Approaching the quantum limit in two-dimensional semiconductor contacts.

The development of next-generation electronics requires scaling of channel material thickness down to the two-dimensional limit while maintaining ultralow contact resistance1,2. Transition-metal dichalcogenides can sustain transistor scaling to the end of roadmap, but despite a myriad of efforts, the device performance remains contact-limited3-12. In particular, the contact resistance has not surpassed that of covalently bonded metal-semiconductor junctions owing to the intrinsic van der Waals gap, and the best contact technologies are facing stability issues3,7. Here we push the electrical contact of monolayer molybdenum disulfide close to the quantum limit by hybridization of energy bands with semi-metallic antimony ([Formula: see text]) through strong van der Waals interactions. The contacts exhibit a low contact resistance of 42 ohm micrometres and excellent stability at 125 degrees Celsius. Owing to improved contacts, short-channel molybdenum disulfide transistors show current saturation under one-volt drain bias with an on-state current of 1.23 milliamperes per micrometre, an on/off ratio over 108 and an intrinsic delay of 74 femtoseconds. These performances outperformed equivalent silicon complementary metal-oxide-semiconductor technologies and satisfied the 2028 roadmap target. We further fabricate large-area device arrays and demonstrate low variability in contact resistance, threshold voltage, subthreshold swing, on/off ratio, on-state current and transconductance13. The excellent electrical performance, stability and variability make antimony ([Formula: see text]) a promising contact technology for transition-metal-dichalcogenide-based electronics beyond silicon.

How Do Quantum Effects Influence the Capacitance and Carrier Density of Monolayer MoS2 Transistors?

When transistor gate insulators have nanometer-scale equivalent oxide thickness (EOT), the gate capacitance (CG) becomes smaller than the oxide capacitance (Cox) due to the quantum capacitance and charge centroid capacitance of the channel. Here, we study the capacitance of monolayer MoS2 as a prototypical two-dimensional (2D) channel while considering spatial variations in the potential, charge density, and density of states. At 0.5 nm EOT, the monolayer MoS2 capacitance is smaller than its quantum capacitance, limiting the single-gated CG of an n-type channel to between 63% and 78% of Cox, for gate overdrive voltages between 0.5 and 1 V. Despite these limitations, for dual-gated devices, the on-state CG of monolayer MoS2 is 50% greater than that of silicon at 0.5 nm EOT and more than three times that of InGaAs at 1 nm EOT, indicating that such 2D semiconductors are promising for improved gate control of nanoscale transistors at future technology nodes.

Ambipolar Thickness-Dependent Thermoelectric Measurements of WSe2.

Thermoelectric materials can harvest electrical energy from temperature gradients, and could play a role as power supplies for sensors and other devices. Here, we characterize fundamental in-plane electrical and thermoelectric properties of layered WSe2 over a range of thicknesses, from 10 to 96 nm, between 300 and 400 K. The devices are electrostatically gated with an ion gel, enabling us to probe both electron and hole regimes over a large range of carrier densities. We extract the highest n- and p-type Seebeck coefficients for thin-film WSe2, -500 and 950 µV/K respectively, reported to date at room temperature. We also emphasize the importance of low substrate thermal conductivity on such lateral thermoelectric measurements, improving this platform for future studies on other nanomaterials.

Probing the Melting Transitions in Phase-Change Superlattices via Thin Film Nanocalorimetry.

Phase-change superlattices with nanometer thin sublayers are promising for low-power phase-change memory (PCM) on rigid and flexible platforms. However, the thermodynamics of the phase transition in such nanoscale superlattices remain unexplored, especially at ultrafast scanning rates, which is crucial for our fundamental understanding of superlattice-based PCM. Here, we probe the phase transition of Sb2Te3 (ST)/Ge2Sb2Te5 (GST) superlattices using nanocalorimetry with a monolayer sensitivity (∼1 Å) and a fast scanning rate (105 K/s). For a 2/1.8 nm/nm Sb2Te3/GST superlattice, we observe an endothermic melting transition with an ∼240 °C decrease in temperature and an ∼8-fold decrease in enthalpy compared to those for the melting of GST, providing key thermodynamic insights into the low-power switching of superlattice-based PCM. Nanocalorimetry measurements for Sb2Te3 alone demonstrate an intrinsic premelting similar to the unique phase transition of superlattices, thus revealing a critical role of the Sb2Te3 sublayer within our superlattices. These results advance our understanding of superlattices for energy-efficient data storage and computing.

Strain-Enhanced Mobility of Monolayer MoS2.

Strain engineering is an important method for tuning the properties of semiconductors and has been used to improve the mobility of silicon transistors for several decades. Recently, theoretical studies have predicted that strain can also improve the mobility of two-dimensional (2D) semiconductors, e.g., by reducing intervalley scattering or lowering effective masses. Here, we experimentally show strain-enhanced electron mobility in monolayer MoS2 transistors with uniaxial tensile strain, on flexible substrates. The on-state current and mobility are nearly doubled with tensile strain up to 0.7%, and devices return to their initial state after release of the strain. We also show a gate-voltage-dependent gauge factor up to 200 for monolayer MoS2, which is higher than previous values reported for sub-1 nm thin piezoresistive films. These results demonstrate the importance of strain engineering 2D semiconductors for performance enhancements in integrated circuits, or for applications such as flexible strain sensors.

Fast-Response Flexible Temperature Sensors with Atomically Thin Molybdenum Disulfide.

Real-time thermal sensing on flexible substrates could enable a plethora of new applications. However, achieving fast, sub-millisecond response times even in a single sensor is difficult, due to the thermal mass of the sensor and encapsulation. Here, we fabricate flexible monolayer molybdenum disulfide (MoS2) temperature sensors and arrays, which can detect temperature changes within a few microseconds, over 100× faster than flexible thin-film metal sensors. Thermal simulations indicate the sensors' response time is only limited by the MoS2 interfaces and encapsulation. The sensors also have high temperature coefficient of resistance, ∼1-2%/K and stable operation upon cycling and long-term measurement when they are encapsulated with alumina. These results, together with their biocompatibility, make these devices excellent candidates for biomedical sensor arrays and many other Internet of Things applications.

Unveiling the Effect of Superlattice Interfaces and Intermixing on Phase Change Memory Performance.

Superlattice (SL) phase change materials have shown promise to reduce the switching current and resistance drift of phase change memory (PCM). However, the effects of internal SL interfaces and intermixing on PCM performance remain unexplored, although these are essential to understand and ensure reliable memory operation. Here, using nanometer-thin layers of Ge2Sb2Te5 and Sb2Te3 in SL-PCM, we uncover that both switching current density (Jreset) and resistance drift coefficient (v) decrease as the SL period thickness is reduced (i.e., higher interface density); however, interface intermixing within the SL increases both. The signatures of distinct versus intermixed interfaces also show up in transmission electron microscopy, X-ray diffraction, and thermal conductivity measurements of our SL films. Combining the lessons learned, we simultaneously achieve low Jreset ≈ 3-4 MA/cm2 and ultralow v ≈ 0.002 in mushroom-cell SL-PCM with ∼110 nm bottom contact diameter, thus advancing SL-PCM technology for high-density storage and neuromorphic applications.

Uncovering Thermal and Electrical Properties of Sb2Te3/GeTe Superlattice Films.

Superlattice-like phase change memory (SL-PCM) promises lower switching current than conventional PCM based on Ge2Sb2Te5 (GST); however, a fundamental understanding of SL-PCM requires detailed characterization of the interfaces within such an SL. Here we explore the electrical and thermal transport of SLs with deposited Sb2Te3 and GeTe alternating layers of various thicknesses. We find up to an approximately four-fold reduction of the effective cross-plane thermal conductivity of the SL stack (as-deposited polycrystalline) compared with polycrystalline GST (as-deposited amorphous and later annealed) due to the thermal interface resistances within the SL. Thermal measurements with varying periods of our SLs show a signature of phonon coherence with a transition from wave-like to particle-like phonon transport, further described by our modeling. Electrical resistivity measurements of such SLs reveal strong anisotropy (∼2000×) between the in-plane and cross-plane directions due to the weakly interacting van der Waals-like gaps. This work uncovers electrothermal transport in SLs based on Sb2Te3 and GeTe for the improved design of low-power PCM.

Dynamic Hybrid Metasurfaces.

Efficient hybrid plasmonic-photonic metasurfaces that simultaneously take advantage of the potential of both pure metallic and all-dielectric nanoantennas are identified as an emerging technology in flat optics. Nevertheless, postfabrication tunable hybrid metasurfaces are still elusive. Here, we present a reconfigurable hybrid metasurface platform by incorporating the phase-change material Ge2Sb2Te5 (GST) into metal-dielectric meta-atoms for active and nonvolatile tuning of properties of light. We systematically design a reduced-dimension meta-atom, which selectively controls the hybrid plasmonic-photonic resonances of the metasurface via the dynamic change of optical constants of GST without compromising the scattering efficiency. As a proof-of-concept, we experimentally demonstrate two tunable metasurfaces that control the amplitude (with relative modulation depth as high as ≈80%) or phase (with tunability >230°) of incident light promising for high-contrast optical switching and efficient anomalous to specular beam deflection, respectively. Our findings further substantiate dynamic hybrid metasurfaces as compelling candidates for next-generation reprogrammable meta-optics.

High-Performance p-n Junction Transition Metal Dichalcogenide Photovoltaic Cells Enabled by MoOx Doping and Passivation.

Layered semiconducting transition metal dichalcogenides (TMDs) are promising materials for high-specific-power photovoltaics due to their excellent optoelectronic properties. However, in practice, contacts to TMDs have poor charge carrier selectivity, while imperfect surfaces cause recombination, leading to a low open-circuit voltage (VOC) and therefore limited power conversion efficiency (PCE) in TMD photovoltaics. Here, we simultaneously address these fundamental issues with a simple MoOx (x ≈ 3) surface charge-transfer doping and passivation method, applying it to multilayer tungsten disulfide (WS2) Schottky-junction solar cells with initially near-zero VOC. Doping and passivation turn these into lateral p-n junction photovoltaic cells with a record VOC of 681 mV under AM 1.5G illumination, the highest among all p-n junction TMD solar cells with a practical design. The enhanced VOC also leads to record PCE in ultrathin (<90 nm) WS2 photovoltaics. This easily scalable doping and passivation scheme is expected to enable further advances in TMD electronics and optoelectronics.

Tuning electrical and interfacial thermal properties of bilayer MoS2via electrochemical intercalation.

Layered two-dimensional (2D) materials such as MoS2have attracted much attention for nano- and opto-electronics. Recently, intercalation (e.g. of ions, atoms, or molecules) has emerged as an effective technique to modulate material properties of such layered 2D films reversibly. We probe both the electrical and thermal properties of Li-intercalated bilayer MoS2nanosheets by combining electrical measurements and Raman spectroscopy. We demonstrate reversible modulation of carrier density over more than two orders of magnitude (from 0.8 × 1012to 1.5 × 1014cm-2), and we simultaneously obtain the thermal boundary conductance between the bilayer and its supporting SiO2substrate for an intercalated system for the first time. This thermal coupling can be reversibly modulated by nearly a factor of eight, from 14 ± 4.0 MW m-2K-1before intercalation to 1.8 ± 0.9 MW m-2K-1when the MoS2is fully lithiated. These results reveal electrochemical intercalation as a reversible tool to modulate and control both electrical and thermal properties of 2D layers.

Microstructural origin of resistance-strain hysteresis in carbon nanotube thin film conductors.

A basic need in stretchable electronics for wearable and biomedical technologies is conductors that maintain adequate conductivity under large deformation. This challenge can be met by a network of one-dimensional (1D) conductors, such as carbon nanotubes (CNTs) or silver nanowires, as a thin film on top of a stretchable substrate. The electrical resistance of CNT thin films exhibits a hysteretic dependence on strain under cyclic loading, although the microstructural origin of this strain dependence remains unclear. Through numerical simulations, analytic models, and experiments, we show that the hysteretic resistance evolution is governed by a microstructural parameter [Formula: see text] (the ratio of the mean projected CNT length over the film length) by showing that [Formula: see text] is hysteretic with strain and that the resistance is proportional to [Formula: see text] The findings are generally applicable to any stretchable thin film conductors consisting of 1D conductors with much lower resistance than the contact resistance in the high-density regime.

Localized Heating and Switching in MoTe2-Based Resistive Memory Devices.

Two-dimensional (2D) materials have recently been incorporated into resistive memory devices because of their atomically thin nature, but their switching mechanism is not yet well understood. Here we study bipolar switching in MoTe2-based resistive memory of varying thickness and electrode area. Using scanning thermal microscopy (SThM), we map the surface temperature of the devices under bias, revealing clear evidence of localized heating at conductive "plugs" formed during switching. The SThM measurements are correlated to electro-thermal simulations, yielding a range of plug diameters (250 to 350 nm) and temperatures at constant bias and during switching. Transmission electron microscopy images reveal these plugs result from atomic migration between electrodes, which is a thermally-activated process. However, the initial forming may be caused by defect generation or Te migration within the MoTe2. This study provides the first thermal and localized switching insights into the operation of such resistive memory and demonstrates a thermal microscopy technique that can be applied to a wide variety of traditional and emerging memory devices.

Quasi-Ballistic Thermal Transport Across MoS2 Thin Films.

Layered two-dimensional (2D) materials have highly anisotropic thermal properties between the in-plane and cross-plane directions. Conventionally, it is thought that cross-plane thermal conductivities (κ z) are low, and therefore c-axis phonon mean free paths (MFPs) are small. Here, we measure κ z across MoS2 films of varying thickness (20-240 nm) and uncover evidence of very long c-axis phonon MFPs at room temperature in these layered semiconductors. Experimental data obtained using time-domain thermoreflectance (TDTR) are in good agreement with first-principles density functional theory (DFT). These calculations suggest that ∼50% of the heat is carried by phonons with MFP > 200 nm, exceeding kinetic theory estimates by nearly 2 orders of magnitude. Because of quasi-ballistic effects, the κ z of nanometer-thin films of MoS2 scales with their thickness and the volumetric thermal resistance asymptotes to a nonzero value, ∼10 m2 K GW-1. This contributes as much as 30% to the total thermal resistance of a 20 nm thick film, the rest being limited by thermal interface resistance with the SiO2 substrate and top-side aluminum transducer. These findings are essential for understanding heat flow across nanometer-thin films of MoS2 for optoelectronic and thermoelectric applications.

Spatial Separation of Carrier Spin by the Valley Hall Effect in Monolayer WSe2 Transistors.

We investigate the valley Hall effect (VHE) in monolayer WSe2 field-effect transistors using optical Kerr rotation measurements at 20 K. While studies of the VHE have so far focused on n -doped MoS2, we observe the VHE in WSe2 in both the n - and p -doping regimes. Hole doping enables access to the large spin-splitting of the valence band of this material. The Kerr rotation measurements probe the spatial distribution of the valley carrier imbalance induced by the VHE. Under current flow, we observe distinct spin-valley polarization along the edges of the transistor channel. From analysis of the magnitude of the Kerr rotation, we infer a spin-valley density of 44 spins/µm, integrated over the edge region in the p -doped regime. Assuming a spin diffusion length less than 0.1 µm, this corresponds to a spin-valley polarization of the holes exceeding 1%.

Contact Engineering High-Performance n-Type MoTe2 Transistors.

Semiconducting MoTe2 is one of the few two-dimensional (2D) materials with a moderate band gap, similar to silicon. However, this material remains underexplored for 2D electronics due to ambient instability and predominantly p-type Fermi level pinning at contacts. Here, we demonstrate unipolar n-type MoTe2 transistors with the highest performance to date, including high saturation current (>400 µA/µm at 80 K and >200 µA/µm at 300 K) and relatively low contact resistance (1.2 to 2 kΩ·µm from 80 to 300 K), achieved with Ag contacts and AlOx encapsulation. We also investigate other contact metals (Sc, Ti, Cr, Au, Ni, Pt), extracting their Schottky barrier heights using an analytic subthreshold model. High-resolution X-ray photoelectron spectroscopy reveals that interfacial metal-Te compounds dominate the contact resistance. Among the metals studied, Sc has the lowest work function but is the most reactive, which we counter by inserting monolayer hexagonal boron nitride between MoTe2 and Sc. These metal-insulator-semiconductor (MIS) contacts partly depin the metal Fermi level and lead to the smallest Schottky barrier for electron injection. Overall, this work improves our understanding of n-type contacts to 2D materials, an important advance for low-power electronics.

Fast Spiking of a Mott VO2-Carbon Nanotube Composite Device.

The recent surge of interest in brain-inspired computing and power-efficient electronics has dramatically bolstered development of computation and communication using neuron-like spiking signals. Devices that can produce rapid and energy-efficient spiking could significantly advance these applications. Here we demonstrate direct current or voltage-driven periodic spiking with sub-20 ns pulse widths from a single device composed of a thin VO2 film with a metallic carbon nanotube as a nanoscale heater, without using an external capacitor. Compared with VO2-only devices, adding the nanotube heater dramatically decreases the transient duration and pulse energy, and increases the spiking frequency, by up to 3 orders of magnitude. This is caused by heating and cooling of the VO2 across its insulator-metal transition being localized to a nanoscale conduction channel in an otherwise bulk medium. This result provides an important component of energy-efficient neuromorphic computing systems and a lithography-free technique for energy-scaling of electronic devices that operate via bulk mechanisms.

Significant Phonon Drag Enables High Power Factor in the AlGaN/GaN Two-Dimensional Electron Gas.

In typical thermoelectric energy harvesters and sensors, the Seebeck effect is caused by diffusion of electrons or holes in a temperature gradient. However, the Seebeck effect can also have a phonon drag component, due to momentum exchange between charge carriers and lattice phonons, which is more difficult to quantify. Here, we present the first study of phonon drag in the AlGaN/GaN two-dimensional electron gas (2DEG). We find that phonon drag does not contribute significantly to the thermoelectric behavior of devices with ∼100 nm GaN thickness, which suppresses the phonon mean free path. However, when the thickness is increased to ∼1.2 µm, up to 32% (88%) of the Seebeck coefficient at 300 K (50 K) can be attributed to the drag component. In turn, the phonon drag enables state-of-the-art thermoelectric power factor in the thicker GaN film, up to ∼40 mW m-1 K-2 at 50 K. By measuring the thermal conductivity of these AlGaN/GaN films, we show that the magnitude of the phonon drag can increase even when the thermal conductivity decreases. Decoupling of thermal conductivity and Seebeck coefficient could enable important advancements in thermoelectric power conversion with devices based on 2DEGs.

High-Field Transport and Velocity Saturation in Synthetic Monolayer MoS2.

Two-dimensional semiconductors such as monolayer MoS2 are of interest for future applications including flexible electronics and end-of-roadmap technologies. Most research to date has focused on low-field mobility, but the peak current-driving ability of transistors is limited by the high-field saturation drift velocity, vsat. Here, we measure high-field transport as a function of temperature for the first time in high-quality synthetic monolayer MoS2. We find that in typical device geometries (e.g. on SiO2 substrates) self-heating can significantly reduce current drive during high-field operation. However, with measurements at varying ambient temperature (from 100 to 300 K), we extract electron vsat = (3.4 ± 0.4) × 106 cm/s at room temperature in this three-atom-thick semiconductor, which we benchmark against other bulk and layered materials. With these results, we estimate that the saturation current in monolayer MoS2 could exceed 1 mA/µm at room temperature, in digital circuits with near-ideal thermal management.

Probing the Optical Properties and Strain-Tuning of Ultrathin Mo1- xW xTe2.

Ultrathin transition metal dichalcogenides (TMDCs) have recently been extensively investigated to understand their electronic and optical properties. Here we study ultrathin Mo0.91W0.09Te2, a semiconducting alloy of MoTe2, using Raman, photoluminescence (PL), and optical absorption spectroscopy. Mo0.91W0.09Te2 transitions from an indirect to a direct optical band gap in the limit of monolayer thickness, exhibiting an optical gap of 1.10 eV, very close to its MoTe2 counterpart. We apply tensile strain, for the first time, to monolayer MoTe2 and Mo0.91W0.09Te2 to tune the band structure of these materials; we observe that their optical band gaps decrease by 70 meV at 2.3% uniaxial strain. The spectral widths of the PL peaks decrease with increasing strain, which we attribute to weaker exciton-phonon intervalley scattering. Strained MoTe2 and Mo0.91W0.09Te2 extend the range of band gaps of TMDC monolayers further into the near-infrared, an important attribute for potential applications in optoelectronics.