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Abstract Owing to its superlative carrier mobility and atomic thinness, graphene exhibits great promise for interconnects in future nanoelectronic integrated circuits. Chemical vapor deposition (CVD), the most popular method for wafer-scale growth of graphene, produces monolayers that are polycrystalline, where misoriented grains are separated by extended grain boundaries (GBs). Theoretical models of GB resistivity focused on small sections of an extended GB, assuming it to be a straight line, and predicted a strong dependence of resistivity on misorientation angle. In contrast, measurements produced values in a much narrower range and without a pronounced angle dependence. Here we study electron transport across rough GBs, which are composed of short straight segments connected together into an extended GB. We found that, due to the zig-zag nature of rough GBs, there always exist a few segments that divide the crystallographic angle between two grains symmetrically and provide a highly conductive path for the current to flow across the GBs. The presence of highly conductive segments produces resistivity between 10 2 to 10 4 Ω μ m regardless of misorientation angle. An extended GB with large roughness and small correlation length has small resistivity on the order of 10 3 Ω μ m, evenmore »
Grain‐Boundary‐Rich Noble Metal Nanoparticle Assemblies: Synthesis, Characterization, and Reactivity
Here, a comprehensive study on the synthesis, characterization, and reactivity of grain‐boundary (GB)‐rich noble metal nanoparticle (NP) assemblies is presented. A facile and scalable synthesis of Pt, Pd, Au, Ag, and Rh NP assemblies is developed, in which NPs are predominantly connected via Σ3 (111) twin GBs, forming a network. Driven by water electrolysis, the random collisions and oriented attachment of colloidal NPs in solution lead to the formation of Σ3 (111) twin boundaries and some highly mismatched GBs. This synthetic method also provides convenient control over the GB density without altering the crystallite size or GB type by varying the NP collision frequency. The structural characterization reveals the presence of localized tensile strain at the GB sites. The ultrahigh activity of GB‐rich Pt NP assembly toward catalytic hydrogen oxidation in air is demonstrated, enabling room‐temperature catalytic hydrogen sensing for the first time. Finally, density functional theory calculations reveal that the strained Σ3(111) twin boundary facilitates oxygen dissociation, drastically enhancing the hydrogen oxidation rate via the dissociative pathway. This reported large‐scale synthesis of the Σ3 (111) twin GB‐rich structures enables the development of a broad range of high‐performance GB‐rich catalysts.
The interaction of alloying elements with grain boundaries (GBs) influences many phenomena, such as microstructural evolution and transport. While GB solute segregation has been the subject of active research in recent years, most studies focus on ground-state GB structures, i.e., lowest energy GBs. The impact of GB metastability on solute segregation remains poorly understood. Herein, we leverage atomistic simulations to generate metastable structures for a series of  and  symmetric tilt GBs in a model Al–Mg system and quantify Mg segregation to individual sites within these boundaries. Our results show large variations in the atomic Voronoi volume due to GB metastability, which are found to influence the segregation energy. The atomistic data are then used to train a Gaussian Process machine learning model, which provides a probabilistic description of the GB segregation energy in terms of the local atomic environment. In broad terms, our approach extends existing GB segregation models by accounting for variability due to GB metastability, where the segregation energy is treated as a distribution rather than a single-valued quantity.
To understand the mechanism underlying the fast, reversible, phase transformation, information about the atomic structure and defects structures in phase change materials class is key. PCMs are investigated for many applications. These devices are chalcogenide based and use self heating to quickly switch between amorphous and crystalline phases, generating orders of magnitude differences in the electrical resistivity. The main challenges with PCMs have been the large power required to heat above crystallization or melting (for melt-quench amorphization) temperatures and limited reliability due to factors such as resistance drifts of the metastable phases, void formation and elemental segregation upon cycling. Characterization of devices and their unique switching behavior result in distinct material properties affected by the atomic arrangement in the respective phase. TEM is used to study the atomic structure of the metastable crystalline phase. The aim is to correlate the microstructure with results from electrical characterization, building on R vs T measurements on various thicknesses GST thin films. To monitor phase changes in real-time as a function of temperature, thin films are deposited directly onto Protochips carriers. The Protochips heating holders provides controlled temperature changes while imaging in the TEM. These studies can provide insights into how changes occur inmore »
Synthesis and Characterization of Free-Stand Graphene/Silver Nanowire/Graphene Nano Composite as Transparent Conductive Film with Enhanced StiffnessAs-grown graphene via chemical vapor deposition (CVD) has potential defects, cracks, and disordered grain boundaries induced by the synthesis and transfer process. Graphene/silver nanowire/graphene (Gr/AgNW/Gr) sandwich composite has been proposed to overcome these drawbacks significantly as the AgNW network can provide extra connections on graphene layers to enhance the stiffness and electrical conductivity. However, the existing substrate (polyethylene terephthalate (PET), glass, silicon, and so on) for composite production limits its application and mechanics behavior study. In this work, a vacuum annealing method is proposed and validated to synthesize the free-stand Gr/AgNW/Gr nanocomposite film on transmission electron microscopy (TEM) grids. AgNW average spacing, optical transmittance, and electrical conductivity are characterized and correlated with different AgNW concentrations. Atomic force microscope (AFM) indentation on the free-stand composite indicates that the AgNW network can increase the composite film stiffness by approximately 460% with the AgNW concentration higher than 0.6 mg/mL. Raman spectroscopy shows the existence of a graphene layer and the disturbance of the AgNW network. The proposed method provides a robust way to synthesize free-stand Gr/AgNW/Gr nanocomposite and the characterization results can be utilized to optimize the nanocomposite design for future applications.