Imaging the electron charge density in monolayer MoS2 at the Ångstrom scale.

Four-dimensional scanning transmission electron microscopy (4D-STEM) has recently gained widespread attention for its ability to image atomic electric fields with sub-Ångstrom spatial resolution. These electric field maps represent the integrated effect of the nucleus, core electrons and valence electrons, and separating their contributions is non-trivial. In this paper, we utilized simultaneously acquired 4D-STEM center of mass (CoM) images and annular dark field (ADF) images to determine the projected electron charge density in monolayer MoS2. We evaluate the contributions of both the core electrons and the valence electrons to the derived electron charge density; however, due to blurring by the probe shape, the valence electron contribution forms a nearly featureless background while most of the spatial modulation comes from the core electrons. Our findings highlight the importance of probe shape in interpreting charge densities derived from 4D-STEM and the need for smaller electron probes.

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.

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.

High-Efficiency WSe2 Photovoltaic Devices with Electron-Selective Contacts.

A rapid surge in global energy consumption has led to a greater demand for renewable energy to overcome energy resource limitations and environmental problems. Recently, a number of van der Waals materials have been highlighted as efficient absorbers for very thin and highly efficient photovoltaic (PV) devices. Despite the predicted potential, achieving power conversion efficiencies (PCEs) above 5% in PV devices based on van der Waals materials has been challenging. Here, we demonstrate a vertical WSe2 PV device with a high PCE of 5.44% under one-sun AM1.5G illumination. We reveal the multifunctional nature of a tungsten oxide layer, which promotes a stronger internal electric field by overcoming limitations imposed by the Fermi-level pinning at WSe2 interfaces and acts as an electron-selective contact in combination with monolayer graphene. Together with the developed bottom contact scheme, this simple yet effective contact engineering method improves the PCE by more than five times.

Direct measurement of nanoscale filamentary hot spots in resistive memory devices.

Resistive random access memory (RRAM) is an important candidate for both digital, high-density data storage and for analog, neuromorphic computing. RRAM operation relies on the formation and rupture of nanoscale conductive filaments that carry enormous current densities and whose behavior lies at the heart of this technology. Here, we directly measure the temperature of these filaments in realistic RRAM with nanoscale resolution using scanning thermal microscopy. We use both conventional metal and ultrathin graphene electrodes, which enable the most thermally intimate measurement to date. Filaments can reach 1300°C during steady-state operation, but electrode temperatures seldom exceed 350°C because of thermal interface resistance. These results reveal the importance of thermal engineering for nanoscale RRAM toward ultradense data storage or neuromorphic operation.

High-specific-power flexible transition metal dichalcogenide solar cells.

Semiconducting transition metal dichalcogenides (TMDs) are promising for flexible high-specific-power photovoltaics due to their ultrahigh optical absorption coefficients, desirable band gaps and self-passivated surfaces. However, challenges such as Fermi-level pinning at the metal contact-TMD interface and the inapplicability of traditional doping schemes have prevented most TMD solar cells from exceeding 2% power conversion efficiency (PCE). In addition, fabrication on flexible substrates tends to contaminate or damage TMD interfaces, further reducing performance. Here, we address these fundamental issues by employing: (1) transparent graphene contacts to mitigate Fermi-level pinning, (2) MoOx capping for doping, passivation and anti-reflection, and (3) a clean, non-damaging direct transfer method to realize devices on lightweight flexible polyimide substrates. These lead to record PCE of 5.1% and record specific power of 4.4 W g-1 for flexible TMD (WSe2) solar cells, the latter on par with prevailing thin-film solar technologies cadmium telluride, copper indium gallium selenide, amorphous silicon and III-Vs. We further project that TMD solar cells could achieve specific power up to 46 W g-1, creating unprecedented opportunities in a broad range of industries from aerospace to wearable and implantable electronics.

Toward Low-Temperature Solid-Source Synthesis of Monolayer MoS2.

Two-dimensional (2D) semiconductors have been proposed for heterogeneous integration with existing silicon technology; however, their chemical vapor deposition (CVD) growth temperatures are often too high. Here, we demonstrate direct CVD solid-source precursor synthesis of continuous monolayer (1L) MoS2 films at 560 °C in 50 min, within the 450-to-600 °C, 2 h thermal budget window required for back-end-of-the-line compatibility with modern silicon technology. Transistor measurements reveal on-state current up to ∼140 µA/µm at 1 V drain-to-source voltage for 100 nm channel lengths, the highest reported to date for 1L MoS2 grown below 600 °C using solid-source precursors. The effective mobility from transfer length method test structures is 29 ± 5 cm2 V-1 s-1 at 6.1 × 1012 cm-2 electron density, which is comparable to mobilities reported from films grown at higher temperatures. The results of this work provide a path toward the realization of high-quality, thermal-budget-compatible 2D semiconductors for heterogeneous integration with silicon manufacturing.

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.

Infrared Detectable MoS2 Phototransistor and Its Application to Artificial Multilevel Optic-Neural Synapse.

Layered two-dimensional (2D) materials have entered the spotlight as promising channel materials for future optoelectronic devices owing to their excellent electrical and optoelectronic properties. However, their limited photodetection range caused by their wide bandgap remains a principal challenge in 2D layered materials-based phototransistors. Here, we developed a germanium (Ge)-gated MoS2 phototransistor that can detect light in the region from visible to infrared (λ = 520-1550 nm) using a detection mechanism based on band bending modulation. In addition, the Ge-gated MoS2 phototransistor is proposed as a multilevel optic-neural synaptic device, which performs both optical-sensing and synaptic functions on one device and is operated in different current ranges according to the light conditions: dark, visible, and infrared. This study is expected to contribute to the development of 2D material-based phototransistors and synaptic devices in next-generation optoelectronics.

Limitation of Optical Enhancement in Ultra-thin Solar Cells Imposed by Contact Selectivity.

Ultra-thin crystalline silicon (c-Si) solar cell suffers both from poor light absorption and minority carrier recombination at the contacts resulting in low contact selectivity. Yet most of the research focuses on improving the light absorption by introducing novel light trapping technique. Our work shows that for ultra-thin absorber, the benefit of optical enhancement is limited by low contact selectivity. Using simulation we observe that performance enhancement from light trapping starts to saturate as the absorber scales down because of the increase in probability of the photo-generated carriers to recombine at the metal contact. Therefore, improving the carrier selectivity of the contacts, which reduces the recombination at contacts, is important to improve the performance of the solar cell beyond what is possible by enhancing light absorption only. The impact of improving contact selectivity increases as the absorber thickness scales below 20 micrometer (µm). Light trapping provides better light management and improving contact selectivity provides better photo-generated carrier management. When better light management increases the number of photo-generated carriers, better carrier management is a useful optimization knob to achieve the efficiency close to the thermodynamic limit. Our work explores a design trade-off in detail which is often overlooked by the research community.

Low-threshold optically pumped lasing in highly strained germanium nanowires.

The integration of efficient, miniaturized group IV lasers into CMOS architecture holds the key to the realization of fully functional photonic-integrated circuits. Despite several years of progress, however, all group IV lasers reported to date exhibit impractically high thresholds owing to their unfavourable bandstructures. Highly strained germanium with its fundamentally altered bandstructure has emerged as a potential low-threshold gain medium, but there has yet to be a successful demonstration of lasing from this seemingly promising material system. Here we demonstrate a low-threshold, compact group IV laser that employs a germanium nanowire under a 1.6% uniaxial tensile strain as the gain medium. The amplified material gain in strained germanium can sufficiently overcome optical losses at 83 K, thus allowing the observation of multimode lasing with an optical pumping threshold density of ~3.0 kW cm-2. Our demonstration opens new possibilities for group IV lasers for photonic-integrated circuits.

Contact Selectivity Engineering in a 2 µm Thick Ultrathin c-Si Solar Cell Using Transition-Metal Oxides Achieving an Efficiency of 10.8.

In this paper, the integration of metal oxides as carrier-selective contacts for ultrathin crystalline silicon (c-Si) solar cells is demonstrated which results in an ∼13% relative improvement in efficiency. The improvement in efficiency originates from the suppression of the contact recombination current due to the band offset asymmetry of these oxides with Si. First, an ultrathin c-Si solar cell having a total thickness of 2 µm is shown to have >10% efficiency without any light-trapping scheme. This is achieved by the integration of nickel oxide (NiOx) as a hole-selective contact interlayer material, which has a low valence band offset and high conduction band offset with Si. Second, we show a champion cell efficiency of 10.8% with the additional integration of titanium oxide (TiOx), a well-known material for an electron-selective contact interlayer. Key parameters including Voc and Jsc also show different degrees of enhancement if single (NiOx only) or double (both NiOx and TiOx) carrier-selective contacts are integrated. The fabrication process for TiOx and NiOx layer integration is scalable and shows good compatibility with the device.

Cubic-phase zirconia nano-island growth using atomic layer deposition and application in low-power charge-trapping nonvolatile-memory devices.

The manipulation of matter at the nanoscale enables the generation of properties in a material that would otherwise be challenging or impossible to realize in the bulk state. Here, we demonstrate growth of zirconia nano-islands using atomic layer deposition on different substrate terminations. Transmission electron microscopy and Raman measurements indicate that the nano-islands consist of nano-crystallites of the cubic-crystalline phase, which results in a higher dielectric constant (κ âˆ¼ 35) than the amorphous phase case (κ âˆ¼ 20). X-ray photoelectron spectroscopy measurements show that a deep quantum well is formed in the Al2O3/ZrO2/Al2O3 system, which is substantially different to that in the bulk state of zirconia and is more favorable for memory application. Finally, a memory device with a ZrO2 nano-island charge-trapping layer is fabricated, and a wide memory window of 4.5 V is obtained at a low programming voltage of 5 V due to the large dielectric constant of the islands in addition to excellent endurance and retention characteristics.

Three-dimensional integration of nanotechnologies for computing and data storage on a single chip.

The computing demands of future data-intensive applications will greatly exceed the capabilities of current electronics, and are unlikely to be met by isolated improvements in transistors, data storage technologies or integrated circuit architectures alone. Instead, transformative nanosystems, which use new nanotechnologies to simultaneously realize improved devices and new integrated circuit architectures, are required. Here we present a prototype of such a transformative nanosystem. It consists of more than one million resistive random-access memory cells and more than two million carbon-nanotube field-effect transistors-promising new nanotechnologies for use in energy-efficient digital logic circuits and for dense data storage-fabricated on vertically stacked layers in a single chip. Unlike conventional integrated circuit architectures, the layered fabrication realizes a three-dimensional integrated circuit architecture with fine-grained and dense vertical connectivity between layers of computing, data storage, and input and output (in this instance, sensing). As a result, our nanosystem can capture massive amounts of data every second, store it directly on-chip, perform in situ processing of the captured data, and produce 'highly processed' information. As a working prototype, our nanosystem senses and classifies ambient gases. Furthermore, because the layers are fabricated on top of silicon logic circuitry, our nanosystem is compatible with existing infrastructure for silicon-based technologies. Such complex nano-electronic systems will be essential for future high-performance and highly energy-efficient electronic systems.

Investigation of the Changes in Electronic Properties of Nickel Oxide (NiOx) Due to UV/Ozone Treatment.

Drastic reduction in nickel oxide (NiOx) film resistivity and ionization potential is observed when subjected to ultraviolet (UV)/ozone (O3) treatment. X-ray photoemission spectroscopy suggests that UV/O3 treatment changes the film stoichiometry by introducing Ni vacancy defects. Oxygen-rich NiOx having Ni vacancy defects behaves as a p-type semiconductor. Therefore, in this work, a simple and effective technique to introduce doping in NiOx is shown. Angle-resolved XPS reveals that the effect of UV/O3 treatment does not only alter the film surface property but also introduces oxygen-rich stoichiometry throughout the depth of the film. Finally, simple metal/interlayer/semiconductor (MIS) contacts are fabricated on p-type Si using NiOx as the interlayer and different metals. Significant barrier height reduction is observed with respect to the control sample following UV/O3 treatment, which is in agreement with the observed reduction in film resistivity. From an energy band diagram point of view, the introduction of the UV/O3 treatment changes the defect state distribution, resulting in a change in the pinning of the Fermi level. Therefore, this work also shows that the Fermi level pinning property of NiOx can be controlled using UV/O3 treatment.

Improved Contacts to MoS2 Transistors by Ultra-High Vacuum Metal Deposition.

The scaling of transistors to sub-10 nm dimensions is strongly limited by their contact resistance (RC). Here we present a systematic study of scaling MoS2 devices and contacts with varying electrode metals and controlled deposition conditions, over a wide range of temperatures (80 to 500 K), carrier densities (10(12) to 10(13) cm(-2)), and contact dimensions (20 to 500 nm). We uncover that Au deposited in ultra-high vacuum (∼10(-9) Torr) yields three times lower RC than under normal conditions, reaching 740 Ω·µm and specific contact resistivity 3 × 10(-7) Ω·cm(2), stable for over four months. Modeling reveals separate RC contributions from the Schottky barrier and the series access resistance, providing key insights on how to further improve scaling of MoS2 contacts and transistor dimensions. The contact transfer length is ∼35 nm at 300 K, which is verified experimentally using devices with 20 nm contacts and 70 nm contact pitch (CP), equivalent to the "14 nm" technology node.

Direct Bandgap Light Emission from Strained Germanium Nanowires Coupled with High-Q Nanophotonic Cavities.

A silicon-compatible light source is the final missing piece for completing high-speed, low-power on-chip optical interconnects. In this paper, we present a germanium nanowire light emitter that encompasses all the aspects of potential low-threshold lasers: highly strained germanium gain medium, strain-induced pseudoheterostructure, and high-Q nanophotonic cavity. Our nanowire structure presents greatly enhanced photoluminescence into cavity modes with measured quality factors of up to 2000. By varying the dimensions of the germanium nanowire, we tune the emission wavelength over more than 400 nm with a single lithography step. We find reduced optical loss in optical cavities formed with germanium under high (>2.3%) tensile strain. Our compact, high-strain cavities open up new possibilities for low-threshold germanium-based lasers for on-chip optical interconnects.

Bandgap-customizable germanium using lithographically determined biaxial tensile strain for silicon-compatible optoelectronics.

Strain engineering has proven to be vital for germanium-based photonics, in particular light emission. However, applying a large permanent biaxial tensile strain to germanium has been a challenge. We present a simple, CMOS-compatible technique to conveniently induce a large, spatially homogenous strain in circular structures patterned within germanium nanomembranes. Our technique works by concentrating and amplifying a pre-existing small strain into a circular region. Biaxial tensile strains as large as 1.11% are observed by Raman spectroscopy and are further confirmed by photoluminescence measurements, which show enhanced and redshifted light emission from the strained germanium. Our technique allows the amount of biaxial strain to be customized lithographically, allowing the bandgaps of different germanium structures to be independently customized in a single mask process.

Monolithic integration of germanium-on-insulator p-i-n photodetector on silicon.

A germanium-on-insulator (GOI) p-i-n photodetector, monolithically integrated on a silicon (Si) substrate, is demonstrated. GOI is formed by lateral-overgrowth (LAT-OVG) of Ge on silicon dioxide (SiO(2)) through windows etched in SiO(2) on Si. The photodetector shows excellent diode characteristics with high on/off ratio (6 × 10(4)), low dark current, and flat reverse current-voltage (I-V) characteristics. Enhanced light absorption up to 1550 nm is observed due to the residual biaxial tensile strain induced during the epitaxial growth of Ge caused by cooling after the deposition. This truly Si-compatible Ge photodetector using monolithic integration enables new opportunities for high-performance GOI based photonic devices on Si platform.