Engineered Two-Dimensional Nanomaterials for Advanced Opto-electronic Applications

Two dimensional (2D) materials have unique properties that make them exciting candidates for various optical and electronic applications. Materials such as graphene and transition metal dichalcogenides (TMDCs) have been intensively studied recently with researchers racing to show advances in 2D device performance while developing a better understanding of the material properties. Despite recent advances,there are still significant roadblocks facing the use of 2D materials for real-world applications. The ability to make reliable, low-resistance electrical contact to TMDCs such as molybdeum disulfide (MoS22) has been a challenge that many researchers have sought to overcome with novel solutions. The work laid out in this dissertation uses novel techniques for addressing these issues through the use of improved device fabrication and with a clean, and potentially scalable doping method to tune 2D material properties.A high-performance field-effect transistor (FET) was fabricated using a new device platform that combined graphene leads with dielectric encapsulation leading to the highest reported value for electron mobility in MoS2. Device fabrication techniques were also investigated and a new, commercially available lithography tool (NanoFrazor) was used to pattern contacts directly onto monolayer MoS2. Through a series of control experiments with conventional lithography, a clear improvement in contact resistance was observed with the use of the NanoFrazor. Plasma-doping, a dry and clean process, was investigated as an alternative to traditional wet-chemistry doping techniques. In addition to developing doping parameters with a chlorine plasma treatment of graphene, a series of experiments on doped graphene were conducted to study its effect on optical properties. Whereas previous studies used electrostatic gating to modify graphene’s optical properties, this work with plasma-doped graphene showed the ability to tune absorbence and plasmon wavelength without the need for an applied bias opening the door to the potential for low-power applications. This work is a just small contribution to the larger body of research in this field but hopefully represents a meaningful step towards a greater understanding of 2D materials and the realization of functional applications

Heterostructures based on inorganic and organic van der Waals systems

The two-dimensional limit of layered materials has recently been realized through the use of van der Waals (vdW) heterostructures composed of weakly interacting layers. In this paper, we describe two different classes of vdW heterostructures: inorganic vdW heterostructures prepared by co-lamination and restacking; and organicinorganic hetero-epitaxy created by physical vapor deposition of organic molecule crystals on an inorganic vdW substrate. Both types of heterostructures exhibit atomically clean vdW interfaces. Employing such vdW heterostructures, we have demonstrated various novel devices, including graphene/hexagonal boron nitride (hBN) and MoS2 heterostructures for memory devices; graphene/MoS2/WSe2/graphene vertical p-n junctions for photovoltaic devices, and organic crystals on hBN with graphene electrodes for high-performance transistorsPhysic

Atomically thin p–n junctions with van der Waals heterointerfaces

Semiconductor p–n junctions are essential building blocks for electronic and optoelectronic devices. In conventional p–n junctions, regions depleted of free charge carriers form on either side of the junction, generating built-in potentials associated with uncompensated dopant atoms. Carrier transport across the junction occurs by diffusion and drift processes influenced by the spatial extent of this depletion region. With the advent of atomically thin van der Waals materials and their heterostructures, it is now possible to realize a p–n junction at the ultimate thickness limit3, 4, 5, 6, 7, 8, 9, 10. Van der Waals junctions composed of p- and n-type semiconductors—each just one unit cell thick—are predicted to exhibit completely different charge transport characteristics than bulk heterojunctions10, 11, 12. Here, we report the characterization of the electronic and optoelectronic properties of atomically thin p–n heterojunctions fabricated using van der Waals assembly of transition-metal dichalcogenides. We observe gate-tunable diode-like current rectification and a photovoltaic response across the p–n interface. We find that the tunnelling-assisted interlayer recombination of the majority carriers is responsible for the tunability of the electronic and optoelectronic processes. Sandwiching an atomic p–n junction between graphene layers enhances the collection of the photoexcited carriers. The atomically scaled van der Waals p–n heterostructures presented here constitute the ultimate functional unit for nanoscale electronic and optoelectronic devices.Physic

Coulomb engineering of the bandgap and excitons in two-dimensional materials

The ability to control the size of the electronic bandgap is an integral part of solid-state technology. Atomically thin two-dimensional crystals offer a new approach for tuning the energies of the electronic states based on the unusual strength of the Coulomb interaction in these materials and its environmental sensitivity. Here, we show that by engineering the surrounding dielectric environment, one can tune the electronic bandgap and the exciton binding energy in monolayers of WS2 and WSe2 by hundreds of meV. We exploit this behaviour to present an in-plane dielectric heterostructure with a spatially dependent bandgap, as an initial step towards the creation of diverse lateral junctions with nanoscale resolution

Multi-terminal transport measurements of MoS2 using a van der Waals heterostructure device platform

Atomically thin two-dimensional semiconductors such as MoS2 hold great promise in electrical, optical, and mechanical devices and display novel physical phenomena. However, the electron mobility of mono- and few-layer MoS2 has so far been substantially below theoretically predicted limits, which has hampered efforts to observe its intrinsic quantum transport behaviours. Potential sources of disorder and scattering include both defects such as sulfur vacancies in the MoS2 itself, and extrinsic sources such as charged impurities and remote optical phonons from oxide dielectrics. To reduce extrinsic scattering, here we developed a van der Waals heterostructure device platform where MoS2 layers are fully encapsulated within hexagonal boron nitride, and electrically contacted in a multi-terminal geometry using gate-tunable graphene electrodes. Magneto-transport measurements show dramatic improvements in performance, including a record-high Hall mobility reaching 34,000 cm2/Vs for 6-layer MoS2 at low temperature, confirming that low-temperature performance in previous studies was limited by extrinsic interfacial impurities rather than bulk defects in the MoS2. We also observed Shubnikov-de Haas oscillations for the first time in high-mobility monolayer and few-layer MoS2. Modeling of potential scattering sources and quantum lifetime analysis indicate that a combination of short-ranged and long-ranged interfacial scattering limits low-temperature mobility of MoS2.Physic

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