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Results for “monolayer semiconductors”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Lineshape characterization of excitons in monolayer WS 2 by two-dimensional electronic spectroscopy

The optical properties of monolayer transition metal dichalcogenides (TMDCs), an important family of two-dimensional (2D) semiconductors for optoelectronic applications, are dominated by two excitons A (XA) and B (XB) located at K/K's valleys. The lineshape of the excitons is an indicator of the interaction of the excitons with other particles and also largely determines the performance of TMDC-based optoelectronic devices. In this work, we apply 2D electronic spectroscopy (2DES), which enables separation of the intrinsic homogeneous linewidth and the extrinsic inhomogeneous linewidth, to dissect the lineshape of XA in monolayer WS 2 . With a home-built broadband optical parametric amplifier, the 2D spectra give the exciton linewidth values for extensive ranges of excitation densities and temperatures, reflecting inter-exciton and exciton–phonon interactions. Meanwhile, the time-domain evolution of the lineshape reveals a similar rate of spectral diffusion to that in quantum wells (QWs) based on III–V semiconductors.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Strong optical response and light emission from a monolayer molecular crystal

Excitons in two-dimensional (2D) materials are tightly bound and exhibit rich physics. So far, the optical excitations in 2D semiconductors are dominated by Wannier-Mott excitons, but molecular systems can host Frenkel excitons (FE) with unique properties. Here, we report a strong optical response in a class of monolayer molecular J-aggregates. The exciton exhibits giant oscillator strength and absorption (over 30% for monolayer) at resonance, as well as photoluminescence quantum yield in the range of 60-100%. We observe evidence of superradiance (including increased oscillator strength, bathochromic shift, reduced linewidth and lifetime) at room-temperature and more progressively towards low temperature. These unique properties only exist in monolayer owing to the large unscreened dipole interactions and suppression of charge-transfer processes. Finally, we demonstrate light-emitting devices with the monolayer J-aggregate. The intrinsic device speed could be beyond 30 GHz, which is promising for next-generation ultrafast on-chip optical communications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Hybrid Heterostructures to Generate Long-Lived and Mobile Photocarriers in Graphene

We report the generation of long-lived and highly mobile photocarriers in hybrid van der Waals heterostructures that are formed by monolayer graphene, few-layer transition metal dichalcogenides, and the organic semiconductor F 8 ZnPc. Samples are fabricated by dry transfer of mechanically exfoliated MoS 2 or WS 2 few-layer flakes on a graphene film, followed by deposition of F 8 ZnPc. Transient absorption microscopy measurements are performed to study the photocarrier dynamics. In heterostructures of F 8 ZnPc/few-layer-MoS 2 /graphene, electrons excited in F 8 ZnPc can transfer to graphene and thus be separated from the holes that reside in F 8 ZnPc. By increasing the thickness of MoS 2 , these electrons acquire long recombination lifetimes of over 100 ps and a high mobility of 2800 cm 2 V–1 s –1 . Graphene doping with mobile holes is also demonstrated with WS 2 as the middle layers. Furthermore, these artificial heterostructures can improve the performance of graphene-based optoelectronic devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Spatial Control of Substitutional Dopants in Hexagonal Monolayer WS 2 : The Effect of Edge Termination

The ability to control the density and spatial distribution of substitutional dopants in semiconductors is crucial for achieving desired physicochemical properties. Substitutional doping with adjustable doping levels has been previously demonstrated in 2D transition metal dichalcogenides (TMDs); however, the spatial control of dopant distribution remains an open field. In this work, edge termination is demonstrated as an important characteristic of 2D TMD monocrystals that affects the distribution of substitutional dopants. Particularly, in chemical vapor deposition (CVD)-grown monolayer WS 2 , it is found that a higher density of transition metal dopants is always incorporated in sulfur-terminated domains when compared to tungsten-terminated domains. Here two representative examples demonstrate this spatial distribution control, including hexagonal iron- and vanadium-doped WS 2 monolayers. Density functional theory (DFT) calculations are further performed, indicating that the edge-dependent dopant distribution is due to a strong binding of tungsten atoms at tungsten-zigzag edges, resulting in the formation of open sites at sulfur-zigzag edges that enable preferential dopant incorporation. Based on these results, it is envisioned that edge termination in crystalline TMD monolayers can be utilized as a novel and effective knob for engineering the spatial distribution of substitutional dopants, leading to in-plane hetero-/multi-junctions that display fascinating electronic, optoelectronic, and magnetic properties.

2D transition metal dichalcogenides↗
DOE OSTI2020

Anomalous Behavior of 2D Janus Excitonic Layers under Extreme Pressures

Newly discovered 2D Janus transition metal dichalcogenides layers have gained much attention from a theory perspective owing to their unique atomic structure and exotic materials properties, but little to no experimental data are available on these materials. Here, experimental and theoretical studies establish the vibrational and optical behavior of 2D Janus S–W–Se and S–Mo–Se monolayers under high pressures for the first time. Chemical vapor deposition (CVD)-grown classical transition metal dichalcogenides (TMD) monolayers are first transferred onto van der Waals (vdW) mica substrates and converted to 2D Janus sheets by surface plasma technique, and then integrated into a 500 µm size diamond anvil cell for high-pressure studies. Overall, the results show that 2D Janus layers do not undergo phase transition up to 15 GPa, and in this pressure regime, their vibrational modes exhibit a nonmonotonic response to the applied pressures (dω/dP). Interestingly, these 2D Janus monolayers exhibit unique blueshift in photoluminescence (PL) upon compression, which is in contrast to many other traditional semiconductor materials. Overall theoretical simulations offer in-depth insights and reveal that the overall optical response is a result of competition between the ab-plane (blueshift) and c-axis (redshift) compression. The overall findings shed the very first light on how 2D Janus monolayers respond under extreme pressures and expand the fundamental understanding of these materials.

2D Janus monolayers↗
DOE OSTI2026

Space-Charge-Limited van der Waals Spin Transistor

Integrating semiconducting and magnetic materials could combine transistorlike operation with nonvolatility and enable architectures such as logic in memory. Here, in this work, we employ correlated electrical transport and scanning nitrogen-vacancy center magnetic imaging to elucidate a spin transistor concept that amalgamates vertical and lateral hopping transport inside a 2D antiferromagnetic semiconductor, mechanistically distinct from vertical tunneling devices. Our device, based on a monolayer-bilayer junction in CrSBr, displays giant, gate-tunable magnetoresistance driven by the dual action of electrostatic doping on space-charge-limited lateral conduction and interlayer exchange coupling. Moreover, we visualize a field-trainable, layer-sharing effect that selects between coherent or domain-wall reversal at the spin-flip transition, enabling multilevel, memristive conductance states. Our layer-dependent space charge mechanism for convergent electrical and magnetic control opens opportunities to address limitations in contemporary computing.

2-dimensional systems↗
DOE OSTI2023

Transition Metal Dichalcogenides: Making Atomic‐Level Magnetism Tunable with Light at Room Temperature

Abstract The capacity to manipulate magnetization in 2D dilute magnetic semiconductors (2D‐DMSs) using light, specifically in magnetically doped transition metal dichalcogenide (TMD) monolayers ( M ‐doped TX 2 , where M = V, Fe, and Cr; T = W, Mo; X = S, Se, and Te), may lead to innovative applications in spintronics, spin‐caloritronics, valleytronics, and quantum computation. This Perspective paper explores the mediation of magnetization by light under ambient conditions in 2D‐TMD DMSs and heterostructures. By combining magneto‐LC resonance (MLCR) experiments with density functional theory (DFT) calculations, we show that the magnetization can be enhanced using light in V‐doped TMD monolayers (e.g., V‐WS 2 , V‐WSe 2 ). This phenomenon is attributed to excess holes in the conduction and valence bands, and carriers trapped in magnetic doping states, mediating the magnetization of the semiconducting layer. In 2D‐TMD heterostructures (VSe 2 /WS 2 , VSe 2 /MoS 2 ), the significance of proximity, charge‐transfer, and confinement effects in amplifying light‐mediated magnetism is demonstrated. We attributed this to photon absorption at the TMD layer that generates electron–hole pairs mediating the magnetization of the heterostructure. These findings will encourage further research in the field of 2D magnetism and establish a novel design of 2D‐TMDs and heterostructures with optically tunable magnetic functionalities, paving the way for next‐generation magneto‐optic nanodevices.

36 MATERIALS SCIENCE↗
DOE OSTI2021

van der Waals Epitaxy Growth of Bi 2 Se 3 on a Freestanding Monolayer Graphene Membrane: Implications for Layered Materials and Heterostructures

Research on two-dimensional and layered materials has expanded over the past 2 decades because of their unique properties and application potential. The key hurdles in realizing this potential are the challenges in controlling their atomic structure and their incompatibility with existing semiconductor nanofabrication techniques. Here we report on high-quality van der Waals epitaxial growth and characterization of a layered topological insulator on freestanding monolayer graphene transferred to different mechanical supports. This “templated” synthesis approach enables direct interrogation of the interfacial atomic structure of the as-grown materials and opens a route toward creating device structures with more traditional semiconductor nanofabrication techniques.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Dark-exciton energy splitting in monolayer W Se 2 : Insights from time-dependent density functional theory

Here, we present here a formalism based on time-dependent density functional theory to describe characteristics of both intra- and intervalley excitons in semiconductors, the latter of which had remained a challenge. Through the usage of an appropriate exchange-correlation kernel (nanoquanta), we trace the energy difference between the intra- and intervalley dark excitons in monolayer (1L) W⁢ Se 2 to the domination of the exchange part in the exchange-correlation energies of these states. Furthermore, our calculated transition contribution maps establish the momentum resolved weights of the electron-hole excitations in both bright and dark excitons thereby providing a comprehensive understanding of excitonic properties of 1L W⁢ Se 2 . We find that the states consist of hybridized excitations around the corresponding valleys which leads to brightening of the dark excitons, i.e., significantly decreasing their lifetime which is reflected in the PL spectrum. Using many-body perturbation theory, we calculate the phonon contribution to the energy band gap and the linewidths of the excited electrons, holes, and (bright) exciton to find that as the temperature increases the band gap significantly decreases, while the linewidths increase. Our work paves for describing the ultrafast charge dynamics of transition metal dichalcogenide within an ab initio framework.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Spectra-Orthogonal Optical Anisotropy in Wafer-Scale Molecular Crystal Monolayers

Controlling the spectral and polarization response of two-dimensional (2D) crystals is vital for developing ultrathin platforms for compact optoelectronic devices. However, independently tuning optical anisotropy and spectral response remains challenging in conventional semiconductors due to the intertwined nature of their lattice and electronic structures. Here, we report spectra-orthogonal optical anisotropy─where polarization anisotropy is tuned independently of spectral response─in wafer-scale, one-atom-thick 2D molecular crystal (2DMC) monolayers synthesized on monolayer transition-metal dichalcogenide (TMD) crystals. Utilizing the concomitant spectral consistency and structural tunability of perylene derivatives, we demonstrate tunable optical polarization anisotropy in 2DMCs with similar spectral profiles, as confirmed by room-temperature scanning tunneling microscopy and cross-polarized reflectance microscopy. Additional angle-dependent analysis of the single-crystal and polycrystalline molecular domains reveals an epitaxial relationship between the 2DMC and TMD. In conclusion, our results establish a scalable, molecule-based 2D crystalline platform for unique and tunable functionalities unattainable in covalent 2D solids.

2D materials↗
DOE OSTI2025

Evolution of the Electronic Gap of Directly Synthesized Versus Mechanically Transferred WS 2 Monolayer to Multilayer Films

The electronic properties of 2D materials play a critical role in determining their potential for device applications. Despite rapid developments in 2D semiconductors, studies of fundamental electronic parameters, including the electronic gap and ionization energy, are limited, with significant discrepancies in reported values. The study focuses on tungsten disulfide (WS₂) and investigates the electronic structure of films comprising an increasing number of layers deposited with two different methods: direct synthesis via metal–organic chemical vapor deposition (MOCVD) and additive mechanical transfer of exfoliated single layers. The films are characterized via Raman, UV–vis, and photoluminescence spectroscopies, as well as ultraviolet photoelectron and inverse photoemission spectroscopies (UPS/IPES). The electronic gap of WS₂ is found to decrease from 2.43 eV for the monolayer to 1.97 eV for the trilayer, indicating a bulk transition at the trilayer thickness. This reduction in the electronic gap is primarily due to the downward shift of the conduction band minimum relative to the valence band maximum. A comparative analysis with MOCVD-grown WS₂ reveals a slightly larger electronic gap for MOCVD-grown samples, attributed to differences in defect densities. The electronic levels evaluated through UPS/IPES highlight the significant influence of preparation methods on the electronic properties of WS₂.

2D materials↗
DOE OSTI2023

Theory of glide symmetry protected helical edge states in a WTe 2 monolayer

Helical edge states in quantum spin Hall (QSH) materials are central building blocks of topological matter design and engineering. Despite their principal topological protection against elastic backscattering, the level of operational stability depends on manifold parameters such as the band gap of the given semiconductor system in the “inverted” regime, temperature, disorder, and crystal orientation. Here, we theoretically investigate electronic and transport properties of QSH edge states in large gap 1-T' WTe 2 monolayers. We explore the impact of edge termination, disorder, temperature, and interactions on experimentally addressable edge state observables, such as local density of states and conductance. We show that conductance quantization can remain surprisingly robust even for heavily disordered samples because of an anomalously small edge state decay length and additional protection related to the large direct gap allowed by glide symmetry. From the simulation of temperature-dependent resistance, we find that moderate disorder enhances the stability of conductance by localizing bulk states. We evaluate the edge state velocity and Luttinger liquid parameter as functions of the chemical potential, finding prospects for physics beyond linear helical Luttinger liquids in samples with ultraclean and well-defined edges.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Beam steering at the nanosecond time scale with an atomically thin reflector

Techniques to mold the flow of light on subwavelength scales enable fundamentally new optical systems and device applications. The realization of programmable, active optical systems with fast, tunable components is among the outstanding challenges in the field. Here, we experimentally demonstrate a few-pixel beam steering device based on electrostatic gate control of excitons in an atomically thin semiconductor with strong light-matter interactions. By combining the high reflectivity of a MoSe 2 monolayer with a graphene split-gate geometry, we shape the wavefront phase profile to achieve continuously tunable beam deflection with a range of 10°, two-dimensional beam steering, and switching times down to 1.6 nanoseconds. Our approach opens the door for a new class of atomically thin optical systems, such as rapidly switchable beam arrays and quantum metasurfaces operating at their fundamental thickness limit.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Enhanced van der Waals epitaxy of germanium by out-of-plane dipole moment induced from transferred graphene on TiN/AlN multilayers

We report recent advances in 3D/2D heterostructures have opened up tremendous opportunities in building highly flexible and durable optoelectronic devices. However, the inherit lack of interfacial bonding and low surface energy of van der Waals surfaces limit the nucleation and growth of 3D materials. Enhancing wettability by providing a porous buffer is effective in growing compound semiconductors on graphene while van der Waals epitaxy of Ge remains challenging. Here, the nucleation of Ge has been significantly improved from an islanded mode to granular modes by using a TiN/AlN multilayered buffer prior to Ge/graphene integration. Highly textured Ge growth with dominating (111), (220), and (311) peaks are identified by x-ray diffraction. The microstructure of the buffer TiN/AlN demonstrates a polycrystalline quality with clean interfaces between each interlayer and the substrate. Kelvin probe force microscopy measurements along the lateral TiN/AlN interface identify a potential drop corresponding to the AlN phase. This contact potential difference between TiN and AlN is the key in generating the out-of-plane dipole moment that modifies the surface energy of the monolayer graphene, resulting in enhanced wettability of the Ge adatoms nucleated on top. Surface dipole induced nucleation of 3D semiconductor thin films on 2D materials via the proper design of buffer layer is fundamentally important to enhance the 3D/2D growth toward flexible optoelectronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Phonon Screening of Excitons in Atomically Thin Semiconductors

Atomically thin semiconductors, encompassing both 2D materials and quantum wells, exhibit a pronounced enhancement of excitonic effects due to geometric confinement. Consequently, these materials have become foundational platforms for the exploration and utilization of excitons. Recent ab initio studies have demonstrated that phonons can substantially screen electron-hole interactions in bulk semiconductors and strongly modify the properties of excitons. While excitonic properties of atomically thin semiconductors have been the subject of extensive theoretical investigations, the role of phonon screening on excitons in atomically thin structures remains unexplored. In this Letter, we demonstrate via ab initio GW-Bethe-Salpeter equation calculations that phonon screening can have a significant impact on optical excitations in atomically thin semiconductors. We further show that the degree of phonon screening can be tuned by structural engineering. We focus on atomically thin GaN quantum wells embedded in AlN and identify specific phonons in the surrounding material, AlN, that dramatically alter the lowest-lying exciton in monolayer GaN via screening. Our studies provide new intuition beyond standard models into the interplay among structural properties, phonon characteristics, and exciton properties in atomically thin semiconductors, and have implications for future experiments.

2-dimensional systems↗
DOE OSTI2020

Control of magnetic properties of MnBi 2 Te 4 using a van der Waals ferroelectric III 2 -VI 3 film and biaxial strain

Using the first-principles calculations, we systematically investigated magnetic properties of a MnBi 2 Te 4 (MBT) monolayer in contact with III 2 -VI 3 two-dimensional ferroelectric substrates. As the electric polarization in the ferroelectric films is switched, a semiconductor to half-metal transition occurs in MBT, and its magnetic easy axis in several cases reorients. As an example, the Curie temperature of MBT/In 2 Se 3 can be enhanced to 21.5 or 32 K under the influence of electric polarization and biaxial strain, much higher than that of the pristine MBT monolayer, which is 14.5 K in our calculations. Our results in this work suggest effective ways to tune magnetic properties of MBT and provide useful insights for the further development of these important van der Waals functional materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

In Situ Attenuated Total Reflectance Infrared Spectroelectrochemistry (ATR-IR-SEC) for the Characterization of Molecular Redox Processes on Surface-Proximal Doped Silicon ATR Crystal Working Electrodes

In situ mid-infrared spectroscopy is a powerful technique for understanding the mechanism of CO 2 reduction (CO 2 R) catalysts because it enables the direct detection of catalytic intermediates and products. Moreover, spectroelectrochemistry (SEC), the coupling of spectroscopy with electrochemistry, allows spectroscopic changes to be correlated with applied potentials to reveal potential-dependent intermediates that are often relevant to photoelectrochemical reactions. Hybrid photoelectrodes, comprised of a narrow bandgap semiconductor, like silicon (Si), with a covalently-linked molecular catalyst, are a promising platform for sunlight-driven catalysis, but characterization of the catalytic mechanism(s) is challenging under photoelectrochemical conditions, particularly when the catalyst is present in monolayer or less concentrations. Here, we have developed a new strategy to use multiple-reflection attenuated total reflectance IR spectroscopy (ATR-IR) coupled with electrochemistry to characterize catalysts directly integrated with a semiconductor surface under applied potential. We show that by surface-proximal n-type or p-type doping of the top ~100-200 nm of the crystal surface, Si ATR crystals can be used simultaneously as the internal reflection element and semiconductor working electrode for ATR-IR-SEC measurements. The surface-proximal doping strategy yields a quasi-equipotential surface with excellent infrared transparency that would have been compromised by free carrier absorption if the crystal was uniformly doped. This approach permits the catalytically-active functionalized surface to be directly probed without modification and overcomes signal-to-noise limitations of other strategies that use separately deposited working electrodes on Si ATR crystals. Proof-of-concept ATR-IR-SEC spectra were collected during the reduction and oxidation of monolayers of Re- and Ru-based transition metal carbonyl complexes, respectively, verifying the viability of the technique to probe redox processes associated with CO 2 R catalysts on Si electrode surfaces with high sensitivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Quasiparticle electronic structure of phthalocyanine:TMD interfaces from first-principles GW

Interfaces formed between monolayer transition metal dichalcogenides and (metallo)phthalocyanine molecules are promising in energy applications and provide a platform for studying mixed-dimensional molecule-semiconductor heterostructures in general. An accurate characterization of the frontier energy level alignment at these interfaces is key in the fundamental understanding of the charge transfer dynamics between the two photon absorbers. Here, we employ the first-principles substrate screening GW approach to quantitatively characterize the quasiparticle electronic structure of a series of interfaces: metal-free phthalocyanine (H 2 Pc) adsorbed on monolayer MX 2 (M = Mo, W; X = S, Se) and zinc phthalocyanine (ZnPc) adsorbed on MoX 2 (X = S, Se). Furthermore, we reveal the dielectric screening effect of the commonly used α-quartz (SiO 2 ) substrate on the H 2 Pc:MoS 2 interface using the dielectric embedding GW approach. Our calculations furnish a systematic set of GW results for these interfaces, providing the structure–property relationship across a series of similar systems and benchmarks for future experimental and theoretical studies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗