Atomically thin two-dimensional (2D) metals may be key ingredients in next-generation quantum and optoelectronic devices. However, 2D metals must be stabilized against environmental degradation and integrated into heterostructure devices at the wafer scale. The high-energy interface between silicon carbide and epitaxial graphene provides an intriguing framework for stabilizing a diverse range of 2D metals. Here we demonstrate large-area, environmentally stable, epitaxial graphene/single-crystal 2D gallium, indium, and tin heterostructures. The 2D metals are covalently bonded to SiC below but present a non-bonded interface to graphene overlayer, i.e. they are "half van der Waals" metals with strong internal gradients in bonding character. These non-centrosymmetric 2D metals open compelling opportunities for superconducting devices, topological phenomena, and advanced optoelectronic properties. For example, the reported 2D-Ga is a superconductor that combines six strongly coupled Ga-derived electron pockets with a large nearly-freeelectron Fermi surface that closely approaches the Dirac points of the graphene overlayer.Major advances in fundamental science have followed from the exfoliation, stacking, and encapsulation of atomically thin 2D layers 1 . The next step towards technological impact of 2D layers and heterostructures is to transition sophisticated "pick and place" devices to a wafer-scale platform. However, the sensitivity of 2D systems to interfacial reactions and environmental influences -especially for two-dimensional metals or small-gap semiconductors -poses challenges for large-scale integration. Very few metals resist degradation of their top few atomic layers upon environmental exposure, and for a 2D metal, these layers constitute the entire system. A general platform for producing environmentally stable and wafer-scale 2D metals that are not prone to interfacial interactions would represent a significant advance. Inspired by the success of wide-bandgap 2D gallium nitride 2 , we turn focus onto the metal alone and demonstrate a platform dubbed confinement heteroepitaxy (CHet), where the interface between epitaxial graphene (EG) and silicon carbide (SiC) stabilizes crystalline 2D forms of Group-III (Ga, In) and group-IV (Sn) elements. Defect engineering of the graphene overlayer enables uniform, large-area intercalation at the high-energy SiC/EG interface; this interface then templates intercalant crystallization at a thermodynamically defined number of atomic layers. The unreactive nature of as-grown EG on SiC (graphene plus buffer layer) performs multiple services: (1) it only partially passivates the SiC surface underneath, thereby sustaining the high-energy interface that drives intercalation; (2) it lowers the energy of the (otherwise exposed) upper surface of the metal, thus facilitating 2D morphologies; (3) it protects the newly formed 2D metal from environmental degradation after intercalation through in situ healing of the graphene defects. Stability of these 2D metals in air over months gr...
There has been a considerable effort in the past decade to incorporate nitrogen into SiO2 in order to improve the electrical properties of ultrathin (2–10 nm) gate oxides. Process conditions affect the nitrogen concentration, coordination, and depth distribution which, in turn, affect the electrical properties. X-ray photoelectron spectroscopy (XPS) is particularly well suited to obtaining the nitrogen coordination and, to a lesser extent, the nitrogen concentration in thin oxynitride films. To date, at least four different nitrogen coordinations have been reported in the XPS literature, all having the general formula: N(–SixOyHz), where x+y+z=3 and x⩽3, y⩽1, z⩽2. In this article we review the XPS literature and report on a fifth nitrogen coordination, (O)2=N–Si, with a nitrogen 1s binding energy of 402.8±0.1 eV. Next nearest neighbor oxygen atoms shifted the N(–Si)3 peak roughly 0.1 eV per oxygen atom. We also discuss results from a novel approach of determining the nitrogen areal density by XPS, the accuracy of which is dependent on the depth distribution of nitrogen. Secondary ion mass spectrometry is used to determine the depth N distribution, while nuclear reaction analysis is used to check the N concentration measured by XPS.
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