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No description available.

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Slippery liquid-infused porous surfaces (SLIPS) – a new class of bio-inspired liquid-repellent surfaces – comprise arbitrarily porous architectures filled with oils that exhibit high interfacial tensions to probe liquids and present ultralow contact angle hysteresis (<〖10〗^°). However, before practical technologies based on SLIPS can be designed at large-scale, a number of fundamental questions remain to be answered. For instance, depending on the sign of the spreading coefficient of the Vapor(V)-lubricant oil(O)-liquid(L) system, defined as S_(OL(V))=γ_LV-γ_LO-γ_OV>0, the lubricating layer forms a layer at the liquid-vapor interface (here, γ_LV is a liquid-vapor interfacial tension, γ_LO – liquid-oil, and γ_OV – oil-vapor). This “cloaking” of liquid drops can deplete SLIPS’ lubricant over time and contaminate the probed liquid. So far, cloaking has been investigated by contact angle goniometry and confocal microscopy, which cannot resolve films of molecular thickness and factors that govern the equilibrium thickness of those films are not entirely clear. Here, we report on the development and application of a reflective-mode SFA platform to characterize the cloaking of water droplets placed on SLIPS. A multilayer matrix method is utilized to analyze the interferometry data. Using this complementary experimental and analytical approach, we determined the thickness of the cloaking layer for the FDTS(solid)-VF-40(lubricant)-water(probe liquid)-air system to be z3= 7±1 nm. Towards deeper insights into the intermolecular and surface forces responsible for cloaking, we demonstrate that repulsive van der Waals interactions are responsible for stabilizing the cloaking film at the water-air interface. Our experimental platform and the analytical framework should facilitate investigations of other SLIPS and probe liquid systems down to the molecular-scale resolution. These findings might aid the rational design of SLIPS, e.g., for drag reduction, anti-biofouling, and anti-corrosion. In addition to investigating SLIPS, We addressed the following questions with the help of atomic force microscopy (AFM): (i) how do zwitterionic osmolytes modulate electrostatic and hydrophobic interactions in nanoscale confinement, and (ii) is it possible to have two negatively charged surfaces attract each other? Our findings are presented as appendices in this thesis.

The family of semiconducting 2H-phase group-VI transition metal dichalcogenides (TMDs) have been suggested to be promising candidates for hosting optically accessible spin qubits due to their desirable optical and electrical properties, however, experimental progress towards this goal has been impeded by the difficulties associated with the fabrication of clean structures with quality contacts. In this thesis, we present the complex process for obtaining functional contacts to two particular TMDs, molybdenum disulfide (MoS2) and tungsten diselenide (WSe2), from which we use as the foundation for the fabrication of three important gate defined quantum structures: quantum dots, a charge detector, and a long 1D channel. These structures all play an important role in furthering the understanding of these materials and are the building blocks for achieving functional spin qubits. More precisely, we investigate the contact resistances associated with various cleaning procedures and contact architectures and report a recipe that results in an ultra-low contact resistance even at cryogenic temperatures. We then demonstrate electrical control of hole quantum dots, the host of the spin qubit, in gated heterostructure devices based on monolayer WSe2 and study its properties. With a similar structure, we demonstrate that a gate-defined nano-constriction is sensitive to the charge occupation of a nearby quantum dot and is therefore suitable to be used as a charge sensor, a valuable component of elaborate quantum circuits. Finally, we demonstrate the realization of a gate-defined quantum confined 1D channel in a high mobility monolayer WSe2 sample and observe an anomalous conductance quantization in units of e2/h. These results pave the way for the development of quantum devices based on electrostatically confined quantum dots defined in semiconducting TMDs and push forward our understanding of their electronic properties.

The exploration of physical extremes drives technological innovation. Recent decades have seen a push towards materials engineering at the absolute limit of space with electronic systems that are a single atom thick. When electrons are confined to two-dimensional structures, exotic and often unexpected phenomena emerge due to enhanced interaction effects and crystalline anisotropies. The study of such unconventional phenomena offers the opportunity to extend knowledge of fundamental physics with an eye towards advancing the state of the art in control over quantum matter. In this thesis we use scanning tunneling microscopy to study the electronic structure of a collection of novel two-dimensional materials: twisted double-bilayer graphene (TDBG), mirror symmetric twisted trilayer graphene (TTG), small angle twisted double trilayer graphene (TDTG), and the van der Waals heavy Fermion material CeSiI. In TDBG, we directly image spontaneous symmetry breaking of the electronic states as a function of carrier density and attribute this to an intrinsic nematic instability of the metallic Fermi liquid. In TTG, we find evidence for a novel form of lattice relaxation, in which twist angle disorder leads to the formation of moiré lattice defects that can act to lock trilayer devices into a magic angle configuration while strongly modulating the local electronic structure, with implications for the superconducting state. In TDTG, we discover yet another form of lattice relaxation in which a global transformation of the stacking structure creates a net energy reduction, even while the stacking energy density in roughly half of the moiré lattice rises. Lastly, we show through quasiparticle interference spectroscopy and theoretical modeling that CeSiI hosts a nodal hybridization between itinerant conduction electrons and a lattice of local moments, giving rise to a strong angular dependence of the heavy Fermion mass enhancement in this van der Waals material.

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Quantum computing and two dimensional van der Waals materials research have been two of the fastest growing fields of condensed matter physics research for the better part of the last two decades. In that time, advances in superconducting qubit design, materials and fabrication have improved their relaxation and coherence times by about 5 orders of magnitude. One of the key components that quantum devices such as qubits require are ultra low loss capacitance elements. Conventional parallel plate capacitors have been unable to fulfill this need due to bulk and inter-facial losses, necessitating the use of coplanar capacitors with extremely large footprints. In fact one of the driving forces behind increase coherence times has been the ever growing footprint of these coplanar capacitor pads, and the reduced electric field density and thus reduced surface losses that they provide. However, this style of capacitor creates a number of challenges when it comes to scaling the number of qubits in a system. First, the large geometric footprint of these pads limits the number of qubits that can be placed on a chip. Second, the dispersion of the electric field, above and below the plane of the capacitor pads can cause unwanted crosstalk between neighbouring qubits, again limiting the number of qubits that can be put on a chip without compromising coherence. Since the isolation of a single atomic layer of graphene in 2004 and the ability to create heterostructures of a variety of two dimensional materials, the field of van der Waals materials research has exploded at a similar rate. Single crystals of van der Waals materials, can be grown with extremely low defect densities, and then be stacked to create heterostructures with ultra-clean laminated interfaces. This work explores how van der Waals materials may be used to create low loss parallel plate capacitors. The parallel plate geometry confines the electric field between the crystalline materials and low loss interfaces of a van der Waals heterostructure, limiting both losses at the surfaces as well as undesired cross talk between qubits. We begin by studying the microwave losses in hexagonal boron nitride (hBN). Next we report a method to make low loss microwave contacts to air sensitive superconducting van der Waals materials like niobium diselinde (NbSe₂). Finally, we demostrate coherence in a transmon where the primary shunt capacitor is an all van der Waals parallel plate capacitor, achieving a 1000× reduction in geometric footprint, when compared to a conventional coplanar capacitor.