The transition metal dichalcogenide 1T-TaS exhibits a Charge Density Wave (CDW) with in-plane chirality. Due to the rich phase diagram, the Ferro-Rotational Order (FRO) can be tuned by external stimuli. The FRO is studied by Angle-Resolved Photoelectron Spectroscopy (ARPES), Raman spectroscopy, and Selected Area Electron Diffraction (SAED).
View Article and Find Full Text PDFHigh-quality 1T-TaS crystals are investigated by angle-resolved photoelectron spectroscopy, Raman spectroscopy, and low-energy electron diffraction. The Ferro-Rotational Order (FRO) of the charge density wave switches configuration at the transition between the commensurate and the nearly commensurate phase. This process requires samples without built-in or externally induced strain.
View Article and Find Full Text PDFFour-dimensional scanning transmission electron microscopy (4D-STEM) offers an attractive approach to simultaneously obtain precise structural determinations and capture details of local electric fields and charge densities. However, accurately extracting quantitative data at the atomic scale poses challenges, primarily due to probe propagation and size-related effects, which may even lead to misinterpretations of qualitative effects. In this study, we present a comprehensive analysis of electric fields and charge densities in both pristine and defective h-BN flakes.
View Article and Find Full Text PDFThe growth of controlled 1D carbon-based nanostructures on metal surfaces is a multistep process whose path, activation energies, and intermediate metastable states strongly depend on the employed substrate. Whereas this process has been extensively studied on gold, less work has been dedicated to silver surfaces, which have a rather different catalytic activity. In this work, we present an experimental and theoretical investigation of the growth of poly--phenylene (PPP) chains and subsequent narrow graphene ribbons starting from 4,4″-dibromo--terphenyl molecular precursors deposited at the silver surface.
View Article and Find Full Text PDFFollowing optical excitations' life span from creation to decay into photons is crucial in understanding materials photophysics. Macroscopically, this is studied using optical techniques, such as photoluminescence excitation spectroscopy. However, excitation and emission pathways can vary at nanometer scales, preventing direct access, as no characterization technique has the relevant spatial, spectral, and time resolution.
View Article and Find Full Text PDFStructural, electronic, and chemical nanoscale modifications of transition metal dichalcogenide monolayers alter their optical properties. A key missing element for complete control is a direct spatial correlation of optical response to nanoscale modifications due to the large gap in spatial resolution between optical spectroscopy and nanometer-resolved techniques. Here, we bridge this gap by obtaining nanometer-resolved optical properties using electron spectroscopy at cryogenic temperatures, specifically electron energy loss spectroscopy for absorption and cathodoluminescence for emission, which are then directly correlated to chemical and structural information.
View Article and Find Full Text PDFHybrid/moiré interlayer and intralayer excitons have been realized in twisted two-dimensional transition metal chalcogenides (2D-TMD) due to variation in local moiré potential within a moiré supercell. Though moiré excitons have been detected in TMD heterostructures by macroscopic spectroscopic techniques, their spatial distribution is experimentally unknown. In the present work, using high-resolution scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy (EELS), we explore the effect of the twist angle in MoS/WSe heterostructures.
View Article and Find Full Text PDFAtomic vibrations and phonons are an excellent source of information on nanomaterials that we can access through a variety of methods including Raman scattering, infrared spectroscopy, and electron energy-loss spectroscopy (EELS). In the presence of a plasmon local field, vibrations are strongly modified and, in particular, their dipolar strengths are highly enhanced, thus rendering Raman scattering and infrared spectroscopy extremely sensitive techniques. Here, we experimentally demonstrate that the interaction between a relativistic electron and vibrational modes in nanostructures is fundamentally modified in the presence of plasmons.
View Article and Find Full Text PDFThe evolution of the scanning modules for scanning transmission electron microscopes (STEM) allows now to generate arbitrary scan pathways, an approach currently explored to improve acquisition speed and to reduce electron dose effects. In this work, we present the implementation of a random scan operating mode in STEM achieved at the hardware level via a custom scan control module. A pre-defined pattern with fully shuffled raster order is used to sample the entire region of interest.
View Article and Find Full Text PDFHere, we analyze the effect of Cr doping on WSe crystals. The topology and the chemistry of the doped samples have been investigated by atom-resolved scanning transmission electron microscopy combined with electron energy loss spectroscopy. Cr (measured to have formal valence 3+) occupies W sites (formal valence 4+), indicating a possible hole doping.
View Article and Find Full Text PDFThe epitaxial graphene buffer layer on the Si face of hexagonal SiC shows a promising band gap, of which the precise origin remains to be understood. In this work, we correlate the electronic to the atomic structure of the buffer layer by combining angle resolved photoemission spectroscopy (ARPES), scanning tunneling microscopy (STM), and high-resolution scanning transmission electron microscopy (HR-STEM). We show that the band structure in the buffer has an electronic periodicity related to the structural periodicity observed in STM images and published X-ray diffraction.
View Article and Find Full Text PDFRecent experimental investigations have confirmed the possibility to synthesize and exploit polytypism in group IV nanowires. Driven by this promising evidence, we use first-principles methods based on density functional theory and many-body perturbation theory to investigate the electronic and optical properties of hexagonal-diamond and cubic-diamond Si NWs as well as their homojunctions. We show that hexagonal-diamond NWs are characterized by a more pronounced quantum confinement effect than cubic-diamond NWs.
View Article and Find Full Text PDFTo date, quantum sources in the ultraviolet (UV) spectral region have been obtained only in semiconductor quantum dots. Color centers in wide bandgap materials may represent a more effective alternative. However, the quest for UV quantum emitters in bulk crystals faces the difficulty of combining an efficient UV excitation/detection optical setup with the capability of addressing individual color centers in potentially highly defective materials.
View Article and Find Full Text PDFGraphene nanoribbons grown on sidewall facets of SiC have demonstrated exceptional quantized ballistic transport up to 15 μm at room temperature. Angular-resolved photoemission spectroscopy (ARPES) has shown that the ribbons have the band structure of charge neutral graphene, while bent regions of the ribbon develop a bandgap. We present scanning tunneling microscopy and transmission electron microscopy of armchair nanoribbons grown on recrystallized sidewall trenches etched in SiC.
View Article and Find Full Text PDFArtificial multiferroic tunnel junctions combining a ferroelectric tunnel barrier of BaTiO(3) with magnetic electrodes display a tunnel magnetoresistance whose intensity can be controlled by the ferroelectric polarization of the barrier. This effect, called tunnel electromagnetoresistance (TEMR), and the corollary magnetoelectric coupling mechanisms at the BaTiO(3)/Fe interface were recently reported through macroscopic techniques. Here, we use advanced spectromicroscopy techniques by means of aberration-corrected scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy (EELS) to probe locally the nanoscale structural and electronic modifications at the ferroelectric/ferromagnetic interface.
View Article and Find Full Text PDFWe demonstrate that free graphene sheet edges can curl back on themselves, reconstructing as nanotubes. This results in lower formation energies than any other nonfunctionalized edge structure reported to date in the literature. We determine the critical tube size and formation barrier and compare with density functional simulations of other edge terminations including a new reconstructed Klein edge.
View Article and Find Full Text PDF