Cryogenic Scanning/Transmission Electron Microscopy has been established as a leading method to image sensitive biological samples and is now becoming a powerful tool to understand materials' behavior at low temperatures. However, achieving precise local temperature calibration at low temperatures remains a challenge, which is especially crucial for studying phase transitions and emergent physical properties in quantum materials. In this study, we employ electron energy loss spectroscopy (EELS) to measure local cryogenic specimen temperatures.
View Article and Find Full Text PDFIt is widely accepted that the interaction of swift heavy ions with many complex oxides is predominantly governed by the electronic energy loss that gives rise to nanoscale amorphous ion tracks along the penetration direction. The question of how electronic excitation and electron-phonon coupling affect the atomic system through defect production, recrystallization, and strain effects has not yet been fully clarified. To advance the knowledge of the atomic structure of ion tracks, we irradiated single crystalline SrTiO with 629 MeV Xe ions and performed comprehensive electron microscopy investigations complemented by molecular dynamics simulations.
View Article and Find Full Text PDFBecause of their large surface areas, nanotubes and nanowires demonstrate exquisite mechanical coupling to their surroundings, promising advanced sensors and nanomechanical devices. However, this environmental sensitivity has resulted in several ambiguous observations of vibrational coupling across various experiments. Herein, we demonstrate a temperature-dependent Radial Breathing Mode (RBM) frequency in free-standing, electron-diffraction-assigned Double-Walled Carbon Nanotubes (DWNTs) that shows an unexpected and thermally reversible frequency downshift of 10 to 15%, for systems isolated in vacuum.
View Article and Find Full Text PDFNarrow gaps between plasmon-supporting materials can confine infrared electromagnetic energy at the nanoscale, thus enabling applications in areas such as optical sensing. However, in nanoparticle dimers, the nature of the transition between touching (zero gap) and nearly nontouching (nonzero gap ≲15 nm) regimes is still a subject of debate. Here, we observe both singular and nonsingular transitions in infrared plasmons confined to dimers of fluorine-doped indium oxide nanocubes when moving from touching to nontouching configurations depending on the dimensionality of the contact region.
View Article and Find Full Text PDFIn heterostructures made from polar materials, e.g., AlN-GaN-AlN, the nonequivalence of the two interfaces is long recognized as a critical aspect of their electronic properties; in that, they host different 2D carrier gases.
View Article and Find Full Text PDFIt is shown that structural disorder-in the form of anisotropic, picoscale atomic displacements-modulates the refractive index tensor and results in the giant optical anisotropy observed in BaTiS, a quasi-1D hexagonal chalcogenide. Single-crystal X-ray diffraction studies reveal the presence of antipolar displacements of Ti atoms within adjacent TiS chains along the c-axis, and threefold degenerate Ti displacements in the a-b plane. Ti solid-state NMR provides additional evidence for those Ti displacements in the form of a three-horned NMR lineshape resulting from a low symmetry local environment around Ti atoms.
View Article and Find Full Text PDFIsotope effects have received increasing attention in materials science and engineering because altering isotopes directly affects phonons, which can affect both thermal properties and optoelectronic properties of conventional semiconductors. However, how isotopic mass affects the optoelectronic properties in 2D semiconductors remains unclear because of measurement uncertainties resulting from sample heterogeneities. Here, we report an anomalous optical bandgap energy red shift of 13 (±7) milli-electron volts as mass of Mo isotopes is increased in laterally structured MoS-MoS monolayers grown by a two-step chemical vapor deposition that mitigates the effects of heterogeneities.
View Article and Find Full Text PDFAmorphous inorganic solids are traditionally isotropic, thus, it is believed that they only grow in a non-preferential way without the assistance of regulators, leading to the morphologies of nanospheres or irregular aggregates of nanoparticles. However, in the presence of (ortho)phosphate (Pi) and pyrophosphate ions (PPi) which have synergistic roles in biomineralization, the highly elongated amorphous nanowires (denoted ACPPNs) form in a regulator-free aqueous solution (without templates, additives, organics, etc). Based on thorough characterization and tracking of the formation process (e.
View Article and Find Full Text PDFLateral heterostructures combining two multilayer group IV chalcogenide van der Waals semiconductors have attracted interest for optoelectronics, twistronics, and valleytronics, owing to their structural anisotropy, bulk-like electronic properties, enhanced optical thickness, and vertical interfaces enabling in-plane charge manipulation/separation, perpendicular to the trajectory of incident light. Group IV monochalcogenides support propagating photonic waveguide modes, but their interference gives rise to complex light emission patterns throughout the visible/near-infrared range both in uniform flakes and single-interface lateral heterostructures. Here, this work demonstrates the judicious integration of pure and alloyed monochalcogenide crystals into multimaterial heterostructures with unique photonic properties, notably the ability to select photonic modes with targeted discrete energies through geometric factors rather than band engineering.
View Article and Find Full Text PDFMaterials with large birefringence (Δn, where n is the refractive index) are sought after for polarization control (e.g., in wave plates, polarizing beam splitters, etc.
View Article and Find Full Text PDFUltrathin MoS has shown remarkable characteristics at the atomic scale with an immutable disorder to weak external stimuli. Ion beam modification unlocks the potential to selectively tune the size, concentration, and morphology of defects produced at the site of impact in 2D materials. Combining experiments, first-principles calculations, atomistic simulations, and transfer learning, it is shown that irradiation-induced defects can induce a rotation-dependent moiré pattern in vertically stacked homobilayers of MoS by deforming the atomically thin material and exciting surface acoustic waves (SAWs).
View Article and Find Full Text PDFGrain boundaries (GBs) are a prolific microstructural feature that dominates the functionality of a wide class of materials. The functionality at a GB results from the unique atomic arrangements, different from those in the grain, that have driven extensive experimental and theoretical studies correlating atomic-scale GB structures to macroscopic electronic, infrared optical, and thermal properties. In this work, a SrTiO GB is examined using atomic-resolution aberration-corrected scanning transmission electron microscopy and ultrahigh-energy-resolution monochromated electron energy-loss spectroscopy, in conjunction with density functional theory.
View Article and Find Full Text PDFQuantum coupling in arrayed nanostructures can produce novel mesoscale properties such as electronic minibands to improve the performance of optoelectronic devices, including ultra-efficient solar cells and infrared photodetectors. Colloidal PbSe quantum dots (QDs) that self-assemble into epitaxially-fused superlattices (epi-SLs) are predicted to exhibit such collective phenomena. Here, we show the emergence of distinct local electronic states induced by crystalline necks that connect individual PbSe QDs and modulate the bandgap energy across the epi-SL.
View Article and Find Full Text PDFThe advancement of nanoenabled wafer-based devices requires the establishment of core competencies related to the deterministic positioning of nanometric building blocks over large areas. Within this realm, plasmonic single-crystal gold nanotriangles represent one of the most attractive nanoscale components but where the formation of addressable arrays at scale has heretofore proven impracticable. Herein, a benchtop process is presented for the formation of large-area periodic arrays of gold nanotriangles.
View Article and Find Full Text PDFWe propose a novel Timed Intervention S, P, E, I, Q, R, D model for projecting the possible futures of the COVID-19 pandemic in the USA. The proposed model introduces a series of timed interventions that can account for the influence of real time changes in government policy and social norms. We consider three separate types of interventions: (i) Protective interventions: Where population moves from susceptible to protected corresponding to mask mandates, stay-at-home orders and/or social distancing.
View Article and Find Full Text PDFQuantum materials are usually heterogeneous, with structural defects, impurities, surfaces, edges, interfaces, and disorder. These heterogeneities are sometimes viewed as liabilities within conventional systems; however, their electronic and magnetic structures often define and affect the quantum phenomena such as coherence, interaction, entanglement, and topological effects in the host system. Therefore, a critical need is to understand the roles of heterogeneities in order to endow materials with new quantum functions for energy and quantum information science applications.
View Article and Find Full Text PDFAs the length scales of materials decrease, the heterogeneities associated with interfaces become almost as important as the surrounding materials. This has led to extensive studies of emergent electronic and magnetic interface properties in superlattices. However, the interfacial vibrations that affect the phonon-mediated properties, such as thermal conductivity, are measured using macroscopic techniques that lack spatial resolution.
View Article and Find Full Text PDFHyperbolic phonon polaritons (HPhPs) in hexagonal boron nitride (hBN) enable the direct manipulation of mid-infrared light at nanometer scales, many orders of magnitude below the free-space light wavelength. High-resolution monochromated electron energy-loss spectroscopy (EELS) facilitates measurement of excitations with energies extending into the mid-infrared while maintaining nanoscale spatial resolution, making it ideal for detecting HPhPs. The electron beam is a precise source and probe of HPhPs, which allows the observation of nanoscale confinement in HPhP structures and directly extract hBN polariton dispersions for both modes in the bulk of the flake and modes along the edge.
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