Disordered enthalpy-entropy descriptor for high-entropy ceramics discovery.

The need for improved functionalities in extreme environments is fuelling interest in high-entropy ceramics1-3. Except for the computational discovery of high-entropy carbides, performed with the entropy-forming-ability descriptor4, most innovation has been slowly driven by experimental means1-3. Hence, advancement in the field needs more theoretical contributions. Here we introduce disordered enthalpy-entropy descriptor (DEED), a descriptor that captures the balance between entropy gains and enthalpy costs, allowing the correct classification of functional synthesizability of multicomponent ceramics, regardless of chemistry and structure. To make our calculations possible, we have developed a convolutional algorithm that drastically reduces computational resources. Moreover, DEED guides the experimental discovery of new single-phase high-entropy carbonitrides and borides. This work, integrated into the AFLOW computational ecosystem, provides an array of potential new candidates, ripe for experimental discoveries.

Toward High-Performance p-Type Two-Dimensional Field Effect Transistors: Contact Engineering, Scaling, and Doping.

n-type field effect transistors (FETs) based on two-dimensional (2D) transition-metal dichalcogenides (TMDs) such as MoS2 and WS2 have come close to meeting the requirements set forth in the International Roadmap for Devices and Systems (IRDS). However, p-type 2D FETs are dramatically lagging behind in meeting performance standards. Here, we adopt a three-pronged approach that includes contact engineering, channel length (Lch) scaling, and monolayer doping to achieve high performance p-type FETs based on synthetic WSe2. Using electrical measurements backed by atomistic imaging and rigorous analysis, Pd was identified as the favorable contact metal for WSe2 owing to better epitaxy, larger grain size, and higher compressive strain, leading to a lower Schottky barrier height. While the ON-state performance of Pd-contacted WSe2 FETs was improved by ∼10× by aggressively scaling Lch from 1 µm down to ∼20 nm, ultrascaled FETs were found to be contact limited. To reduce the contact resistance, monolayer tungsten oxyselenide (WOxSey) obtained using self-limiting oxidation of bilayer WSe2 was used as a p-type dopant. This led to ∼5× improvement in the ON-state performance and ∼9× reduction in the contact resistance. We were able to achieve a median ON-state current as high as ∼10 µA/µm for ultrascaled and doped p-type WSe2 FETs with Pd contacts. We also show the applicability of our monolayer doping strategy to other 2D materials such as MoS2, MoTe2, and MoSe2.

Extreme γ-Ray Radiation Tolerance of Spectrometer-Grade CsPbBr3 Perovskite Detectors.

The perovskite compound CsPbBr3 has recently been discovered as a promising room-temperature semiconductor radiation detector, offering an inexpensive and easy-to-manufacture alternative to the current benchmark material Cd1-x Znx Te (CZT). The performance of CsPbBr3 sensors is evaluated under harsh conditions, such as high radiation doses often found in industrial settings and extreme radiation in space. Results show minimal degradation in detector performance after exposure to 1 Mrad of Co-60 gamma radiation, with no significant change to energy resolution or hole mobility and lifetime. Additionally, many of the devices are still functional after being exposed to a 10 Mrad dose over 3 days, and those that do not survive can still be refabricated into working detectors. These results suggest that the failure mode in these devices is likely related to the interface between the electrode and material and their reaction, or the electrode itself and not the material itself. Overall, the study suggests that CsPbBr3 has high potential as a reliable and efficient radiation detector in various applications, including those involving extreme fluxes and energies of gamma-ray radiation.

Radiation Resilient Two-Dimensional Electronics.

Limitations in cloud-based computing have prompted a paradigm shift toward all-in-one "edge" devices capable of independent data sensing, computing, and storage. Advanced defense and space applications stand to benefit immensely from this due to their need for continual operation in areas where maintaining remote oversight is difficult. However, the extreme environments relevant to these applications necessitate rigorous testing of technologies, with a common requirement being hardness to ionizing radiation. Two-dimensional (2D) molybdenum disulfide (MoS2) has been noted to enable the sensing, storage, and logic capabilities necessary for all-in-one edge devices. Despite this, the investigation of ionizing radiation effects in MoS2-based devices remains incomplete. In particular, studies on gamma radiation effects in MoS2 have been largely limited to standalone films, with few device investigations; to the best of our knowledge, no explorations have been made into gamma radiation effects on the sensing and memory capabilities of MoS2-based devices. In this work, we have used a statistical approach to study high-dose (1 Mrad) gamma radiation effects on photosensitive and programmable memtransistors fabricated from large-area monolayer MoS2. Memtransistors were divided into separate groups to ensure accurate extraction of device characteristics pertaining to baseline performance, sensing, and memory before and after irradiation. All-MoS2 logic gates were also assessed to determine the gamma irradiation impact on logic implementation. Our findings show that the multiple functionalities of MoS2 memtransistors are not severely impacted by gamma irradiation even without dedicated shielding/mitigation techniques. We believe that these results serve as a foundation for more application-oriented studies going forward.

Ultrascaled Contacts to Monolayer MoS2 Field Effect Transistors.

Two-dimensional (2D) semiconductors possess promise for the development of field-effect transistors (FETs) at the ultimate scaling limit due to their strong gate electrostatics. However, proper FET scaling requires reduction of both channel length (LCH) and contact length (LC), the latter of which has remained a challenge due to increased current crowding at the nanoscale. Here, we investigate Au contacts to monolayer MoS2 FETs with LCH down to 100 nm and LC down to 20 nm to evaluate the impact of contact scaling on FET performance. Au contacts are found to display a ∼2.5× reduction in the ON-current, from 519 to 206 µA/µm, when LC is scaled from 300 to 20 nm. It is our belief that this study is warranted to ensure an accurate representation of contact effects at and beyond the technology nodes currently occupied by silicon.

Active pixel sensor matrix based on monolayer MoS2 phototransistor array.

In-sensor processing, which can reduce the energy and hardware burden for many machine vision applications, is currently lacking in state-of-the-art active pixel sensor (APS) technology. Photosensitive and semiconducting two-dimensional (2D) materials can bridge this technology gap by integrating image capture (sense) and image processing (compute) capabilities in a single device. Here, we introduce a 2D APS technology based on a monolayer MoS2 phototransistor array, where each pixel uses a single programmable phototransistor, leading to a substantial reduction in footprint (900 pixels in ∼0.09 cm2) and energy consumption (100s of fJ per pixel). By exploiting gate-tunable persistent photoconductivity, we achieve a responsivity of ∼3.6 × 107 A W-1, specific detectivity of ∼5.6 × 1013 Jones, spectral uniformity, a high dynamic range of ∼80 dB and in-sensor de-noising capabilities. Further, we demonstrate near-ideal yield and uniformity in photoresponse across the 2D APS array.

Plasmonic high-entropy carbides.

Discovering multifunctional materials with tunable plasmonic properties, capable of surviving harsh environments is critical for advanced optical and telecommunication applications. We chose high-entropy transition-metal carbides because of their exceptional thermal, chemical stability, and mechanical properties. By integrating computational thermodynamic disorder modeling and time-dependent density functional theory characterization, we discovered a crossover energy in the infrared and visible range, corresponding to a metal-to-dielectric transition, exploitable for plasmonics. It was also found that the optical response of high-entropy carbides can be largely tuned from the near-IR to visible when changing the transition metal components and their concentration. By monitoring the electronic structures, we suggest rules for optimizing optical properties and designing tailored high-entropy ceramics. Experiments performed on the archetype carbide HfTa4C5 yielded plasmonic properties from room temperature to 1500K. Here we propose plasmonic transition-metal high-entropy carbides as a class of multifunctional materials. Their combination of plasmonic activity, high-hardness, and extraordinary thermal stability will result in yet unexplored applications.

Boosting phase contrast with a grating Bonse-Hart interferometer of 200 nanometre grating period.

We report on a grating Bonse-Hart interferometer for phase-contrast imaging with hard X-rays. The method overcomes limitations in the level of sensitivity that can be achieved with the well-known Talbot grating interferometer, and without the stringent spectral filtering at any given incident angle imposed by the classic Bonse-Hart interferometer. The device operates in the far-field regime, where an incident beam is split by a diffraction grating into two widely separated beams, which are redirected by a second diffraction grating to merge at a third grating, where they coherently interfere. The wide separation of the interfering beams results in large phase contrast, and in some cases absolute phase images are obtained. Imaging experiments were performed using diffraction gratings of 200 nm period, at 22.5 keV and 1.5% spectral bandwidth on a bending-magnetic beamline. Novel design and fabrication process were used to achieve the small grating period. Using a slitted incident beam, we acquired absolute and differential phase images of lightly absorbing samples. An advantage of this method is that it uses only phase modulating gratings, which are easier to fabricate than absorption gratings of the same periods.

Subnanoradian X-ray phase-contrast imaging using a far-field interferometer of nanometric phase gratings.

Hard X-ray phase-contrast imaging characterizes the electron density distribution in an object without the need for radiation absorption. The power of phase contrast to resolve subtle changes, such as those in soft tissue structures, lies in its ability to detect minute refractive bending of X-rays. Here we report a far-field, two-arm interferometer based on the new nanometric phase gratings, which can detect X-ray refraction with subnanoradian sensitivity, and at the same time overcomes the fundamental limitation of ultra-narrow bandwidths (Δλ/λ~10⁻4) of the current, most sensitive methods based on crystal interferometers. On a 1.5% bandwidth synchrotron source, we demonstrate clear visualization of blood vessels in unstained mouse organs in simple projection views, with over an order-of-magnitude higher phase contrast than current near-field grating interferometers.

Interferometric hard x-ray phase contrast imaging at 204 nm grating period.

We report on hard x-ray phase contrast imaging experiments using a grating interferometer of approximately 1/10th the grating period achieved in previous studies. We designed the gratings as a staircase array of multilayer stacks which are fabricated in a single thin film deposition process. We performed the experiments at 19 keV x-ray energy and 0.8 µm pixel resolution. The small grating period resulted in clear separation of different diffraction orders and multiple images on the detector. A slitted beam was used to remove overlap of the images from the different diffraction orders. The phase contrast images showed detailed features as small as 10 µm, and demonstrated the feasibility of high resolution x-ray phase contrast imaging with nanometer scale gratings.