Flexible high-temperature dielectric materials from polymer nanocomposites.

Dielectric materials, which store energy electrostatically, are ubiquitous in advanced electronics and electric power systems. Compared to their ceramic counterparts, polymer dielectrics have higher breakdown strengths and greater reliability, are scalable, lightweight and can be shaped into intricate configurations, and are therefore an ideal choice for many power electronics, power conditioning, and pulsed power applications. However, polymer dielectrics are limited to relatively low working temperatures, and thus fail to meet the rising demand for electricity under the extreme conditions present in applications such as hybrid and electric vehicles, aerospace power electronics, and underground oil and gas exploration. Here we describe crosslinked polymer nanocomposites that contain boron nitride nanosheets, the dielectric properties of which are stable over a broad temperature and frequency range. The nanocomposites have outstanding high-voltage capacitive energy storage capabilities at record temperatures (a Weibull breakdown strength of 403 megavolts per metre and a discharged energy density of 1.8 joules per cubic centimetre at 250 degrees Celsius). Their electrical conduction is several orders of magnitude lower than that of existing polymers and their high operating temperatures are attributed to greatly improved thermal conductivity, owing to the presence of the boron nitride nanosheets, which improve heat dissipation compared to pristine polymers (which are inherently susceptible to thermal runaway). Moreover, the polymer nanocomposites are lightweight, photopatternable and mechanically flexible, and have been demonstrated to preserve excellent dielectric and capacitive performance after intensive bending cycles. These findings enable broader applications of organic materials in high-temperature electronics and energy storage devices.

Quality enhancement of low temperature metal organic chemical vapor deposited MoS2: an experimental and computational investigation.

Electronic quality of chemical vapor deposited MoS2 is a function of crystallinity, which tends to decline with decrease in deposition temperature. Conventional thermal annealing can improve the quality but requires very high temperatures. In this study, we investigate a novel low temperature (room temperature to 400 °C) annealing process that exploits the electron wind force during passage of current. Here, moderate current density gives rise to atomic scale mechanical force whenever the electrons encounter defects in the lattice or grain boundaries (GBs). After hypothesizing that this force can significantly enhance defect mobility without any temperature field, we demonstrate the process using in situ transmission electron microscope and molecular dynamics simulation. Monolayer metal organic chemical vapor deposited MoS2 deposited at 400 °C was post processed at temperature as low as 20 °C. Experimental results show five times enhancement in electrical conductivity, which is supported by electron diffraction patterns indicating significant grain growth. Discrete spots in diffraction indicate evolution of high crystallinity even at room temperature. Our computational model shows the mechanisms behind healing lattice defects as well as reorienting the GBs. The enhancement in microstructure of the specimen is also reflected in mechanical properties simulations on pre- and post-annealed specimens.

In situ transmission electron microscopy of transistor operation and failure.

Microscopy is typically used as a post-mortem analytical tool in performance and reliability studies on nanoscale materials and devices. In this study, we demonstrate real time microscopy of the operation and failure of AlGaN/GaN high electron mobility transistors inside the transmission electron microscope. Loading until failure was performed on the electron transparent transistors to visualize the failure mechanisms caused by self-heating. At lower drain voltages, thermo-mechanical stresses induce irreversible microstructural deformation, mostly along the AlGaN/GaN interface, to initiate the damage process. At higher biasing, the self-heating deteriorates the gate and catastrophic failure takes place through metal/semiconductor inter-diffusion and/or buffer layer breakdown. This study indicates that the current trend of recreating the events, from damage nucleation to catastrophic failure, can be replaced by in situ microscopy for a quick and accurate account of the failure mechanisms.

Transformation of 2D group-III selenides to ultra-thin nitrides: enabling epitaxy on amorphous substrates.

The experimental realization of two-dimensional (2D) gallium nitride (GaN) has enabled the exploration of 2D nitride materials beyond boron nitride. Here we demonstrate one possible pathway to realizing ultra-thin nitride layers through a two-step process involving the synthesis of naturally layered, group-III chalcogenides (GIIIC) and subsequent annealing in ammonia (ammonolysis) that leads to an atomic-exchange of the chalcogen and nitrogen species in the 2D-GIIICs. The effect of nitridation differs for gallium and indium selenide, where gallium selenide undergoes structural changes and eventual formation of ultra-thin GaN, while indium selenide layers are primarily etched rather than transformed by nitridation. Further investigation of the resulting GaN films indicates that ultra-thin GaN layers grown on silicon dioxide act as effective 'seed layers' for the growth of 3D GaN on amorphous substrates.

Role of sulphur atoms on stress relaxation and crack propagation in monolayer MoS2.

We present in-situ transmission electron microscopy of crack propagation in a freestanding monolayer MoS2 and molecular dynamic analysis of the underlying mechanisms. Chemical vapor deposited monolayer MoS2 was transferred from sapphire substrate using interfacial etching for defect and contamination minimization. Atomic resolution imaging shows crack tip atoms sustaining 14.5% strain before bond breaking, while the stress field decays at unprecedented rate of 2.15 GPa Å-1. Crack propagation is seen mostly in the zig-zag direction in both model and experiment, suggesting that the mechanics of fracture is not brittle. Our computational model captures the mechanics of the experimental observations on crack propagation in MoS2. While molybdenum atoms carry most of the mechanical load, we show that the sliding motion of weakly bonded sulphur atoms mediate crack tip stress relaxation, which helps the tip sustain very high, localized stress levels.

Synergistic Thermal and Electron Wind Force-Assisted Annealing for Extremely High-Density Defect Mitigation.

This study investigates the effectiveness of combined thermal and athermal stimuli in mitigating the extremely high-density nature of dislocation networks in the form of low-angle grain boundaries in FeCrAl alloy. Electron wind force, generated from very low duty cycle and high current density pulses, was used as the athermal stimulus. The electron wind force stimulus alone was unable to remove the residual stress (80% low-angle grain boundaries) due to cold rolling to 25% thickness reduction. When the duty cycle was increased to allow average temperature of 100 °C, the specimen could be effectively annealed in 1 min at a current density of 3300 A/mm2. In comparison, conventional thermal annealing requires at least 750 °C and 1.5 h. For specimens with 50% thickness reduction (85% low-angle grain boundaries), the electron wind force was again unable to anneal the defects even at 3300 A/mm2 current density and average temperature of 100 °C. Intriguingly, allowing average concurrent temperature of 200 °C eliminated almost all the low-angle grain boundaries at a current density of 700 A/mm2, even lower than that required for the 25% thickness reduced specimens. Comprehensive electron and X-ray diffraction evidence show that alloys with extremely high defect density can be effectively annealed in less than a minute at approximately 200 °C, offering a substantial improvement over conventional high-temperature annealing.

Real-Time Observation of Nanoscale Kink Band Mediated Plasticity in Ion-Irradiated Graphite: An In Situ TEM Study.

Graphite IG-110 is a synthetic polycrystalline material used as a neutron moderator in reactors. Graphite is inherently brittle and is known to exhibit a further increase in brittleness due to radiation damage at room temperature. To understand the irradiation effects on pre-existing defects and their overall influence on external load, micropillar compression tests were performed using in situ nanoindentation in the Transmission Electron Microscopy (TEM) for both pristine and ion-irradiated samples. While pristine specimens showed brittle and subsequent catastrophic failure, the 2.8 MeV Au2+ ion (fluence of 4.378 × 1014 cm-2) irradiated specimens sustained extensive plasticity at room temperature without failure. In situ TEM characterization showed nucleation of nanoscale kink band structures at numerous sites, where the localized plasticity appeared to close the defects and cracks while allowing large average strain. We propose that compressive mechanical stress due to dimensional change during ion irradiation transforms buckled basal layers in graphite into kink bands. The externally applied load during the micropillar tests proliferates the nucleation and motion of kink bands to accommodate the large plastic strain. The inherent non-uniformity of graphite microstructure promotes such strain localization, making kink bands the predominant mechanism behind unprecedented toughness in an otherwise brittle material.

Is stress concentration relevant for nanocrystalline metals?

Classical fracture mechanics as well as modern strain gradient plasticity theories assert the existence of stress concentration (or strain gradient) ahead of a notch tip, albeit somewhat relaxed in ductile materials. In this study, we present experimental evidence of extreme stress homogenization in nanocrystalline metals that result in immeasurable amount of stress concentration at a notch tip. We performed in situ uniaxial tension tests of 80 nm thick (50 nm average grain size) freestanding, single edge notched aluminum specimens inside a transmission electron microscope. The theoretical stress concentration for the given notch geometry was as high as 8, yet electron diffraction patterns unambiguously showed absence of any measurable stress concentration at the notch tip. To identify possible mechanisms behind such an anomaly, we performed molecular dynamics simulations on scaled down samples. Extensive grain rotation driven by grain boundary diffusion, exemplified by an Ashby-Verrall type of grain switching process, was observed at the notch tip to relieve stress concentration. We conclude that in the absence of dislocations, grain realignment or rotation may have played a critical role in accommodating externally applied strain and neutralizes any stress concentration during the process.

A Biomimetic Adapter for Passive Self-alignment of Prosthetic Feet.

INTRODUCTION: Dynamic alignment of lower limb prostheses is subjective and time-consuming. Compensatory gait strategies caused by prosthesis misalignment can negatively affect lower limb amputees who cannot access a certified prosthetist for alignment adjustments. The objective of this study is to evaluate a novel six-degrees-of-freedom passive transtibial prosthetic adapter that self-aligns during various phases of gait. This self-aligning adapter may benefit service members and veterans stationed or living far from a clinical facility. METHODS: Four transtibial amputee subjects, aged 47 to 62 (mean: 55.75) years with mean weight of 163.6 lbs and mean K-level of 3.25, walked at self-selected speeds on a 10-m level walkway. Subjects walked with the self-aligning and a size- or weight-matched control adapter, assembled to a commercially available energy-storing-and-returning foot and their own socket, with 22-mm alignment perturbations in the anterior, posterior, medial, or lateral directions. Subjects were blinded to both adapter type and misalignment. Socket moments, spatiotemporal gait parameters, and subjective socket comfort were recorded. RESULTS: Preliminary results showed improvements in mean peak socket moments and step length differential with the self-aligning adapter across all alignments. Walking speed and prosthesis-side base of support showed little change in all configurations. Prosthesis-side stance duration and Functional Ambulation Profile Score increased with the self-aligning adapter in some alignments. Patient-reported socket comfort increased slightly with the self-aligning adapter across all misalignments. CONCLUSION: Subjects maintained similar walking speeds and experienced greater gait symmetry and reduced sagittal plane peak moments with the self-aligning adapter when exposed to misalignments. These trends suggest a benefit to transtibial amputees from a reduction in secondary gait effects from prosthesis misalignments. Additionally, a wider range of acceptable prosthesis alignments may be possible with the self-aligning adapter. Subsequent trials are underway to evaluate the self-aligning adapter in real-world environments like walking on uneven terrains, stairs, ramps, and abrupt turns.