arXiv subjects

Joan M. Redwing

Publications and source records attributed to Joan M. Redwing.

17 recordsLinked to original sources

arXiv2026

Lifetime Sample Tracking (LiST): A Data Platform for Materials Science

The 2D Crystal Consortium Materials Innovation Platform (2DCC-MIP) is an NSF supported national user facility focused on advancing the synthesis of 2D materials, monolayers, surfaces, and interfaces. The need for the facility to organize and share data with users led to the development of an internal data management and analysis engine, the Lifetime Sample Tracking platform (LiST). This infrastructure allows the automated capture, curation, analysis and dissemination of data ranging from experimental materials synthesis parameters and characterization, to theoretical first-principles and ReaxFF molecular dynamics modeling1. The system currently hosts synthesis and property data (accessible via a REST API) on approximately twenty thousand samples produced by the 2DCC grown using a variety of techniques from bulk crystal growth to metal-organic chemical vapor deposition (MOCVD) and molecular beam epitaxy (MBE), among others. Data used in publications can easily be grouped by the system into data packages that are given digital object identifiers (DOIs) for inclusion with each publication. The LiST platform is now being used by groups outside of the 2DCC as a solution for data curation in materials science. Data management tools such as LiST support the materials development process by allowing a closed loop iteration between synthesis, characterization, theory, and targeted materials design. This also enables machine learning (ML) research, artificial intelligence (AI) analysis, and the potential for autonomous synthesis in the future.

cond-mat.mtrl-sci↗

arXiv2026

Controlled non-volatile modulation of optical dispersion in monolayer tungsten disulfide via ferroelectric polarization patterning

The manipulation of optical properties, including reflection, refraction, polarization, phase, and frequency, has long been central to advancing photonic and optoelectronic technologies. However, existing electro-optical approaches rely on volatile mechanisms that require continuous power consumption. Here, we demonstrate strong, nonvolatile modulation of optical dispersion in monolayer tungsten disulfide (ML WS2) using patterned ferroelectric domains in aluminum scandium nitride (AlScN). By locally poling ferroelectric domains into opposite states, we achieve substantial manipulation of the complex refractive index (Delta n > 0.7, Delta k > 0.4) and excitonic energy shifts (~50 meV) in ML WS2, comparable to previous gate-tuning approaches while eliminating continuous power consumption. We introduce an asymmetric screening model that reveals how ferroelectric polarization induces carrier-density-dependent Coulomb screening, leading to distinct excitonic behaviors between electron- and hole-doped regions. Furthermore, we demonstrate a gate-free lateral p-n homojunction with a rectification ratio of 6e10^3, formed through spatial carrier redistribution. These findings establish ferroelectric/2D heterostructures as a powerful platform for nonvolatile optical dispersion engineering, enabling energy-efficient, reconfigurable photonic and optoelectronic devices.

physics.optics↗

arXiv2025

Proximity-tuned Magnetic and Transport Anomalies in All-epitaxial Fe5-xGeTe2/WSe2 Van der Waals Heterostructures

Van der Waals (vdW) heterostructures combining two-dimensional (2D) ferromagnets and semiconducting transition-metal dichalcogenides (TMDCs) offer highly promising opportunities for tailoring 2D magnetism through interfacial proximity effects, enabling unique physical phenomena inaccessible in 3D systems and achieving functionalities beyond conventional spintronics. However, current fabrication of vdW heterostructures still relies heavily on the manual stacking of exfoliated 2D flakes, leading to critical challenges in scalability, interfacial quality, thickness control and device integration. This work reports on the realization of all-epitaxial, high-quality Fe5-xGeTe2(FGT)/WSe2 heterostructures exhibiting perpendicular magnetic anisotropy (PMA) and room-temperature ferromagnetism. The FGT/WSe2 system demonstrates temperature-driven magnetic transitions, higher-order PMA contributions and large anisotropic magnetoresistance, highlighting sublattice-specific contributions to magnetic and transport properties. Notably, the FGT/WSe2 heterostructures display unconventional physical phenomena, including thickness- and temperature-dependent sign reversal of exchange bias, a reversed thickness trend in the unconventional Hall effect, and a non-monotonic PMA-thickness dependence. These anomalies indicate pronounced interfacial contributions arising from proximity effects enhanced by epitaxial interface quality. Collectively, this study provides deep insights into the magnetic and transport properties of FGT/WSe2 vdW heterostructures, establishing a scalable platform for exploring emergent 2D physics and advancing next-generation 2D spintronic technologies.

cond-mat.mes-hall↗

arXiv2025

Cross-Modal Characterization of Thin Film MoS$_2$ Using Generative Models

The growth and characterization of materials using empirical optimization typically requires a significant amount of expert time, experience, and resources. Several complementary characterization methods are routinely performed to determine the quality and properties of a grown sample. Machine learning (ML) can support the conventional approaches by using historical data to guide and provide speed and efficiency to the growth and characterization of materials. Specifically, ML can provide quantitative information from characterization data that is typically obtained from a different modality. In this study, we have investigated the feasibility of projecting the quantitative metric from microscopy measurements, such as atomic force microscopy (AFM), using data obtained from spectroscopy measurements, like Raman spectroscopy. Generative models were also trained to generate the full and specific features of the Raman and photoluminescence spectra from each other and the AFM images of the thin film MoS$_2$. The results are promising and have provided a foundational guide for the use of ML for the cross-modal characterization of materials for their accelerated, efficient, and cost-effective discovery.

cond-mat.mtrl-sci↗

arXiv2024

Broadband Light Harvesting from Scalable Two-Dimensional Semiconductor Heterostructures

Broadband absorption in the visible spectrum is essential in optoelectronic applications that involve power conversion such as photovoltaics and photocatalysis. Most ultrathin broadband absorbers use parasitic plasmonic structures that maximize absorption using surface plasmons and/or Fabry-Perot cavities, which limits the weight efficiency of the device. Here, we show the theoretical and experimental realization of an unpatterned/planar semiconductor thin-film absorber based on monolayer transition metal dichalcogenides (TMDCs). We experimentally demonstrate an average total absorption in the visible range (450 nm - 700 nm) of > 70% using > 4 nm of semiconductor absorbing materials scalable over large areas with vapor phase growth techniques. Our analysis suggests that a power conversion efficiency (PCE) of 15.54% and a specific power > 300 W g^-1 may be achieved in a photovoltaic cell based on this metamaterial absorber.

physics.optics↗

arXiv2024

Quantum Confined Luminescence in Two dimensions

Achieving localized light emission from monolayer two-dimensional (2D) transition metal dichalcogenides (TMDs) embedded in the matrix of another TMD has been theoretically proposed but not experimentally proven. In this study, we used cathodoluminescence performed in a scanning transmission electron microscope to unambiguously resolve localized light emission from 2D monolayer MoSe2 nanodots of varying sizes embedded in monolayer WSe2 matrix. We observed that the light emission strongly depends on the nanodot size wherein the emission is dominated by MoSe2 excitons in dots larger than 85 nm, and by MoSe2/WSe2 interface excitons below 50 nm. Interestingly, at extremely small dot sizes (< 10 nm), the electron energy levels in the nanodot become quantized, as demonstrated by a striking blue-shift in interface exciton emission, thus inducing quantum confined luminescence. These results establish controllable light emission from spatially confined 2D nanodots, which holds potential to be generalized to other 2D systems towards future nanophotonic applications.

cond-mat.mtrl-sci↗

arXiv2024

High-Performance Ferroelectric Field-Effect Transistors with Ultra-High Current and Carrier Densities

Ferroelectric field-effect transistors (FeFET) with two-dimensional (2D) semiconductor channels are promising low-power, embedded non-volatile memory (NVM) candidates for next-generation in-memory computing. However, the performance of FeFETs can be limited by a charge imbalance between the ferroelectric layer and the channel, and for low-dimensional semiconductors, also by a high contact resistance between the metal electrodes and the channel. Here, we report a significant enhancement in performance of contact-engineered FeFETs with a 2D MoS2 channel and a ferroelectric Al0.68Sc0.32N (AlScN) gate dielectric. Replacing Ti with In contact electrodes results in a fivefold increase in on-state current (~120 uA/um at 1 V) and on-to-off ratio (~2*10^7) in the FeFETs. In addition, the high carrier concentration in the MoS2 channel during the on-state (> 10^14 cm^-2) facilitates the observation of a metal-to-insulator phase transition in monolayer MoS2 permitting observation of high field effect mobility (> 100 cm^2V^-1s^-1) at cryogenic temperatures. Our work and devices broaden the potential of FeFETs and provides a unique platform to implement high-carrier-density transport in a 2D channel.

physics.app-ph↗

arXiv2023

Light-driven C-H bond activation mediated by 2D transition metal dichalcogenides

C-H bond activation enables the facile synthesis of new chemicals. While C-H activation in short-chain alkanes has been widely investigated, it remains largely unexplored for long-chain organic molecules. Here, we report light-driven C-H activation in complex organic materials mediated by 2D transition metal dichalcogenides (TMDCs) and the resultant solid-state synthesis of luminescent carbon dots in a spatially-resolved fashion. We unravel the efficient H adsorption and a lowered energy barrier of C-C coupling mediated by 2D TMDCs to promote C-H activation. Our results shed light on 2D materials for C-H activation in organic compounds for applications in organic chemistry, environmental remediation, and photonic materials.

cond-mat.mtrl-sci↗

arXiv2023

Non-Volatile Control of Valley Polarized Emission in 2D WSe2-AlScN Heterostructures

Achieving robust and electrically controlled valley polarization in monolayer transition metal dichalcogenides (ML-TMDs) is a frontier challenge for realistic valleytronic applications. Theoretical investigations show that integration of 2D materials with ferroelectrics is a promising strategy; however, its experimental demonstration has remained elusive. Here, we fabricate ferroelectric field-effect transistors using a ML-WSe2 channel and a AlScN ferroelectric dielectric, and experimentally demonstrate efficient tuning as well as non-volatile control of valley polarization. We measured a large array of transistors and obtained a maximum valley polarization of ~27% at 80 K with stable retention up to 5400 secs. The enhancement in the valley polarization was ascribed to the efficient exciton-to-trion (X-T) conversion and its coupling with an out-of-plane electric field, viz. the quantum-confined Stark effect. This changes the valley depolarization pathway from strong exchange interactions to slow spin-flip intervalley scattering. Our research demonstrates a promising approach for achieving non-volatile control over valley polarization and suggests new design principles for practical valleytronic devices.

cond-mat.mes-hall↗

arXiv2023

Exciton Confinement in Two-Dimensional, In-Plane, Quantum Heterostructures

Two-dimensional (2D) semiconductors are promising candidates for optoelectronic application and quantum information processes due to their inherent out-of-plane 2D confinement. In addition, they offer the possibility of achieving low-dimensional in-plane exciton confinement, similar to zero-dimensional quantum dots, with intriguing optical and electronic properties via strain or composition engineering. However, realizing such laterally confined 2D monolayers and systematically controlling size-dependent optical properties remain significant challenges. Here, we report the observation of lateral confinement of excitons in epitaxially grown in-plane MoSe2 quantum dots (~15-60 nm wide) inside a continuous matrix of WSe2 monolayer film via a sequential epitaxial growth process. Various optical spectroscopy techniques reveal the size-dependent exciton confinement in the MoSe2 monolayer quantum dots with exciton blue shift (12-40 meV) at a low temperature as compared to continuous monolayer MoSe2. Finally, single-photon emission was also observed from the smallest dots at 1.6 K. Our study opens the door to compositionally engineered, tunable, in-plane quantum light sources in 2D semiconductors.

cond-mat.mes-hall↗

arXiv2022

High Density, Localized Quantum Emitters in Strained 2D Semiconductors

Two-dimensional chalcogenide semiconductors have recently emerged as a host material for quantum emitters of single photons. While several reports on defect and strain-induced single photon emission from 2D chalcogenides exist, a bottom-up, lithography-free approach to producing a high density of emitters remains elusive. Further, the physical properties of quantum emission in the case of strained 2D semiconductors are far from being understood. Here, we demonstrate a bottom-up, scalable, and lithography-free approach to creating large areas of localized emitters with high density (~150 emitters/um2) in a WSe2 monolayer. We induce strain inside the WSe2 monolayer with high spatial density by conformally placing the WSe2 monolayer over a uniform array of Pt nanoparticles with a size of 10 nm. Cryogenic, time-resolved, and gate-tunable luminescence measurements combined with near-field luminescence spectroscopy suggest the formation of localized states in strained regions that emit single photons with a high spatial density. Our approach of using a metal nanoparticle array to generate a high density of strained quantum emitters opens a new path towards scalable, tunable, and versatile quantum light sources.

cond-mat.mes-hall↗

arXiv2021

Light-Matter Coupling in Scalable Van der Waals Superlattices

Two-dimensional (2D) crystals have renewed opportunities in design and assembly of artificial lattices without the constraints of epitaxy. However, the lack of thickness control in exfoliated van der Waals (vdW) layers prevents realization of repeat units with high fidelity. Recent availability of uniform, wafer-scale samples permits engineering of both electronic and optical dispersions in stacks of disparate 2D layers with multiple repeating units. We present optical dispersion engineering in a superlattice structure comprised of alternating layers of 2D excitonic chalcogenides and dielectric insulators. By carefully designing the unit cell parameters, we demonstrate > 90 % narrowband absorption in < 4 nm active layer excitonic absorber medium at room temperature, concurrently with enhanced photoluminescence in cm2 samples. These superlattices show evidence of strong light-matter coupling and exciton-polariton formation with geometry-tunable coupling constants. Our results demonstrate proof of concept structures with engineered optical properties and pave the way for a broad class of scalable, designer optical metamaterials from atomically-thin layers.

cond-mat.mtrl-sci↗

arXiv2020

Illuminating Invisible Grain Boundaries in Coalesced Single-Orientation WS2 Monolayer Films

Engineering atomic-scale defects is crucial for realizing wafer-scale, single-crystalline transition metal dichalcogenide monolayers for electronic devices. However, connecting atomic-scale defects to larger morphologies poses a significant challenge. Using electron microscopy and atomistic simulations, we provide insights into WS2 crystal growth mechanisms, providing a direct link between synthetic conditions and the microstructure. Dark-field TEM imaging of coalesced monolayer WS2 films illuminates defect arrays that atomic-resolution STEM imaging identifies as translational grain boundaries. Imaging reveals the films to have nearly a single orientation with imperfectly stitched domains. Through atomic-resolution imaging and ReaxFF reactive force field-based molecular dynamics simulations, we observe two types of translational mismatch and discuss their atomic structures and origin. Our results indicate that the mismatch results from relatively fast growth rates. Through statistical analysis of >1300 facets, we demonstrate that the macrostructural features are constructed from nanometer-scale building blocks, describing the system across sub-Ångstrom to multi-micrometer length scales.

cond-mat.mtrl-sci↗

arXiv2020

Wafer-scale epitaxial growth of single orientation WS2 monolayers on sapphire

Realization of wafer-scale single-crystal films of transition metal dichalcogenides (TMDs) such as tungsten sulfide requires epitaxial growth and coalescence of oriented domains to form a continuous monolayer. The domains must be oriented in the same crystallographic direction on the substrate to avoid the formation of metallic inversion domain boundaries (IDBs) which are a common feature of layered chalcogenides. Here we demonstrate fully-coalesced single orientation tungsten sulfide monolayers on 2-inch diameter c-plane sapphire by metalorganic chemical vapor deposition using a multi-step growth process. High growth temperatures and sulfur/metal ratios were required to reduce domain misorientation and achieve epitaxial tungsten sulfide monolayers with low in-plane rotational twist (0.09 deg). Transmission electron microscopy analysis reveals that the tungsten sulfide monolayers lack IDBs but instead have translational boundaries that arise when tungsten sulfide domains with slightly off-set lattices merge together. By adjusting the monolayer growth rate, the density of translational boundaries and bilayer coverage were significantly reduced. The preferred orientation of domains is attributed to the presence of steps on the sapphire surface coupled with growth conditions promote surface diffusion and oriented attachment. The transferred tungsten sulfide monolayers show neutral and charged exciton emission at 80K with negligible defect-related luminescence. Back-gated tungsten sulfide field effect transistors exhibited mobility of 16 cm2/Vs. The results demonstrate the potential of achieving wafer-scale TMD monolayers free of inversion domains with properties approaching that of exfoliated flakes.

cond-mat.mtrl-sci↗

arXiv2019

Epitaxial Growth of 2D Layered Transition Metal Dichalcogenides

Transition metal dichalcogenide (TMD) monolayers and heterostructures have emerged as a compelling class of materials with transformative new science that may be harnessed for novel device technologies. These materials are commonly fabricated by exfoliation of flakes from bulk crystals, but wafer-scale epitaxy of single crystal films is required to advance the field. This article reviews the fundamental aspects of epitaxial growth of van der Waals bonded crystals specific to TMD films. The structural and electronic properties of TMD crystals are initially described along with sources and methods used for vapor phase deposition. Issues specific to TMD epitaxy are critically reviewed including substrate properties and film-substrate orientation and bonding. The current status of TMD epitaxy on different substrate types is discussed along with characterization techniques for large area epitaxial films. Future directions are proposed including developments in substrates, in situ and full wafer characterization techniques and heterostructure growth.

cond-mat.mtrl-sci↗

arXiv2018

Considerations for utilizing sodium chloride in epitaxial molybdenum disulfide

The utilization of alkali salts, such as NaCl and KI, have enabled the successful growth of large single domain and fully coalesced polycrystalline two-dimensional (2D) transition metal dichalcogenide layers. However, the impact of alkali salts on photonic and electronic properties are not fully established. In this work, we report alkali-free epitaxy of MoS2 on sapphire and benchmark the properties against alkali-assisted growth of MoS2. This study demonstrates that although NaCl can dramatically increase the domain size of monolayer MoS2 by 20 times, it can also induce strong optical and electronic heterogeneities in as-grown large-scale films. This work elucidates that utilization of NaCl can lead to variation in growth rates, loss of epitaxy, and a high density of nanoscale MoS2 particles (4/μm2). Such phenomena suggest that alkali atoms play an important role in Mo and S adatom mobility and strongly influence the 2D/sapphire interface during growth. Compared to alkali-free synthesis under the same growth conditions, MoS2 growth assisted by NaCl results in >1% tensile strain in as-grown domains, which reduces photoluminescence by ~20x and degrades transistor performance.

cond-mat.mtrl-sci↗

arXiv2016

Graphene stabilization of two-dimensional gallium nitride

The spectrum of two-dimensional (2D) materials beyond graphene offers a remarkable platform to study new phenomena in condensed matter physics. Among these materials, layered hexagonal boron nitride (hBN), with its wide bandgap energy (~5.0-6.0 eV), has clearly established that 2D nitrides are key to advancing novel devices1. A gap, however, remains between the theoretical prediction of 2D nitrides beyond hBN and experimental realization of such structures. Here we demonstrate the synthesis of 2D gallium nitride (GaN) via a novel migration-enhanced encapsulated growth (MEEG) technique utilizing epitaxial graphene. We theoretically predict and experimentally validate that the atomic structure of 2D GaN grown via MEEG is notably different from reported theory. Moreover, we establish that graphene plays a critical role in stabilizing the direct-bandgap (nearly 5.0 eV), 2D buckled structure. Our results provide a foundation for discovery and stabilization of novel 2D nitrides that are difficult to prepare via traditional synthesis.

cond-mat.mtrl-sci↗