promising applications based on these 2D materials with ion beam tailored features have been realized in a broad range of fields. In this work, we systematically review the latest research progress on the deployed techniques and property modifications of graphene and other 2D materials under the treatment of various ion beams. A few selected applications are presented to indicate the practical potentials of ion beam modified 2D materials in distinct areas. Perspectives on future developments are also provided by focusing on several promising topics.

Environmental resilience with 2D materials: A futuristic perspective

Two-dimensional (2D) materials have attracted increasing interest in the last few years due to their unique morphology and properties and their use in a variety of applications, ranging from electronics to energy storage or catalysis, to name a few. Apart from various well-established 2D materials, such as graphene, h-BN, or MoS2, black phosphorus (BP) has received considerable attention over the last two years because its direct bandgap and his appealing properties for electronic and ultrafast optoelectronic applications. However, its lack of environmental stability severely limits its synthesis and processing. We have recently demonstrated that high-quality, few-layer BP nanosheets, with controllable size and observable photoluminescence, can be produced in large quantities by liquid phase exfoliation under ambient conditions.1 Beyond this success, a more sophisticated chemical modification is highly desirable, like the molecular doping, that is an effective and flexible method towards modulating the electronic properties of 2D materials. Herein, we have developed a chemical route for the non-covalent functionalization of BP with different moieties, including electron-withdrawing organic molecules or tailor-made surfactants.2 Moreover we have extended these concepts towards a new 2D material: antimonene, creating stable suspensions in water and developing its non-covalent functionalization.3 1) D. Hanlon, C. Backes, E. Doherty, C. S. Cucinotta, N. C. Berner, C. Boland, K. Lee, A. Harvey, P. Lynch, Z. Gholamvand, S. F. Zhang, K. P. Wang, G. Moynihan, A. Pokle, Q. M. Ramasse, N. McEvoy, W. J. Blau, J. Wang, G. Abellan, F. Hauke, A. Hirsch, S. Sanvito, D. D. O’Regan, G. S. Duesberg, V. Nicolosi, J. N. Coleman, Nat. Commun. 2015, 6, 8563. 2) G. Abellán, V. Lloret, U. Mundloch, M. Marcia, C. Neiss, A. Görling, M. Varela, F. Hauke, A. Hirsch, Angew. Chem. In. Ed., 2016, 55 (47), 14557. 3) C. Gibaja, D. Rodriguez-San-Miguel, P. Ares, J. Gómez-Herrero, M. Varela, R. Gillen, J. Maultzsch, F. Hauke, A. Hirsch, G. Abellán, F. Zamora, Angew. Chem. In. Ed., 2016, 55 (46), 14345.

Two-dimensional (2D) materials have captured the attention of the scientific community due to the wide range of unique properties at nanometer-scale thicknesses. While significant exploratory research in 2D materials has been achieved, the understanding of 2D electronic transport and carrier dynamics remains in a nascent stage. Furthermore, because prior review articles have provided general overviews of 2D materials or specifically focused on charge transport in graphene, here we instead highlight charge transport mechanisms in post-graphene 2D materials, with particular emphasis on transition metal dichalcogenides and black phosphorus. For these systems, we delineate the intricacies of electronic transport, including band structure control with thickness and external fields, valley polarization, scattering mechanisms, electrical contacts, and doping. In addition, electronic interactions between 2D materials are considered in the form of van der Waals heterojunctions and composite films. This review concludes with a perspective on the most promising future directions in this fast-evolving field.

Two-dimensional (2D) materials have emerged as a forefront of research in materials science, driven by their exceptional and diverse properties. These materials, often with atomic thickness, exhibit phase transitions with small energy barrier, which can enable the development of energy-efficicient devices. Understanding these phase transitions is not only a fascinating scientific endeavor but also crucial for technological innovation. In this presentation, we will cover phase transitions in 2D materials, encompassing both intralayer and interlayer phenomena. We will dissect the mechanisms by which phase transitions can radically modify the electrical, optical, and mechanical properties of these materials, and discuss the engineering approaches designed to control energy barrier and transition process. Special attention will be given to the devices developed from phase transition phenomena in 2D materials, highlighting their potential applications in the realms of memory storage and sensory technology.

The Moore’s law of scaling of metal oxide semiconductor field effect transistor (MOSFET) had been a driving force toward the unprecedented advancement in development of integrated circuit over the last five decades. As the technology scales down to 7 nm node and below following the Moore’s law, conventional MOSFETs are becoming more vulnerable to extremely high off-state leakage current exhibiting a tremendous amount of standby power dissipation. Moreover, the fundamental physical limit of MOSFET of 60 mV/decade subthreshold slope exacerbates the situation further requiring current transport mechanism other than drift and diffusion for the operation of transistors. One way to limit such unrestrained amount of power dissipation is to explore novel materials with superior thermal and electrical properties compared to traditional bulk materials. On the other hand, energy efficient steep subthreshold slope devices are the other possible alternatives to conventional MOSFET based on emerging novel materials. This dissertation addresses the potential of both advanced materials and devices for development of next generation energy efficient integrated circuits. Among the different steep subthreshold slope devices, tunnel field effect transistor (TFET) has been considered as a promising candidate after MOSFET. A superior gate control on source-channel band-to-band tunneling providing subthreshold slopes well below than 60 mV/decade. With the emergence of atomically thin two-dimensional (2D) materials, interest in the design of TFET based on such novel 2D materials has also grown significantly. Graphene being the first and the most studied among 2D materials with exotic electronic and thermal properties. This dissertation primarily considers current transport modeling of graphene based tunnel devices from transport phenomena to energy efficient integrated circuit design. Three current transport models: semi-classical, semi-quantum and numerical simulations are described for the modeling of graphene nanoribbon tunnel field effect transistor (GNR TFET) where the semi-classical model is in close agreement with the quantum transport simulation. Moreover, the models produced are also extended for integrated circuit design using Verilog-A hardware description language for logic design. In order to overcome the challenges associated with the band gap engineering for making graphene transistor for logic operation, the promise of graphene based interlayer tunneling transistors are discussed along with their existing fundamental physical limitation of subthreshold slope. It has been found that such interlayer tunnel transistor has very poor electrostatic gate control on drain current. It gives subthreshold slope greater than the thermionic limit of 60 mV/decade at room temperature. In order to resolve such limitation of

Two-dimensional (2D) materials are increasingly being adopted in hybrid photonics via integration with photonic structures, including cavities. The utility of 2D materials for dielectric environment engineering in hybrid nanophotonic devices remains largely unexplored. We demonstrate self-aligned hybrid nanocavities in which 2D material flakes are used to form cavities locally wherever they are placed along the PhC waveguide postfabrication. We successfully fabricated such hybrid nanocavities with various 2D materials on silicon PhC waveguides, obtaining Q factors as high as 4.0 × 105. Remarkably, even monolayer flakes can provide sufficient local refractive index modulation to induce high Q nanocavity formation. We have also observed cavity PL enhancement in a self-aligned MoTe2 cavity device with an enhancement factor of about 15. Our results highlight the prospect of using such 2D material-induced PhC nanocavities to realize a wide range of photonic components for hybrid integrated photonic circuits.

Atomically thin nanomaterials represent a unique paradigm for interfacing with biological systems due to their mechanical flexibility, exceptional interfacial area, and ease of chemical functionalization. In particular, these two-dimensional (2D) materials are able to bend, curve, and fold in response to biologically-generated forces or other external stimuli. Such origami-like folding of 2D materials into wrinkled or crumpled topographies allows them to withstand large deformations by accordion-like unfolding, with implications for stretchable and shape-changing devices. Here, we review how mechanically manipulated 2D materials can interact with biological systems across a multitude of length scales. We focus on recent work where wrinkling, crumpling, or bending of 2D materials permits new chemical and material properties, with four case studies: (i) programming biomolecular reactivity and enhanced sensing, (ii) directed adhesion and encapsulation of bacteria or mammalian cells, (iii) stimuli-responsive actuators and soft robotics, and (iv) stretchable barrier technologies and wearable human-scale sensors. Finally, we consider future directions for manufacturing, materials and systems integration, as well as biocompatibility. Taken together, these 2D materials may enable new avenues for ultrasensitive molecular detection, biomaterial scaffolds, soft machines, and wearable technologies.

Since the discovery of Dirac physics in graphene, research in 2D materials has exploded with the aim of finding new materials and harnessing their unique and tunable electronic and optical properties. The follow-on work on 2D dielectrics and semiconductors has led to the emergence and development of hexagonal boron nitride, black phosphorus, and transition metal disulfides. However, the spectrum of good insulating materials is still very narrow. Likewise, 2D materials exhibiting correlated phenomena such as superconductivity, magnetism, and ferroelectricity have yet to be developed or discovered. These properties will significantly enrich the spectrum of functional 2D materials, particularly in the case of high phase-transition temperatures. They will also advance a fascinating fundamental frontier of size and proximity effects on correlated ground states. Here, a broad family of layered metal thio(seleno)phosphate materials that are moderate- to wide-bandgap semiconductors with incipient ionic conductivity and a host of ferroic properties are reviewed. It is argued that this material class has the potential to merge the sought-after properties of complex oxides with electronic functions of 2D and quasi-2D electronic materials, as well as to create new avenues for both applied and fundamental materials research in structural and magnetic correlations.

The development of two-dimensional (2D) materials for biomedical applications has accelerated exponentially. Contrary to their bulk counterparts, the exceptional properties of 2D materials make them highly prospective for contrast agents for bioimage, drug, and heat delivery in biomedical treatment. Nevertheless, empty space in the integration and utilisation of 2D materials in living biological systems, potential toxicity, as well as required complicated synthesis and high-cost production limit the real application of 2D materials in those advance medical treatments. On the other hand, green technology appears to be one of strategy to shed a light on the blurred employment of 2D in medical applications, thus, with the increasing reports of green technology that promote advanced technologies, here, we compile, summarise, and synthesise information on the biomedical technology of 2D materials through green technology point of view. Beginning with a fundamental understanding, of crystal structures, the working mechanism, and novel properties, this article examines the recent development of 2D materials. As well as 2D materials made from natural and biogenic resources, a recent development in green-related synthesis was also discussed. The biotechnology and biomedical-related application constraints are also discussed. The challenges, solutions, and prospects of the so-called green 2D materials are outlined.

Two-dimensional (2D) materials, such as graphene and transition-metal dichalcogenide monolayers, have unique properties that are distinctly different from those of their bulk counterparts, and hopefully possess a wide range of applications in 2D semiconductor device. Structural defects are known to have profound influences on the properties of crystalline materials; thus, correlating the defect structure with local properties in 2D material is of fundamental importance. However, electron microscopy studies of 2D materials on an atomic scale have become a challenge as most of these materials are susceptible to electron beam irradiation damage under high voltage and high dose experimental conditions. The development of low voltage aberration-corrected scanning transmission electron microscopy (STEM) has made it possible to study 2D materials at a single atom level without damaging their intrinsic structures. In addition, controllable structural modification by using electron beam becomes feasible by controlling the electron beam-sample interaction. New nanostructures can be created and novel 2D materials can be fabricated in-situ by using this approach. In this article, we review some of our recent studies of graphene and transition-metal dichalcogenides to showcase the applications of low voltage aberration corrected STEM in 2D material research.

The post-graphene era is undoubtedly marked by two-dimensional (2D) materials such as quasi-van der Waals antimonene. This emerging material has a fascinating structure, exhibits a pronounced chemical reactivity (in contrast to graphene), possesses outstanding electronic properties and has been postulated for a plethora of applications. However, chemistry and physics of antimonene remain in their infancy, but fortunately recent discoveries have shed light on its unmatched allotropy and rich chemical reactivity offering a myriad of unprecedented possibilities in terms of fundamental studies and applications. Indeed, antimonene can be considered as one of the most appealing post-graphene 2D materials reported to date, since its structure, properties and applications can be chemically engineered from the ground up (both using top-down and bottom-up approaches), offering an unprecedented level of control in the realm of 2D materials. In this review, we provide an in-depth analysis of the recent advances in the synthesis, characterization and applications of antimonene. First, we start with a general introduction to antimonene, and then we focus on its general chemistry, physical properties, characterization and synthetic strategies. We then perform a comprehensive study on the allotropy, the phase transition mechanisms, the oxidation behaviour and chemical functionalization. From a technological point of view, we further discuss the applications recently reported for antimonene in the fields of optoelectronics, catalysis, energy storage, cancer therapy and sensing. Finally, important aspects such as new scalable methodologies or the promising perspectives in biomedicine are discussed, pinpointing antimonene as a cutting-edge material of broad interest for researchers working in chemistry, physics, materials science and biomedicine.

Plasmonics and polarotonics of two dimensional (2D) materials have attracted significant attention due to their desirable dispersion relation. Regarding plasmons, according to the 2D dispersion equation, the cutoff frequency limit can be eliminated. Additionally, their large tuneability, high doping (ultradoping) range, and the existence of favorable depolarization factors allow for their better control. Among 2D materials, molybdenum disulfides and molybdenum oxides have recently received increased attention.1-5 The polariton propagation has also been recently shown in atomically smooth molybdenum oxides. For plasmonic propagatrions, tunable plasmon resonances in suspended 2D molybdenum oxide and molybdenum sulfide flakes are demonstrated. The 2D configuration generates a large depolarization factor and the presence of ultra-doping produces visible-light plasmon resonances. The ultra-doping process is conducted by reducing the semiconducting 2D molybdenum trioxide flakes using simulated solar irradiation. The generated plasmon resonances are controlled by the doping levels and the flakes’ lateral dimensions, as well as by exposure to model proteins and enzymes. It is also possible to reach ultradoping levels. Alternatively, by electrochemically intercalating lithium into 2D molybdenum disulfide nanoflakes, plasmon resonances in the visible and near UV wavelength ranges are achieved. These plasmon resonances are controlled by the high doping level of the nanoflakes after the intercalation, producing two distinct resonance peak areas based on the crystal arrangements. The system is also benchmarked for biosensing using bovine serum albumin. The talk will provide the foundation for developing future 2D molybdenum sulphide and oxide based biological and optical units. Polaronic propagation in full stoichiometric molybdenum oxides will also be discussed.6 References 1 Zhang, B. Y.; Zavabeti, A.; Chrimes, A. F.; Haque, F.; O'Dell, L. A.; Khan, H.; Syed, N.; Datta, R.; Wang, Y.; Chesman, A. S. R.; Daeneke, T.; Kalantar-zadeh, K.; Ou, J. Z.,. Advanced Functional Materials 2018, 28, 1706006. 2 Wang, Y.; Ou, J. Z.; Chrimes, A. F.; Carey, B. J.; Daeneke, T.; Alsaif, M. M. Y. A.; Mortazavi, M.; Zhuiykov, S.; Medhekar, N.; Bhaskaran, M.; Friend, J. R.; Strano, M. S.; Kalantar-Zadeh, K., Nano Letters 2015, 15, 883-890. 3 Ma, W.; Alonso-González, P.; Li, S.; Nikitin, A. Y.; Yuan, J.; Martín-Sánchez, J.; Taboada-Gutiérrez, J.; Amenabar, I.; Li, P.; Vélez, S.; Tollan, C.; Dai, Z.; Zhang, Y.; Sriram, S.; Kalantar-Zadeh, K.; Lee, S. T.; Hillenbrand, R.; Bao, Q., Nature 2018, 562, 557-562. 4 de Castro, I. A.; Datta, R. S.; Ou, J. Z.; Castellanos-Gomez, A.; Sriram, S.; Daeneke, T.; Kalantar-zadeh, K., Advanced Materials 2017, 29, 1701619. 5 Alsaif, M. M. Y. A.; Latham, K.; Field, M. R.; Yao, D. D.; Medhekar, N. V.; Beane, G. A.; Kaner, R. B.; Russo, S. P.; Ou, J. Z.; Kalantar-Zadeh, K., Advanced Materials 2014, 26, 3931-3937. 6 Ma W.; Alonso-González, P.; Li, S.; Nikitin, A.W.; Yuan, J.; Martín-Sánchez, J.; Taboada-Gutiérrez, J.; Amenabar, I.; Li, P., Vélez, S.; Tollan, C.; Dai, Z.; Zhang, Y.; Sriram, S.; Kalantar-Zadeh, K.; Lee. S-T., Hillenbrand, R.; Bao, Q. Nature 2018, 562, 557-562.

2D materials, especially their monolayers, have garnered significant attention due to their unique electrical, optical and mechanical properties. Strain engineering is an effective way to modulate these properties. However, challenges remain in preventing slip or decoupling between the 2D material and the substrate due to the inherent weak van der Waals interactions. In this study, metal films are employed to apply strain to 2D materials. The high surface energy of metals helps to provide higher interaction forces, thereby improving strain transfer efficiency. Biaxial compressive and uniaxial tensile strain can be applied to monolayer MoS2, with the highest modulation rate of 542 and 161.7 meV/%, respectively, as characterized by photoluminescence (PL) spectra. Furthermore, this new approach can be broader to other 2D materials, such as WS2 or WSe2, allowing for precise control over strain manipulation. The work introduces a promising new approach for efficient and controllable strain engineering of 2D materials.

The area of two-dimensional (2D) materials research would benefit greatly from the development of synthetically tunable van der Waals (vdW) materials. While the bottom-up synthesis of 2D frameworks from nanoscale building blocks holds great promise in this quest, there are many remaining hurdles, including the design of building blocks that reliably produce 2D lattices and the growth of macroscopic crystals that can be exfoliated to produce 2D materials. Here we report the regioselective synthesis of the cluster [trans-Co6Se8(CN)4(CO)2]3-/4-, a "superatomic" building block designed to polymerize and assemble into a 2D cyanometalate lattice whose surfaces are chemically addressable. The resulting vdW material, [Co(py)4]2[trans-Co6Se8(CN)4(CO)2], grows as bulk single crystals that can be mechanically exfoliated to produce flakes as thin as bilayers, with photolabile CO ligands on the exfoliated surface. As a proof of concept, we show that these surface CO ligands can be replaced by 4-isocyanoazobenzene under blue light irradiation. This work demonstrates that the bottom-up assembly of layered vdW materials from superatoms is a promising and versatile approach to create 2D materials with tunable physical and chemical properties.