Stretchable and Highly Bendable Thin Film Transistors Based on Atomically Thin Chemical Vapor Deposited Molybdenum Disulfide

Two-dimensional (2D) materials have received tremendous research attention recently, as they possess peculiar physical properties in their monolayer and few-layer forms, which further lead to novel applications. A wide range of 2D materials covers insulators, metals, superconductors and semiconductors with various bandgap, giving a fresh platform to reinvent conventional electronic and optoelectronic devices with new advantages. Molybdenum disulfide (MoS2), belonging to the group of transition metal dichalcogenides (TMDCs), has been widely studied for its particular physical properties and potential applications as a leading example among 2D semiconductors. In this thesis, we focus on the applications ofMoS2 in microelectronic and micro-electromechanical devices. The MoS2 we studied is grown specifically by chemical vapor deposition, which offers the highest potential in large area growth. Utilizing the flexible nature such as high in-plane fracture strain and low bending stiffness of atomically thinMoS2, we developed stretchable thin film transistors (TFTs) on polydimethylsiloxane (PDMS) and highly bendable thin film transistors on polyimide. The fabrication process is ameliorated and designed to provide good chemical and temperature compatibility to the polymer substrates. Electrical performance of the flexible devices under different degrees of bending and stretching has been studied. The stretchableMoS2 TFTs could sustain up to 4% of uniaxial tensile strain maintaining device function, and the failure occurs at 5% of strain due to the fracture in gate dielectric layer. The highly bendableMoS2 TFTs with parylene-C gate dielectric layer exhibit tolerance to the smallest bending radius of 0.625 mm. Different encapsulation layers such as HfO2, Cytop and SU8 have been implemented on the bendable devices to improve the performance represented by the increase in field effect mobility, reduction in hysteresis and better endurance to mechanical deformation. The resulting flexibleMoS2 TFTs show field effect mobility of 21.4 cm^2V^-1s^-1 and a large on-off ratio of 106 in air. The SU8 encapsulation layer is further demonstrated as controllable n-type doping strategy with low temperature process, which is ideal for flexible MoS2 devices as it additionally exhibits good stability in air and water.

Charge-transport properties of monolayer MoS2 at the interface with dielectric materials

Simone Bertolazzi

Two-dimensional (2D) semiconductors, consisting of single-sheets of layered transition metal dichalcogenides (TMD), are attracting enormous interest from both fundamental science and technology. Monolayer molybdenum disulfide (MoS2), a typical example from this class of materials, is currently under intense research investigation because its direct band gap, atomic-scale thickness and mechanical flexibility could enable a wide range of novel technological applications, such as low-power flexible/transparent electronics, displays and wearable sensors. Critical to all these applications are the material mechanical strength, the mobility of charge-carriers in the 2D semiconductor and its interaction with the surrounding environment. This thesis describes experimental research conducted on these critical aspects and shows a proof-of-concept device application based on heterostructures of MoS2 and graphene. The main goal of the research was to assess experimentally the potential of monolayer MoS2 for application in flexible electronics. The thesis is based on three papers. The first paper describes the measurements of the in-plane stiffness and breaking strength of free-standing membranes of monolayer MoS2. Nanoindentation experiments were performed with the tip of an atomic force microscope (AFM) to extract the material's Young's modulus (E ~ 270 GPa) and breaking strength (Ïmax ~ 23 GPa). Breaking occurred at maximum internal strain Îµint ~ 11%, which indicates that monolayer MoS2 is suitable for integration on flexible plastic substrates. The second paper represents the core work of this thesis. It explores the charge transport properties of monolayer MoS2 supported by different dielectric substrates, such as thin polymer films of parylene, atomically flat sapphire and 2D sheets of hexagonal boron nitride (h-BN). It was found that substrate surface corrugations do not represent a major limit to charge-carrier mobility in monolayer MoS2, which seems at this stage dominated by impurities and material's defects. Field-effect transistors with mobility ~ 100 cm2/Vs and on/off current ratio Ion/Ioff > 10^5 were successfully integrated on parylene substrates, whose root-mean-square roughness Rq can be more than two times larger than the thickness of the transistor channel itself. Because parylene is also a flexible material, this work showed a viable method for the realization of high-mobility and high performance flexible devices based on 2D semiconductors. Finally, the third paper describes a flash-memory cell fabricated using monolayer MoS2/graphene heterostructures and dielectric layers of HfO2 grown by atomic layer deposition (ALD). The architecture of the device resembles that of a floating-gate transistor. Monolayer MoS2 acts as the transistor channel, graphene electrodes are used to collect and inject the charge carriers, and a piece of multilayer graphene serves as ultrathin charge trapping layer. In this paper, it was shown that graphene contacts to monolayer MoS2 result in ohmic-like current-voltage characteristics at room temperature. Moreover, the use of graphene and 2D semiconductors in flash memory technology was indicated as a potential strategy for further scaling of memory cells and for their integration in flexible electronic devices.

EPFL2015

Spin-valley optoelectronics based on two-dimensional materials

Dmitrii Unuchek

Two-dimensional (2D) materials, in particular graphene and transition metal dichalcogenides (TMDC), have attracted great scientific interest over the last decade, revealing exceptional mechanical, electrical and optical properties. Owing to their layered nature, subnanometer-thick single-layer forms of these crystals can be chemically grown or mechanically isolated, representing an ultimately scaled-down platform for further miniaturization of electronic devices. Indeed, the large family of 2D materials contains hundreds of members, including metals, semiconductors, insulators, and others, covering the whole spectrum of potential applications. Availability of all necessary building blocks for the construction of all-2D solid-state devices makes this platform ideal for fabrication of ultrathin, transparent and flexible devices. Extensively investigated graphene has demonstrated excellent electrical properties. However, the absence of a bandgap is an obstacle for its interaction with light and therefore limits applications in optics. In this aspect, atomically thin TMDC semiconductors appear to be an alternative, more promising platform, as they possess a direct band gap in the visible range in the monolayer form. Despite being only three atoms thick, these semiconductors demonstrate exceptionally large light absorption, efficient light emission, and strong light-matter interaction, attracting justified interest from the optics community. We will focus on their potential applications for optoelectronics in Chapter 4. Even more, broken inversion symmetry and strong spin-orbit coupling in single-layer TMDC crystals reveal a new quantum number, the so-called valley index. Indeed, this unique degree of freedom of charge carriers is known for some materials since the 1970s. However, in the case of 2D semiconductors, spin-valley locking mechanism and valley contrasting optical selection rules open new ways for addressing, manipulation and sensing of this pseudospin, opening the whole new field of valleytronics. Due to the large splitting of the valence band, spin and valley degree of freedom become locked in these atomically thin materials. We employ this unique feature in Chapter 5 for indirect injection of spins into graphene by pumping valley polarized carriers in an adjacent TMDC monolayer. Being gapless, graphene does not allow direct optical injection of spins. Another striking feature of 2D materials is their unique ability to be stacked in vertical heterostructures with strong electrical coupling between layers. The weak van der Waals force, which keeps components together, provides freedom in the assembly process, so that a lattice mismatch or a twist angle becomes unimportant in the first approximation. This provides a novel platform for harvesting complementary properties of the constituent materials, allowing the engineering of new artificial meta-materials as we demonstrate in Chapter 6. Furthermore, synergistic effects in van der Waals heterostructures enable completely new properties and phenomena, which do not exist in the single materials, with twist angle being an important knob for tuning these effects. We observe and exploit such novel phenomena arising in heterostructures of 2D semiconductors in the last chapter of this thesis. On the way to the realization of practical optoelectronic and valleytronic applications, this thesis studies fundamental aspects of rich spin-valley physics of atomically thin semiconductors

EPFL2019

Single-Layer MoS2 Electronics

Simone Bertolazzi, Andras Kis, Dominik Sebastian Lembke

CONSPECTUS: Atomic crystals of two-dimensional materials consisting of single sheets extracted from layered materials are gaining increasing attention. The most well-known material from this group is graphene, a single layer of graphite that can be extracted from the bulk material or grown on a suitable substrate. Its discovery has given rise to intense research effort culminating in the 2010 Nobel Prize in physics awarded to Andre Geim and Konstantin Novoselov. Graphene however represents only the proverbial tip of the iceberg, and increasing attention of researchers is now turning towards the veritable zoo of so-called "other 2D materials". They have properties complementary to graphene, which in its pristine form lacks a bandgap: MoS2, for example, is a semiconductor, while NbSe2 is a superconductor. They could hold the key to important practical applications and new scientific discoveries in the two-dimensional limit. This family of materials has been studied since the 1960s, but most of the research focused on their tribological applications: MoS2 is best known today as a high-performance dry lubricant for ultrahigh-vacuum applications and in car engines. The realization that single layers of MoS2 and related materials could also be used in functional electronic devices where they could offer advantages compared with silicon or graphene created a renewed interest in these materials. MoS2 is currently gaining the most attention because the material is easily available in the form of a mineral, molybdenite, but other 2D transition metal dichalcogenide (TMD) semiconductors are expected to have qualitatively similar properties.In this Account, we describe recent progress in the area of single-layer MoS2-based devices for electronic circuits. We will start with MoS2 transistors, which showed for the first time that devices based on MoS2 and related TMDs could have electrical properties on the same level as other, more established semiconducting materials. This allowed rapid progress in this area and was followed by demonstrations of basic digital circuits and transistors operating in the technologically relevant gigahertz range of frequencies, showing that the mobility of MoS2 and TMD materials is sufficiently high to allow device operation at such high frequencies.Monolayer MoS2 and other TMDs are also direct band gap semiconductors making them interesting for realizing optoelectronic devices. These range from simple phototransistors showing high sensitivity and low noise, to light emitting diodes and solar cells. All the electronic and optoelectronic properties of MoS2 and TMDs are accompanied by interesting mechanical properties with monolayer MoS2 being as stiff as steel and 30x stronger. This makes it especially interesting in the context of flexible electronics where it could combine the high degree of mechanical flexibility commonly associated with organic semiconductors with high levels of electrical performance. All these results show that MoS2 and TMDs are promising materials for electronic and optoelectronic applications.

2015