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Large scale self-assembly of plasmonic nanoparticles on deformed graphene templates

AbstractHierarchical heterostructures of two-dimensional (2D) nanomaterials are versatile platforms for nanoscale optoelectronics. Further coupling of these 2D materials with plasmonic nanostructures, especially in non-close-packed morphologies, imparts new metastructural properties such as increased photosensitivity as well as spectral selectivity and range. However, the integration of plasmonic nanoparticles with 2D materials has largely been limited to lithographic patterning and/or undefined deposition of metallic structures. Here we show that colloidally synthesized zero-dimensional (0D) gold nanoparticles of various sizes can be deterministically self-assembled in highly-ordered, anisotropic, non-close-packed, multi-scale morphologies with templates designed from instability-driven, deformed 2D nanomaterials. The anisotropic plasmonic coupling of the particle arrays exhibits emergent polarization-dependent absorbance in the visible to near-IR regions. Additionally, controllable metasurface arrays of nanoparticles by functionalization with varying polymer brushes modulate the plasmonic coupling between polarization dependent and independent assemblies. This self-assembly method shows potential for bottom-up nanomanufacturing of diverse optoelectronic components and can potentially be adapted to a wide array of nanoscale 0D, 1D, and 2D materials.
Publications

High-Volume Production of Repeatable High Enhancement SERS Substrates Using Solid-State Superionic Stamping

Abstract Surface-enhanced Raman spectroscopy (SERS) is emerging as a powerful tool for detecting and identifying chemical and biological substances because of its high sensitivity, specificity, speed, and label-free detection. For SERS substrates to be effective in sensing applications, they must exhibit reproducible and robust high signal enhancement and cost-effective scalability. This article introduces a highly sensitive, large-area silver SERS substrate patterned with a uniform array of 3D retroreflecting inverted pyramids and develops a manufacturing pathway for it, using a novel and facile electrochemical imprinting process called solid-state superionic stamping (S4). Substrates, approximately 4 mm2 in area, are produced and tested with 1,2-bis(4-pyridyl) ethylene (BPE). Uniformly high and reproducible spatially averaged enhancement factor (EF), typically around a value of 2 × 107 with a relative standard deviation of 6.7% and a high batch-to-batch repeatability with a relative standard deviation of 10.5% between batches were observed. Passivating a substrate's surface with atomically thin layers of alumina, deposited using atomic layer deposition (ALD) was effective in maintaining the EF constant over a 60-day period, albeit with a trade-off between its EF and its lifespan. S4 has the potential to make substrates with EF consistently greater than 107 available at a cost of $1 to $2 per substrate, allowing SERS to be adopted across a wide spectrum of high-volume applications, including security, food safety, medical diagnostics, and chem-bio analysis.
Publications

Evidence of pseudogravitational distortions of the Fermi surface geometry in the antiferromagnetic metal FeRh

AbstractThe confluence between high-energy physics and condensed matter has produced groundbreaking results via unexpected connections between the two traditionally disparate areas. In this work, we elucidate additional connectivity between high-energy and condensed matter physics by examining the interplay between spin-orbit interactions and local symmetry-breaking magnetic order in the magnetotransport of thin-film magnetic semimetal FeRh. We show that the change in sign of the normalized longitudinal magnetoresistance observed as a function of increasing in-plane magnetic field results from changes in the Fermi surface morphology. We demonstrate that the geometric distortions in the Fermi surface morphology are more clearly understood via the presence of pseudogravitational fields in the low-energy theory. The pseudogravitational connection provides additional insights into the origins of a ubiquitous phenomenon observed in many common magnetic materials and points to an alternative methodology for understanding phenomena in locally-ordered materials with strong spin-orbit interactions.
Publications

Achieving sub-0.5-angstrom–resolution ptychography in an uncorrected electron microscope

Subangstrom resolution has long been limited to aberration-corrected electron microscopy, where it is a powerful tool for understanding the atomic structure and properties of matter. Here, we demonstrate electron ptychography in an uncorrected scanning transmission electron microscope (STEM) with deep subangstrom spatial resolution down to 0.44 angstroms, exceeding the conventional resolution of aberration-corrected tools and rivaling their highest ptychographic resolutions​. Our approach, which we demonstrate on twisted two-dimensional materials in a widely available commercial microscope, far surpasses prior ptychographic resolutions (1 to 5 angstroms) of uncorrected STEMs. We further show how geometric aberrations can create optimized, structured beams for dose-efficient electron ptychography. Our results demonstrate that expensive aberration correctors are no longer required for deep subangstrom resolution.
Publications

Dynamic and weak electric double layers in ultrathin nanopores

The unique properties of aqueous electrolytes in ultrathin nanopores have drawn a great deal of attention in a variety of applications, such as power generation, water desalination, and disease diagnosis. Inside the nanopore, at the interface, properties of ions differ from those predicted by the classical ionic layering models (e.g., Gouy–Chapman electric double layer) when the thickness of the nanopore approaches the size of a single atom (e.g., nanopores in a single-layer graphene membrane). Here, using extensive molecular dynamics simulations, the structure and dynamics of aqueous ions inside nanopores are studied for different thicknesses, diameters, and surface charge densities of carbon-based nanopores [ultrathin graphene and finite-thickness carbon nanotubes (CNTs)]. The ion concentration and diffusion coefficient in ultrathin nanopores show no indication of the formation of a Stern layer (an immobile counter-ionic layer) as the counter-ions and nanopore atoms are weakly correlated in time compared to the strong correlation observed in thick nanopores. The weak correlation observed in ultrathin nanopores is indicative of a weak adsorption of counter-ions onto the surface compared to that of thick pores. The vanishing counter-ion adsorption (ion–wall correlation) in ultrathin nanopores leads to several orders of magnitude shorter ionic residence times (picoseconds) compared to the residence times in thick CNTs (seconds). The results of this study will help better understand the structure and dynamics of aqueous ions in ultrathin nanopores.

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