Jordan A. Hachtel

Quaternary 2D Transition Metal Dichalcogenides (TMDs) with Tunable Bandgap

Alloying/doping in 2D material is important due to wide range bandgap tunability. Increasing the number of components would increase the degree of freedom which can provide more flexibility in tuning the bandgap and also reduces the growth temperature. Here, synthesis of quaternary alloys Mox W1-x S2y Se2(1-y) is reported using chemical vapor deposition. The composition of alloys is tuned by changing the growth temperatures. As a result, the bandgap can be tuned which varies from 1.61 to 1.85 eV. The detailed theoretical calculation supports the experimental observation and shows a possibility of wide tunability of bandgap.

Bias dependence of total ionizing dose effects in SiGe-SiO2HfO2 p MOS FinFETs

The total ionizing dose (TID) response of double-gate SiGe- SiO₂/HfO₂ pMOS FinFET devices is investigated under different device bias conditions. Negative bias irradiation leads to the worst-case degradation due to increased hole trapping in the HfO₂ layer, in contrast to what is typically observed for devices with SiO₂ or HfO₂ gate dielectrics. This occurs in the devices because radiation-induced holes that are generated in the SiO₂ interfacial layer can transport and become trapped in the HfO₂ under negative bias, leading to a more negative threshold voltage shift than observed at 0 V bias. Similarly, radiation-induced electrons that are generated in the SiO₂ interfacial layer can transport into the HfO₂ and become trapped under positive bias, leading to a more positive threshold voltage shift than observed at 0 V bias.

Re Doping in 2D Transition Metal Dichalcogenides as a New Route to Tailor Structural Phases and Induced Magnetism

Alloying in 2D results in the development of new, diverse, and versatile systems with prospects in bandgap engineering, catalysis, and energy storage. Tailoring structural phase transitions using alloying is a novel idea with implications in designing all 2D device architecture as the structural phases in 2D materials such as transition metal dichalcogenides are correlated with electronic phases. Here, this study develops a new growth strategy employing chemical vapor deposition to grow monolayer 2D alloys of Re-doped MoSe2 with show composition tunable structural phase variations. The compositions where the phase transition is observed agree well with the theoretical predictions for these 2D systems. It is also shown that in addition to the predicted new electronic phases, these systems also provide opportunities to study novel phenomena such as magnetism which broadens the range of their applications.

Gold nanotriangles decorated with superparamagnetic iron oxide nanoparticles: a compositional and microstructural study

The combination of iron oxide and gold in a single nanoparticle results in both magnetic and plasmonic properties that can stimulate novel applications in bio-sensing, medical imaging, or therapeutics. Microwave assisted heating allows the fabrication of multi-component, multi-functional nanostructures by promoting selective heating at desired sites. Recently, we reported a microwave-assisted polyol route yielding gold nanotriangles decorated with iron oxide nanoparticles. Here, we present an in-depth microstructural and compositional characterization of the system using scanning transmission electron microscopy (STEM) and electron energy loss spectroscopy (EELS). A method to remove the iron oxide nanoparticles from the gold nanocrystals and some insights on crystal nucleation and growth mechanisms are also provided.

Probing plasmons in three dimensions by combining complementary spectroscopies in a scanning transmission electron microscope

The nanoscale optical response of surface plasmons in three-dimensional metallic nanostructures plays an important role in many nanotechnology applications, where precise spatial and spectral characteristics of plasmonic elements control device performance. Electron energy loss spectroscopy (EELS) and cathodoluminescence (CL) within a scanning transmission electron microscope have proven to be valuable tools for studying plasmonics at the nanoscale. Each technique has been used separately, producing three-dimensional reconstructions through tomography, often aided by simulations for complete characterization. Here we demonstrate that the complementary nature of the two techniques, namely that EELS probes beam-induced electronic excitations while CL probes radiative decay, allows us to directly obtain a spatially- and spectrally-resolved picture of the plasmonic characteristics of nanostructures in three dimensions. The approach enables nanoparticle-by-nanoparticle plasmonic analysis in three dimensions to aid in the design of diverse nanoplasmonic applications.

Unveiling Complex Plasmonic Resonances in Archimedean Nanospirals through Cathodoluminescence in a Scanning Transmission Electron Microscope

Metallic nanostructures with a complex plasmonic response, such as the Archimedean nanospiral (ANS) present novel ways to utilize plasmonics in modern technology [1,2]. The nanospiral can support several resonant modes, with distinct electric field profiles as shown by finite-difference time-domain (FDTD) simulations such as the hourglass (500-650nm) and focusing (650-980nm) modes [2]. In addition to the linear plasmonic response, the ANS exhibits a stronger second-order nonlinearity than seen in other metallic nanostructured systems. A high spatial-resolution picture of the plasmonic modes is critical to understanding the interactions between plasmonic modes that drive the high non-linear efficiencies [3].

Quantitative first-principles theory of interface absorption in multilayer heterostructures

The unique chemical bonds and electronic states of interfaces result in optical properties that are different from those of the constituting bulk materials. In the nanoscale regime, the interface effects can be dominant and impact the optical response of devices. Using density functional theory (DFT), the interface effects can be calculated, but DFT is computationally limited to small systems. We describe a method to combine DFT with macroscopic methodologies to extract the interface effect on absorption in a consistent and quantifiable manner. The extracted interface effects are an independent parameter and can be applied to more complicated systems. We demonstrate, using NiSi2/Si heterostructures, that by varying the relative volume fractions of interface and bulk, we can tune the spectral range of the heterostructure absorption.

Exploring the capabilities of monochromated electron energy loss spectroscopy in the infrared regime

Monochromated electron energy loss spectroscopy (EELS) is one of the leading techniques to study materials properties that correspond to low (<5 eV) energy losses (i.e. band-gaps, plasmons, and excitons) with nanoscale spatial resolution. Recently a new generation of monochromators have become available, opening regimes and unlocking excitations that were previously unobservable in the electron microscope. The capabilities of these new instruments are still being explored, and here we study the effect of monochromation on various aspects of EELS analysis in the infrared (<1 eV) regime. We investigate the effect of varying levels of monochromation on energy resolution, zero-loss peak (ZLP) tail reduction, ZLP tail shape, signal-to-noise-ratio, and spatial resolution. From these experiments, the new capabilities of monochromated EELS are shown to be highly promising for the future of localized spectroscopic analysis.

Polarization- and wavelength-resolved near-field imaging of complex plasmonic modes in Archimedean nanospirals

Asymmetric nanophotonic structures enable a wide range of opportunities in optical nanotechnology because they support efficient optical nonlinearities mediated by multiple plasmon resonances over a broad spectral range. The Archimedean nanospiral is a canonical example of a chiral plasmonic structure because it supports even-order nonlinearities that are not generally accessible in locally symmetric geometries. However, the complex spiral response makes nanoscale experimental characterization of the plasmonic near-field structure highly desirable. Here we employ high-efficiency, high-spatial-resolution cathodoluminescence imaging in a scanning transmission electron microscope to describe the spatial, spectral, and polarization response of plasmon modes in the nanospiral geometry.

Structural Phase Transformation in Strained Monolayer MoWSe2 Alloy

Two-dimensional (2D) materials exhibit different mechanical properties from their bulk counterparts owing to their monolayer atomic thickness. Here, we have examined the mechanical behavior of 2D molybdenum tungsten diselenide (MoWSe2) precipitation alloy grown using chemical vapor deposition and composed of numerous nanoscopic MoSe2 and WSe2 regions. Applying a bending strain blue-shifted the MoSe2 and WSe2 A1g Raman modes with the stress concentrated near the precipitate interfaces predominantly affecting the WSe2 modes. In situ local Raman measurements suggested that the crack propagated primarily thorough MoSe2-rich regions in the monolayer alloy. Molecular dynamics (MD) simulations were performed to study crack propagation in an MoSe2 monolayer containing nanoscopic WSe2 regions akin to the experiment. Raman spectra calculated from MD trajectories of crack propagation confirmed the emergence of intermediate peaks in the strained monolayer alloy, mirroring experimental results. The simulations revealed that the stress buildup around the crack tip caused an irreversible structural transformation from the 2H to 1T phase both in the MoSe2 matrix and WSe2 patches. This was corroborated by high-angle annular dark-field images. Crack branching and subsequent healing of a crack branch were also observed in WSe2, indicating the increased toughness and crack propagation resistance of the alloyed 2D MoWSe2 over the unalloyed counterparts.