arXiv subjects

Timothy J. Booth

Publications and source records attributed to Timothy J. Booth.

12 recordsLinked to original sources

arXiv2025

Enhanced and directional light emission from two-dimensional excitons using Mie voids

Controlling light emission at the nanoscale has important applications in solid-state lighting, displays, and quantum light sources. Achieving this control requires both enhanced local electromagnetic fields to boost emission intensity and engineered radiation patterns to direct photons efficiently. Mie voids, consisting of an air cavity surrounded by a high-index semiconductor, are particularly suited for this purpose because they expose their strongest fields in an accessible region for nearby emitters while supporting resonances that shape directional emission through interference. Here, we demonstrate an all-van der Waals nanophotonic platform that couples excitons in atomically thin WS$_2$ to Mie void resonators formed in WSe$_2$. Guided by electromagnetic simulations, we identify void geometries that maximize photoluminescence through synergistic enhancement of excitation and emission processes. We also develop a two-step fabrication strategy that enables independent control of void diameter and depth, providing a route to systematically tune the optical response. Experimentally, we observe up to a 600-fold increase in photoluminescence intensity from monolayer WS$_2$ placed on individual voids compared to on an unstructured WSe$_2$, along with pronounced out-of-plane beaming of light that yields a forward-to-off-axis enhancement of 2.6 dB. Our results establish Mie voids in van der Waals semiconductors as a new platform for controlling light-matter interactions and realizing compact, directional, and efficient nanoscale light sources.

physics.optics↗

arXiv2025

Gradient Electronic Landscapes in van der Waals Heterostructures

Two-dimensional (2D) materials such as graphene and hexagonal boron nitride (hBN) provide a versatile platform for quantum electronics. Experiments generally require encapsulating graphene within hBN flakes, forming a protective van der Waals (vdW) heterostructure that preserves delicate properties of the embedded crystal. To produce functional devices, heterostructures are typically shaped by electron beam lithography and etching, which has driven progress in 2D materials research. However, patterns are primarily restricted to in-plane geometries such as boxes, holes, and stripes, limiting opportunities for advanced architectures. Here, we use thermal scanning-probe lithography (tSPL) to produce smooth topographic landscapes in vdW heterostructures, controlling the thickness degree of freedom with nanometer precision. We electrically gate a sinusoidal topography to impose an electric-field gradient on the graphene layer to spatially modulate charge-carrier doping. We observe signatures of the landscape in transport measurements-resistance-peak spreading and commensurability oscillations-establishing tSPL for tailoring high-quality quantum electronics.

cond-mat.mes-hall↗

arXiv2025

Fourier-Tailored Light-Matter Coupling in van der Waals Heterostructures

Dielectric structures can support low-absorption optical modes, which are attractive for engineering light-matter interactions with excitonic resonances in two-dimensional (2D) materials. However, the coupling strength is often limited by the electromagnetic field being confined inside the dielectric, reducing spatial overlap with the active excitonic material. Here, we demonstrate a scheme for enhanced light-matter coupling by embedding excitonic tungsten disulfide (WS$_2$) within dielectric hexagonal boron nitride (hBN), forming a van der Waals (vdW) heterostructure that optimizes the field overlap and alignment between excitons and optical waveguide modes. To tailor diffractive coupling between free-space light and the waveguide modes in the vdW heterostructure, we fabricate Fourier surfaces in the top hBN layer using thermal scanning-probe lithography and etching, producing sinusoidal topographic landscapes with nanometer precision. We observe the formation of exciton-polaritons with a Rabi splitting indicating that the system is at the onset of strong coupling. These results demonstrate the potential of Fourier-tailored vdW heterostructures for exploring advanced optoelectronic and quantum devices.

physics.optics↗

arXiv2024

Quantitative mapping of smooth topographic landscapes produced by thermal scanning-probe lithography

Scanning probe microscopy (SPM) is a powerful technique for mapping nanoscale surface properties through tip-sample interactions. Thermal scanning-probe lithography (tSPL) is an advanced SPM variant that uses a silicon tip on a heated cantilever to sculpt and measure polymer films with nanometer precision. The surfaces produced by tSPL-smooth topographic landscapes-allow mathematically defined contours to be fabricated on the nanoscale, enabling sophisticated functionalities for photonic, electronic, chemical, and biological technologies. Evaluating the physical effects of a landscape requires fitting arbitrary mathematical functions to SPM datasets, however, this capability does not exist in standard analysis programs. Here, we provide an open-source software package (FunFit) to fit analytical functions to SPM data and develop a fabrication and characterization protocol based on this analysis. We demonstrate the benefit of this approach by patterning periodic and quasiperiodic landscapes in a polymer resist with tSPL, which we transfer to hexagonal boron nitride (hBN) flakes with high fidelity via reactive-ion etching. The topographic landscapes in polymers and hBN are measured with tSPL and atomic force microscopy (AFM), respectively. Within the FunFit program, the datasets are corrected for artefacts, fit with analytical functions, and compared, providing critical feedback on the fabrication procedure. Beyond application to tSPL, this protocol can improve analysis, reproducibility, and process development for a broad range of SPM experiments. The protocol can be performed within a working day by an inexperienced user, where fabrication and characterization take a few hours and software analysis takes a few minutes.

cond-mat.mes-hall↗

arXiv2023

Terahertz s-SNOM reveals nonlocal nanoscale conductivity of graphene

As photonic and electronic technologies approach nanometre length scales and terahertz operating speeds, electrical conductivity can no longer be treated as a purely local material parameter. In this regime, charge transport becomes intrinsically nonlocal, with conductivity depending on both frequency and momentum, $\sigma(\omega,q)$, fundamentally limiting field confinement, dispersion, and loss in nanoscale devices. Here, we directly measure the nonlocal nanoscale conductivity of graphene using terahertz scattering-type near-field optical microscopy. By combining broadband THz near-field spectroscopy with quantitative electrodynamic modelling, we extract the complex conductivity of single- and few-layer graphene with $\sim$50 nm spatial resolution. We find that nonlocal response dominates the terahertz conductivity of monolayer graphene even at length scales comparable to practical device dimensions. These results establish nonlocal conductivity as a measurable and design-relevant material property in the terahertz regime, providing a quantitative foundation for predicting performance limits in ultracompact photonic and electronic systems.

physics.optics↗

arXiv2022

Fermi Level Depinning in Two-Dimensional Materials Using a Fluorinated Bilayer Graphene Barrier

Strong Fermi level pinning (FLP) - often attributed to metal-induced gap states at the interfacial contacts - severely reduces the tunability of the Schottky barrier height of the junction and limits applications of the 2D materials in electronics and optoelectronics. Here, we show that fluorinated bilayer graphene (FBLG) can be used as a barrier to effectively prevent FLP at metal/2D materials interfaces. FLBG can be produced via short exposure (1-3 min) to SF6 plasma that fluorinates only the top layer of a bilayer graphene with covalent C-F bonding, while the bottom layer remains intrinsic, resulting in a band gap opening of about 75 meV. Inserting FBLG between the metallic contacts and a layer of MoS2 reduces the Schottky barrier height dramatically for the low-work function metals (313 and 260 meV for Ti and Cr, respectively) while it increases for the high-work function one ( 160 meV for Pd), corresponding to an improved pinning factor. Our results provide a straightforward method to generate atomically thin dielectrics with applications not only for depinning the Fermi level at metal/transition metal dichalcogenide (TMD) interfaces but also for solving many other problems in electronics and optoelectronics

physics.app-ph↗

arXiv2021

Brobdingnagian photon bunching in cathodoluminescence of excitons in WS$_2$ monolayer

Cathodoluminescence spectroscopy in conjunction with second-order auto-correlation measurements of $g_2(\tau)$ allows to extensively study the synchronization of quantum light sources in low-dimensional structures. Co-existing excitons in two-dimensional transition metal dichalcogenide monolayers provide a great source of identical quantum emitters which can be simultaneously excited by an electron. In this article, we demonstrate large photon bunching with $g_2(0)$ up to $156\pm16$ of a tungsten disulfide monolayer, exhibiting a strong dependence on the electron-beam current density. To further improve the excitation synchronization and the electron-emitter interaction, we show exemplary that the careful selection of a simple and compact geometry -- a thin, monocrystalline gold nanodisk -- can be used to realize a record-high bunching $g_2(0)$ of up to $2152\pm236$. This approach to control the electron excitation of excitons in a \ce{WS2} monolayer allows for the synchronization of quantum emitters in an ensemble, which is important to further advance quantum information processing and computing technologies.

cond-mat.mes-hall↗

arXiv2021

Universal Non-Volatile Resistive Switching Behavior in 2D Metal Dichalcogenides Featuring Unique Conductive-Point Random Access Memory Effect

Two-dimensional materials have been discovered to exhibit non-volatile resistive switching (NVRS) phenomenon. In our work, we reported the universal NVRS behavior in a dozen metal dichalcogenides, featuring low switching voltage, large on/off ratio, fast switching speed and forming free characteristics. A unique conductive-point random access memory (CPRAM) effect is used to explain the switching mechanisms, supported by experimental results from current-sweep measurements.

cond-mat.mes-hall↗

arXiv2021

Super-Resolution Nanolithography of Two-Dimensional Materials by Anisotropic Etching

Nanostructuring allows altering of the electronic and photonic properties of two-dimensional (2D) materials. The efficiency, flexibility, and convenience of top-down lithography processes are however compromised by nm-scale edge roughness and resolution variability issues, which especially affects the performance of 2D materials. Here we study how dry anisotropic etching of multilayer 2D materials with sulfur hexafluoride (SF6) may overcome some of these issues, showing results for hexagonal boron nitride (hBN), tungsten disulfide (WS2), tungsten diselenide (WSe2), molybdenum disulfide (MoS2), molybdenum ditelluride (MoTe2). Scanning and transmission electron microscopy reveal that etching leads to anisotropic hexagonal features in the studied transition metal dichalcogenides, with the relative degree of anisotropy ranked as: WS2 > WSe2 > MoTe2 / MoS2. Etched holes are terminated by zigzag edges while etched dots (protrusions) are terminated by armchair edges. This can be explained by Wulff constructions, taking the relative stabilities of the edges and the AA stacking order into account. Patterns in WS2 are transferred to an underlying graphite layer, demonstrating a possible use for creating sub-10 nm features. In contrast, multilayer hBN exhibits no lateral anisotropy, but shows consistent vertical etch angles, independent of crystal orientation. This is used to create super-resolution lithographic patterns with ultra-sharp corners at the base of the hBN crystal, which are transferred into an underlying graphite crystal. We find that the anisotropic SF6 reactive ion etching process makes it possible to downsize nanostructures to obtain smooth edges, sharp corners, and feature sizes significantly below the resolution limit of electron beam lithography. The nanostructured 2D materials can be used themselves or as etch-masks to pattern other nanomaterials.

cond-mat.mtrl-sci↗

arXiv2018

A general approach for the synthesis of two-dimensional binary compounds

Only a few of the vast range of potential two-dimensional materials have been isolated or synthesised to date. Typically, 2D materials are discovered by mechanically exfoliating naturally occurring bulk crystals to produce atomically thin layers, after which a material-specific vapour synthesis method must be developed to grow interesting candidates in a scalable manner. Here we show a general approach for synthesising thin layers of two-dimensional binary compounds. We apply the method to obtain high quality, epitaxial MoS2 films, and extend the principle to the synthesis of a wide range of other materials - both well-known and never-before isolated - including transition metal sulphides, selenides, tellurides, and nitrides. This approach greatly simplifies the synthesis of currently known materials, and provides a general framework for synthesising both predicted and unexpected new 2D compounds.

cond-mat.mtrl-sci↗

arXiv2018

Raman Spectral Indicators of Catalyst Decoupling for Transfer of CVD Grown 2D Materials

Through a combination of monitoring the Raman spectral characteristics of 2D materials grown on copper catalyst layers, and wafer scale automated detection of the fraction of transferred material, we reproducibly achieve transfers with over 97.5% monolayer hexagonal boron nitride and 99.7% monolayer graphene coverage, for up to 300 mm diameter wafers. We find a strong correlation between the transfer coverage obtained for graphene and the emergence of a lower wavenumber 2D- peak component, with the concurrent disappearance of the higher wavenumber 2D+ peak component during oxidation of the catalyst surface. The 2D peak characteristics can therefore act as an unambiguous predictor of the success of the transfer. The combined monitoring and transfer process presented here is highly scalable and amenable for roll-to-roll processing.

cond-mat.mtrl-sci↗

arXiv2016

The hot pick-up technique for batch assembly of van der Waals heterostructures

The assembly of individual two-dimensional materials into van der Waals heterostructures enables the construction of layered three-dimensional materials with desirable electronic and optical properties. A core problem in the fabrication of these structures is the formation of clean interfaces between the individual two-dimensional materials which would affect device performance. We present here a technique for the rapid batch fabrication of van der Waals heterostructures, demonstrated by the controlled production of 22 mono-, bi- and trilayer graphene stacks encapsulated in hexagonal boron nitride with close to 100% yield. For the monolayer devices we found semiclassical mean free paths up to 0.9 micrometer, with the narrowest samples showing clear indications of the transport being affected by boundary scattering. The presented method readily lends itself to fabrication of van der Waals heterostructures in both ambient and controlled atmospheres, while the ability to assemble pre-patterned layers paves the way for complex three-dimensional architectures.

cond-mat.mes-hall↗