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At least 235 records · Page 13

Tunable Microwave Conductance of Nanodomains in Ferroelectric PbZr 0.2 Ti 0.8 O 3 Thin Film

Ferroelectric materials exhibit spontaneous polarization that can be switched by electric field. Beyond traditional applications as nonvolatile capacitive elements, the interplay between polarization and electronic transport in ferroelectric thin films has enabled a path to neuromorphic device applications involving resistive switching. A fundamental challenge, however, is that finite electronic conductivity may introduce considerable power dissipation and perhaps destabilize ferroelectricity itself. In this work, tunable microwave frequency electronic response of domain walls injected into ferroelectric lead zirconate titanate (PbZr 0.2 Ti 0.8 O 3 ) on the level of a single nanodomain is revealed. Tunable microwave response is detected through first-order reversal curve spectroscopy combined with scanning microwave impedance microscopy measurements taken near 3 GHz. Contributions of film interfaces to the measured AC conduction through subtractive milling, where the film exhibited improved conduction properties after removal of surface layers, are investigated. Using statistical analysis and finite element modeling, we inferred that the mechanism of tunable microwave conductance is the variable area of the domain wall in the switching volume. These observations open the possibilities for ferroelectric memristors or volatile resistive switches, localized to several tens of nanometers and operating according to well-defined dynamics under an applied field.

36 MATERIALS SCIENCE↗

Edge supercurrent reveals competition between condensates in a Weyl superconductor

In topological materials, the edge states are readily distinguished from the bulk states. The situation where a topological semimetal becomes superconducting so that Cooper pairs occupy both the bulk and the edge states is not well understood. In particular, we do not know if we can force their pairing symmetries to be different. Here we show that, when supercurrent is injected into the superconducting Weyl semimetal MoTe 2 from Nb contacts, the invasive s-wave pairing potential from Nb is incompatible with the intrinsic Cooper pair condensate in MoTe 2 . This incompatibility leads to strong stochasticity in the switching current and an unusual anti-hysteretic behaviour in the current–voltage loops. There is also an asymmetry in the edge oscillations where, as the magnetic field crosses zero, the phase noise switches from one with a noisy spectrum to one that is noise free. Furthermore, using the noise spectrum as a guide, we track the anomalous features to field-induced switching of the device gap function between s-wave symmetry and the unconventional symmetry intrinsic to MoTe 2 . We infer that the behaviour of the gap function along the edges is different from that in the bulk.

Superconducting properties and materials↗

Tests of the Rockwell Si:As Back-Illuminated Blocked-Impurity Band (BIBIB) detectors

Two arrays of Rockwell's Si:As back-illuminated blocked-impurity-band detectors were tested at the Max-Planck-Institute for Astronomy (MPIA) at low background and low temperature for possible use in the astronomical space experiment ISOPHOT. For these measurements special test equipment was put together. A cryostat was mechanically modified to accommodate the arrays and special peripheral electronics was added to a microprocessor system to drive the cold multiplexer and to acquire the output data. The first device, a 16x50 element array on a fan-out board was used to test individual pixels with a trans-impedance-amplifier at a photon background of 10(exp 8) Ph s(-1)cm(-2) and at temperatures of 2.7 to 4.4 K. The noise-equivalent-power NEP is in the range 5 - 7 x 10(exp -18) WHz(exp -1/2), the responsivity is less than or equal to 100 AW(exp -1)(f = 10 Hz). The second device was a 10x50 array including a cold readout electronics of switched FETs (SWIFET). Measurements of this array were done in a background range of 5 x 10(exp 5) to 5 x 10(exp 11) Ph s(exp-1)cm(exp-2) and at operating temperatures between 3.0 and 4.8 K. The NEP ranges from less than 10(exp -18) at the lowest background to 2 x 10(exp -16) WHz(exp -1/2) at the highest flux.

Wolf, J.↗

Disentangling Ferroelectric Wall Dynamics and Identification of Pinning Mechanisms via Deep Learning

Field-induced domain-wall dynamics in ferroelectric materials underpins multiple applications ranging from actuators to information technology devices and necessitates a quantitative description of the associated mechanisms including giant electromechanical couplings, controlled nonlinearities, or low coercive voltages. While the advances in dynamic piezoresponse force microscopy measurements over the last two decades have rendered visualization of polarization dynamics relatively straightforward, the associated insights into the local mechanisms have been elusive. This work explores the domain dynamics in model polycrystalline materials using a workflow combining deep-learning-based segmentation of the domain structures with nonlinear dimensionality reduction using multilayer rotationally invariant autoencoders (rVAE). The former allows unambiguous identification and classification of the ferroelectric and ferroelastic domain walls. Here, the rVAE discovers the latent representations of the domain wall geometries and their dynamics, consequently providing insight into the intrinsic mechanisms of polarization switching, that can further be compared to simple physical models. The rVAE disentangles the factors affecting the pinning efficiency of ferroelectric walls, offering insights into the correlation of ferroelastic wall distribution and ferroelectric wall pinning.

36 MATERIALS SCIENCE↗

Analyses of Transistor Punchthrough Failures

The failure of two transistors in the Altitude Switch Assembly for the Solid Rocket Booster followed by two additional failures a year later presented a challenge to failure analysts. These devices had successfully worked for many years on numerous missions. There was no history of failures with this type of device. Extensive checks of the test procedures gave no indication for a source of the cause. The devices were manufactured more than twenty years ago and failure information on this lot date code was not readily available. External visual exam, radiography, PEID, and leak testing were performed with nominal results Electrical testing indicated nearly identical base-emitter and base-collector characteristics (both forward and reverse) with a low resistance short emitter to collector. These characteristics are indicative of a classic failure mechanism called punchthrough. In failure analysis punchthrough refers to an condition where a relatively low voltage pulse causes the device to conduct very hard producing localized areas of thermal runaway or "hot spots". At one or more of these hot spots, the excessive currents melt the silicon. Heavily doped emitter material diffuses through the base region to the collector forming a diffusion pipe shorting the emitter to base to collector. Upon cooling, an alloy junction forms between the pipe and the base region. Generally, the hot spot (punch-through site) is under the bond and no surface artifact is visible. The devices were delidded and the internal structures were examined microscopically. The gold emitter lead was melted on one device, but others had anomalies in the metallization around the in-tact emitter bonds. The SEM examination confirmed some anomalies to be cosmetic defects while other anomalies were artifacts of the punchthrough site. Subsequent to these analyses, the contractor determined that some irregular testing procedures occurred at the time of the failures heretofore unreported. These testing irregularities involved the use of a breakout box and were the likely cause of the failures. There was no evidence to suggest a generic failure mechanism was responsible for the failure of these transistors.

Nicolas, David P.↗

Bottom-up Assembly of Nanoporous Graphene with Emergent Electronic States

The incorporation of nanoscale pores into a sheet of graphene allows it to switch from an impermeable semimetal to a semiconducting nanosieve. Nanoporous graphenes are desirable for applications ranging from high-performance semiconductor device channels to atomically thin molecular sieve membranes, and their performance is highly dependent on the periodicity and reproducibility of pores at the atomic level. Achieving precise nanopore topologies in graphene using top-down lithographic approaches has proven to be challenging due to poor structural control at the atomic level. Alternatively, atomically precise nanometer-sized pores can be fabricated via lateral fusion of bottom-up synthesized graphene nanoribbons. This technique, however, typically requires an additional high temperature cross-coupling step following the nanoribbon formation that inherently yields poor lateral conjugation, resulting in 2D materials that are weakly connected both mechanically and electronically. Here, we demonstrate a novel bottom-up approach for forming fully conjugated nanoporous graphene through a single, mild annealing step following the initial polymer formation. We find emergent interface-localized electronic states within the bulk band gap of the graphene nanoribbon that hybridize to yield a dispersive two-dimensional low-energy band of states. We show that this low-energy band can be rationalized in terms of edge states of the constituent single-strand nanoribbons. The localization of these 2D states around pores makes this material particularly attractive for applications requiring electronically sensitive molecular sieves.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High‐Efficiency Magnon‐Mediated Magnetization Switching in All‐Oxide Heterostructures with Perpendicular Magnetic Anisotropy

Abstract The search for efficient approaches to realize local switching of magnetic moments in spintronic devices has attracted extensive attention. One of the most promising approaches is the electrical manipulation of magnetization through electron‐mediated spin torque. However, the Joule heat generated via electron motion unavoidably causes substantial energy dissipation and potential damage to spintronic devices. Here, all‐oxide heterostructures of SrRuO 3 /NiO/SrIrO 3 are epitaxially grown on SrTiO 3 single‐crystal substrates following the order of the ferromagnetic transition metal oxide SrRuO 3 with perpendicular magnetic anisotropy, insulating and antiferromagnetic NiO, and metallic transition metal oxide SrIrO 3 with strong spin–orbit coupling. It is demonstrated that instead of the electron spin torques, the magnon torques present in the antiferromagnetic NiO layer can directly manipulate the perpendicular magnetization of the ferromagnetic layer. This magnon mechanism may significantly reduce the electron motion‐related energy dissipation from electron‐mediated spin currents. Interestingly, the threshold current density to generate a sufficient magnon current to manipulate the magnetization is one order of magnitude smaller than that in conventional metallic systems. These findings suggest a route for developing highly efficient all‐oxide spintronic devices operated by magnon current.

Zheng, Dongxing↗

Increasing Multilayer Ceramic Capacitor Lifetime With Bipolar Voltage Cycling

Enhancing the lifetime of multilayer ceramic capacitors (MLCCs) is critical in many aerospace, naval, or electrical grid applications, where device failure could lead to catastrophic consequences. The migration of oxygen vacancies from the ceramic to the electrode interface under constant bias is known to reduce the lifetime of oxide-based MLCCs. Bias cycling presents an opportunity to enhance MLCC lifetime by reducing oxygen vacancy migration. The ideal frequency range is expected to lie between frequencies low enough to avoid self-heating but high enough to avoid interfacial defect formation. However, the impact of low-frequency bipolar voltage cycling (BVC) on MLCC degradation mechanisms has not been well studied. This work investigates the impact of periodic BVC on the degradation of MLCCs through highly accelerated lifetime testing (HALT) on X7R capacitors. HALT tests were conducted at 255 °C and 60 V using different switching frequencies: 0 (dc), 0.1, 2.5, and 10 Hz. BVC was found to improve the lifetime of MLCCs compared to dc test conditions. MLCCs tested at 10-Hz BVC showed a 311% increase in average time to failure compared to the dc case. Impedance spectroscopy shows that BVC decreases the rate of resistance degradation within MLCCs, indicating that oxygen vacancy migration to the electrodes is mitigated. The impedance spectra taken on BVC samples highlight how grain boundaries play a vital role in trapping oxygen vacancies. Periodic cycling causes oxygen vacancies to become trapped at grain boundaries, resulting in oxygen vacancies taking longer to reach the electrode interface and thus increasing MLCC lifetime. This work highlights not only how BVC can be used to increase MLCC lifetime but also how periodically cycling MLCCs could increase lifetime in extreme environments, such as at elevated temperatures and electric fields.

Chuong, Kayla Y.↗

Propellantless Attitude Control of Solar Sail Technology Utilizing Reflective Control Devices

Solar sails offer an opportunity for a CubeSatscale, propellant-free spacecraft technology that enables long-term and long-distance missions not possible with traditional methods. Solar sails operate using the transfer of linear momentum from photons of sunlight reflected from the surface of the sail. To propel the spacecraft, no mechanically moving parts, thrusters, or propellant are needed. However, attitude control, or orientation, is still performed using traditional methods involving reaction wheels and propellant ejection, which severely limit mission lifetime. For example, the current state of the art solutions employed by upcoming missions couple solar sails with a state of the art propellant ejection gas system. Here, the use of the gas thruster has limited the lifetime of the mission. To solve the limited mission lifetime problem, the Propellantless Attitude Control of Solar Sail Technology Utilizing Reflective Control Devices project team is working on propellantless attitude control using thin layers of material, an optical film, electrically switchable from transparent to reflective. The technology is based on a polymer-dispersed liquid crystal (PDLC), which allows this switch upon application of a voltage. This technology removes the need for propellant, which reduces weight and cost while improving performance and lifetime.

Solar sail technology↗

Structure and Dynamics of Domains in Ferroelectric Nanostructures – Phase-Field Modeling (Final Technical Report)

Domain pattern formation is one of the most common phenomena in nature and is a topic of immense interest in many fields ranging from materials science and physics to chemistry and biology. This DOE sponsored research project explored the basic science concerning the thermodynamic stability of mesoscale polarization domain patterns and their temporal evolution mechanisms during formation and subsequent switching in ferroelectric nanostructures and heterostructures. The project employed the computational phase-field method in combination of microelasticity and electrostatic theories. The research was carried out in close collaboration with a number of experimental groups who used High Resolution Transmission Electron Microscopy (HRTEM), in situ TEM with Scanning Probe Microscopy (SPM), or Piezoresponse Force Microscopy (PFM) to characterize the domain structures and dynamics of ferroelectric thin films and heterostructures and who grow high-quality ferroelectric and multiferroic thin films using advanced growth techniques such as Molecular Beam Epitaxy (MBE), Pulsed Laser Deposition (PLLD), and sputtering. The research efforts of the project help establish the phase-field method as the most powerful method for understanding and predicting domain structures in ferroelectric thin films and nanostructures. The findings of the project led to the basic understanding of stability and switching mechanisms of ferroelectric domains under different mechanical boundary conditions and under either homogeneous capacitor configurations or local fields using metallic probes as electrodes and the emergence of charged domain walls during domain switching. The project predicted the spatial length scales, temperature ranges, and electromechanical conditions for different polar states in heterostructures and guided the discovery of both transient and stable novel polarization states containing vortex lattices in oxide superlattices. The project resulted in 134 journal publications and 6 PhD theses with all the PhD graduates currently working in either academia or industry within the United States. The basic understanding on the stability of mesoscale polar states and pattern evolution achieved by the project improved our ability to control and engineer properties of ferroelectric thin films and heterostructures for potential applications in nanoscale electronic devices.

36 MATERIALS SCIENCE↗

Photoabsorption and Stability in Triple-Cation Perovskites Influenced by Interfacial Engineering of the Collector

Charge carrier dynamics in three-dimensional (3D) perovskites is critical to understand for enhancing device performance since the photoabsorption mechanism in perovskites influences key functional devices such as photodetectors and solar cells. Temperature-dependent optoelectronic transport measurements were conducted on our triple cation formulation for the first time from 4 K to 300 K to investigate the role of an interfacial Ti underlayer, beneath the conventional Au collector electrode. The photocurrent was 10X larger with the use of a Ti interfacial layer compared to only Au, where device measurements were made using a broadband white light source at room temperature. As temperature increased from 4 K, the photocurrent increased in both cases, consistent with the semiconducting nature of the triple-cation absorber. Besides computing the responsivity as a function of power and temperature, time-domain measurements with ON/OFF pulses of incident white light, showed the switching time constants to be in the tens to few hundred milliseconds range, and largely temperature-invariant for the two contacts examined. Finally, we constructed solar cells with the same triple cation absorber, in an n-i-p architecture with a Spiro-OMeTAD hole transport layer, but the collector was composed of both types of contacts. Exposing our devices to moisture-rich conditions of up to 70% relative humidity showed the Au/Ti contacted devices to be more robust. Here, our experimental results demonstrate that the addition of a Ti interlayer improves collector efficiency through the photoabsorption process while also potentially stabilizing the solar cells, compared to the bare Au, in moisture-rich environments

optoelectronics↗

Magnetic‐Field‐Switchable Laser via Optical Pumping of Rubrene

Abstract Volumetric optical imaging of magnetic fields is challenging with existing magneto‐optical materials, motivating the search for dyes with strong magnetic field interactions, distinct emission spectra, and an ability to withstand high photon flux and incorporation within samples. Here, the magnetic field effect on singlet‐exciton fission is exploited to demonstrate spatial imaging of magnetic fields in a thin film of rubrene. Doping rubrene with the high‐quantum yield dye dibenzotetraphenylperiflanthene (DBP) is shown to enable optically pumped, slab waveguide lasing. This laser is magnetic‐field‐switchable: when operated just below the lasing threshold, application of a 0.4 T magnetic field switches the device between nonlasing and lasing modes, accompanied by an intensity modulation of +360%. This is thought to be the first demonstration of a magnetically switchable laser, as well as the largest magnetically induced change in emission brightness in a singlet‐fission material to date. These results demonstrate that singlet‐fission materials are promising materials for magnetic sensing applications and could inspire a new class of magneto‐optical modulators.

36 MATERIALS SCIENCE↗

Optical-Gating of Spin-based Quantum States (Final Report)

This project developed a generalizable strategy for optical control of spin-based quantum states through the Photoisomerization-Induced Spin–Charge Excited State (PISCES) process, in which a photochromic spirooxazine ligand bound to an electronically bistable metal complex enables reversible, room-temperature optical switching of spin states in both dilute matrices and the solid state. A multidisciplinary team integrated synthesis, spectroscopy, theory, and surface science to establish design principles for opto-spintronic quantum materials. Systematic structure–property studies across four spirooxazine series revealed that donor–π–acceptor interactions govern thermal isomerization, which proceeds via a rotational pathway. Pulsed EPR measurements demonstrated millisecond-scale coherence times in cobalt-dioxolene-spirooxazine complexes, establishing their promise as optically addressable molecular qubits; the approach was extended to Cu(II), Ni(II), and lanthanide complexes, including optical modulation of zero-field splittings and clock transitions. Two-dimensional IR spectroscopy resolved picosecond ground-state population exchange dynamics, while ab initio calculations elucidated photoisomerization mechanisms and parametrized Hamiltonians for spin relaxation and decoherence. Toward device integration, the team fabricated 2D polymer scaffolds for covalent qubit organization, developed tip-enhanced Raman imaging of molecular monolayers, and demonstrated optical gating of gate voltage in spirooxazine-graphene field-effect transistors. The project produced numerous publications, dissertations, and presentations, and trained over 30 researchers.

2D polymers↗

Resistive Switching of Spinel Li 4 Ti 5 O 12 Lithium-Ion Battery Material for Neuromorphic Computing

The rapid rise of AI has exposed significant limitations in conventional Von Neumann computing architecture, particularly in regard to speed and energy efficiency. To address these challenges, researchers are exploring a brain-inspired neuromorphic architecture that mimics biological neural networks, enabling massive parallel processing with reduced power consumption for complex AI computational demands. Recent interest has focused on utilizing battery electrodes and solid electrolyte materials for their resistive switching properties in developing a neuromorphic architecture. These properties are precisely tuned through local- and bulk-level chemical composition modifications via voltage bias stimuli. In this study, we demonstrate fabricating a three-terminal lithium-ion electrochemical transistor based on lithium titanium oxide (Li 4 Ti 5 O 12 ), a popular lithium-ion battery anode material. We deposited and characterized LTO thin films using RF sputtering, demonstrating a 6 orders of magnitude increase in electronic conductivity upon lithiation, with conductivity plateauing after 20% lithiation. Density functional theory calculations revealed transformation from the insulating to conducting state, supported by experimental characterization through X-Ray Photoelectron Spectroscopy (XPS) and Direct Current (DC) polarization analyses. The fabricated transistor consisted of LTO as the channel layer, gold as source/drain terminals, lithium phosphorus oxynitride (LiPON) as the lithium-ion conductor, and copper as the gate terminal. The device exhibited clear hysteresis in transfer characteristics due to lithium insertion/extraction processes. Long-term potentiation (LTP) and long-term depression (LTD) measurements showed an asymmetric ratio of 1.425 and maximum/minimum conductance ratio of 7.83. When implemented in a deep neural network (DNN) for MNIST handwritten digit recognition, the device achieved 92.03% accuracy over 20 training epochs. Detailed transport mechanism analysis revealed the crucial role of oxygen vacancies and interface effects in device operation. Our preliminary findings establish LTO-based lithium-ion electrochemical transistors as promising candidates for energy-efficient neuromorphic computing applications, offering potential solutions to traditional Von Neumann architecture limitations.

25 ENERGY STORAGE↗

First-principles investigation of the resistive switching energetics in monolayer MoS 2 : insights into metal diffusion and adsorption

A deeper understanding of resistive switching (RS) in 2D materials is essential for advancing neuromorphic computing. The Dissociation-Diffusion-Adsorption (DDA) model offers a useful framework for probing RS mechanisms in non-volatile memory (NVM) and in-memory computing. We have employed first-principles density functional theory (DFT) to explore dissociation, diffusion, and adsorption phenomena within the DDA model, focusing on the interactions between exemplary metal atoms (Au, Ag, Cu) and monolayer MoS 2 . Nudged elastic band (NEB) calculations evaluated diffusion barriers in pristine and sulfur-vacancy MoS 2 . Charged systems were modeled to assess the impact of applied bias on migration pathways. We also examined metal dissociation from bulk electrodes and adsorption at S vacancies. Ag/MoS 2 shows the lowest dissociation barrier (~0.034 eV), while Au and Cu exhibit similar values (~0.32 eV). These insights highlight Ag as a promising candidate for low-energy RS applications and provide guidance for optimizing switching efficiency in 2D memory devices.

Atomistic models↗

On the Ordering Mechanism of Cu + in 2D van der Waals Multiferroic CuCrP 2 S 6

CuCrP 2 S 6 is a van der Waals multiferroic where the tunable Cu + sublattice underpins its exceptional ferroelectric and electronic switching properties. Yet, the microscopic mechanism governing Cu + ordering has remained elusive. Here, we combine single-crystal X-ray and neutron diffraction with pair distribution function analysis to uncover a temperature-driven evolution of Cu + ordering, giving rise to an incommensurate quasi-antipolar phase between the paraelectric and antiferroelectric states. The modulation originates from correlated Cu + occupancy redistribution coupled to breathing distortion of surrounding S 3 triangles, establishing a symmetry-adapted lattice distortion mode. Diffuse scattering persisting over 35 K above the transition confirms that the structural instability follows an order-disorder mechanism. The spontaneous off-centering of Cu + positions CuCrP 2 S 6 as a model platform for correlated order-disorder phenomena in 2D layered ferroics, and provides design principles for next-generation memory and logic devices.

ferroelectrics↗

Ferroelectric Switching of Pure Spin Polarization in Two-Dimensional Electron Gas

Two-dimensional electron gas (2DEG) created at compound interfaces can exhibit a broad range of exotic physical phenomena, including quantum Hall phase, emergent ferromagnetism, and superconductivity. Although electron spin plays key roles in these phenomena, the fundamental understanding and application prospects of such emergent interfacial states have been largely impeded by the lack of purely spin-polarized 2DEG. In this paper, by first-principles calculations of the multiferroic superlattice GeTe/MnTe, we find the ferroelectric polarization of GeTe is concurrent with the half-metallic 2DEG at interfaces. Remarkably, the pure spin polarization of the 2DEG can be created and annihilated by polarizing and depolarizing the ferroelectrics and can be switched (between pure spin-up and pure spin-down) by flipping the ferroelectric polarization. Given the electric-field amplification effect of ferroelectric electronics, we envision multiferroic superlattices could open up new opportunities for low-power, high-efficiency spintronic devices such as spin field-effect transistors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Self-Intercalation Tunable Interlayer Exchange Coupling in a Synthetic van der Waals Antiferromagnet

One of the most promising avenues in 2D materials research is the synthesis of antiferromagnets employing 2D van der Waals (vdW) magnets. However, it has proven challenging, due in part to the complicated fabrication process and undesired adsorbates as well as the significantly deteriorated ferromagnetism at atomic layers. Here, the engineering of the antiferromagnetic (AFM) interlayer exchange coupling between atomically thin yet ferromagnetic CrTe 2 layers in an ultra-high vacuum-free 2D magnetic crystal, Cr 5 Te 8 is reported. By self-introducing interstitial Cr atoms in the vdW gaps, the emergent AFM ordering and the resultant giant magnetoresistance effect are induced. A large negative magnetoresistance (10%) with a plateau-like feature is revealed, which is consistent with the AFM interlayer coupling between the adjacent CrTe 2 main layers in a temperature window of 30 K below the Néel temperature. Notably, the AFM state has a relatively weak interlayer exchange coupling, allowing a switching between the interlayer AFM and ferromagnetic states at moderate magnetic fields. Here this work represents a new route to engineering low-power devices that underpin the emerging spintronic technologies, and an ideal laboratory to study 2D magnetism.

36 MATERIALS SCIENCE↗