Electrical spectroscopy of defect states and their hybridization in monolayer MoS2.

Defects in solids are unavoidable and can create complex electronic states that can significantly influence the electrical and optical properties of semiconductors. With the rapid progress in the integration of 2D semiconductors in practical devices, it is imperative to understand and characterize the influence of defects in this class of materials. Here, we examine the electrical response of defect filling and emission using deep level transient spectroscopy (DLTS) and reveal defect states and their hybridization in a monolayer MOCVD-grown material deposited on CMOS-compatible substrates. Supported by aberration-corrected STEM imaging and theoretical calculations, we find that neighboring sulfur vacancy pairs introduce additional shallow trap states via hybridization of individual vacancy levels. Even though such vacancy pairs only represent ~10% of the total defect concentration, they can have a substantial influence on the off currents and switching slopes of field-effect transistors based on 2D semiconductors. Our technique, which can quantify the energy states of different defects and their interactions, allows rapid and nondestructive electrical characterization of defect states important for the defect engineering of 2D semiconductors.

Disorder-induced bulk photovoltaic effect in a centrosymmetric van der Waals material.

Sunlight is widely seen as one of the most abundant forms of renewable energy, with photovoltaic cells based on pn junctions being the most commonly used platform attempting to harness it. Unlike in conventional photovoltaic cells, the bulk photovoltaic effect (BPVE) allows for the generation of photocurrent and photovoltage in a single material without the need to engineer a pn junction and create a built-in electric field, thus offering a solution that can potentially exceed the Shockley-Queisser efficiency limit. However, it requires a material with no inversion symmetry and is therefore absent in centrosymmetric materials. Here, we demonstrate that breaking the inversion symmetry by structural disorder can induce BPVE in ultrathin PtSe2, a centrosymmetric semiconducting van der Waals material. Homogenous illumination of defective PtSe2 by linearly and circularly polarized light results in a photoresponse termed as linear photogalvanic effect (LPGE) and circular photogalvanic effect (CPGE), which is mostly absent in the pristine crystal. First-principles calculations reveal that LPGE originates from Se vacancies that act as asymmetric scattering centers for the photo-generated electron-hole pairs. Our work emphasizes the importance of defects to induce photovoltaic functionality in centrosymmetric materials and shows how the range of materials suitable for light sensing and energy-harvesting applications can be extended.

Room-temperature electrical control of polarization and emission angle in a cavity-integrated 2D pulsed LED.

Devices based on two-dimensional (2D) semiconductors hold promise for the realization of compact and versatile on-chip interconnects between electrical and optical signals. Although light emitting diodes (LEDs) are fundamental building blocks for integrated photonics, the fabrication of light sources made of bulk materials on complementary metal-oxide-semiconductor (CMOS) circuits is challenging. While LEDs based on van der Waals heterostructures have been realized, the control of the emission properties necessary for information processing remains limited. Here, we show room-temperature electrical control of the location, directionality and polarization of light emitted from a 2D LED operating at MHz frequencies. We integrate the LED in a planar cavity to couple the polariton emission angle and polarization to the in-plane exciton momentum, controlled by a lateral voltage. These findings demonstrate the potential of TMDCs as fast, compact and tunable light sources, promising for the realization of electrically driven polariton lasers.

Engineering Optically Active Defects in Hexagonal Boron Nitride Using Focused Ion Beam and Water.

Hexagonal boron nitride (hBN) has emerged as a promising material platform for nanophotonics and quantum sensing, hosting optically active defects with exceptional properties such as high brightness and large spectral tuning. However, precise control over deterministic spatial positioning of emitters in hBN remained elusive for a long time, limiting their proper correlative characterization and applications in hybrid devices. Recently, focused ion beam (FIB) systems proved to be useful to engineer several types of spatially defined emitters with various structural and photophysical properties. Here we systematically explore the physical processes leading to the creation of optically active defects in hBN using FIB and find that beam-substrate interaction plays a key role in the formation of defects. These findings are confirmed using transmission electron microscopy, which reveals local mechanical deterioration of the hBN layers and local amorphization of ion beam irradiated hBN. Additionally, we show that, upon exposure to water, amorphized hBN undergoes a structural and optical transition between two defect types with distinctive emission properties. Moreover, using super-resolution optical microscopy combined with atomic force microscopy, we pinpoint the exact location of emitters within the defect sites, confirming the role of defected edges as primary sources of fluorescent emission. This lays the foundation for FIB-assisted engineering of optically active defects in hBN with high spatial and spectral control for applications ranging from integrated photonics, to nanoscale sensing, and to nanofluidics.

Superconducting 2D NbS2 Grown Epitaxially by Chemical Vapor Deposition.

Metallic two-dimensional (2D) transition metal dichalcogenides (TMDCs) are attracting great attention because of their interesting low-temperature properties such as superconductivity, magnetism, and charge density waves (CDW). However, further studies and practical applications are being slowed down by difficulties in synthesizing high-quality materials with a large grain size and well-determined thickness. In this work, we demonstrate epitaxial chemical vapor deposition (CVD) growth of 2D NbS2 crystals on a sapphire substrate, with a thickness-dependent structural phase transition. NbS2 crystals are epitaxially aligned by the underlying c-plane sapphire resulting in high-quality growth. The thickness of NbS2 is well controlled by growth parameters to be between 1.5 and 10 nm with a large grain size of up to 500 µm. As the thickness increases, we observe in our NbS2 a transition from a metallic 3R-polytype to a superconducting 2H-polytype, confirmed by Raman spectroscopy, aberration-corrected scanning transmission electron microscopy (STEM) and electrical transport measurements. A Berezinskii-Kosterlitz-Thouless (BKT) superconducting transition occurs in the CVD-grown 2H-phase NbS2 below the transition temperature (Tc) of 3 K. Our work demonstrates thickness and phase-controllable synthesis of high-quality superconducting 2D NbS2, which is imperative for its practical applications in next-generation TMDC-based electrical devices.

Observation of Thermal Spin-Orbit Torque in W/CoFeB/MgO Structures.

Coupling of spin and heat currents enables the spin Nernst effect, the thermal generation of spin currents in nonmagnets that have strong spin-orbit interaction. Analogous to the spin Hall effect that electrically generates spin currents and associated electrical spin-orbit torques (SOTs), the spin Nernst effect can exert thermal SOTs on an adjacent magnetic layer and control the magnetization direction. Here, the thermal SOT caused by the spin Nernst effect is experimentally demonstrated in W/CoFeB/MgO structures. It is found that an in-plane temperature gradient across the sample generates a magnetic torque and modulates the switching field of the perpendicularly magnetized CoFeB. The W thickness dependence suggests that the torque originates mainly from thermal spin currents induced in W. Moreover, the thermal SOT reduces the critical current for SOT-induced magnetization switching, demonstrating that it can be utilized to control the magnetization in spintronic devices.

Probing magnetism in atomically thin semiconducting PtSe2.

Atomic-scale disorder in two-dimensional transition metal dichalcogenides is often accompanied by local magnetic moments, which can conceivably induce long-range magnetic ordering into intrinsically non-magnetic materials. Here, we demonstrate the signature of long-range magnetic orderings in defective mono- and bi-layer semiconducting PtSe2 by performing magnetoresistance measurements under both lateral and vertical measurement configurations. As the material is thinned down from bi- to mono-layer thickness, we observe a ferromagnetic-to-antiferromagnetic crossover, a behavior which is opposite to the one observed in the prototypical 2D magnet CrI3. Our first-principles calculations, supported by aberration-corrected transmission electron microscopy imaging of point defects, associate this transition to the interplay between the defect-induced magnetism and the interlayer interactions in PtSe2. Furthermore, we show that graphene can be effectively used to probe the magnetization of adjacent semiconducting PtSe2. Our findings in an ultimately scaled monolayer system lay the foundation for atom-by-atom engineering of magnetism in otherwise non-magnetic 2D materials.