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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
NASA NTRS2010

Non-Geiger-Mode Single-Photon Avalanche Detector with Low Excess Noise

This design constitutes a self-resetting (gain quenching), room-temperature operational semiconductor single-photon-sensitive detector that is sensitive to telecommunications optical wavelengths and is scalable to large areas (millimeter diameter) with high bandwidth and efficiencies. The device can detect single photons at a 1,550-nm wavelength at a gain of 1 x 10(exp 6). Unlike conventional single photon avalanche detectors (SPADs), where gain is an extremely sensitive function to the bias voltage, the multiplication gain of this device is stable at 1 x 10(exp 6) over a wide range of bias from 30.2 to 30.9 V. Here, the multiplication gain is defined as the total number of charge carriers contained in one output pulse that is triggered by the absorption of a single photon. The statistics of magnitude of output signals also shows that the device has a very narrow pulse height distribution, which demonstrates a greatly suppressed gain fluctuation. From the histograms of both pulse height and pulse charge, the equivalent gain variance (excess noise) is between 1.001 and 1.007 at a gain of 1 x 10(exp 6). With these advantages, the device holds promise to function as a PMT-like photon counter at a 1,550- nm wavelength. The epitaxial layer structure of the device allows photons to be absorbed in the InGaAs layer, generating electron/hole (e-h) pairs. Driven by an electrical field in InGaAs, electrons are collected at the anode while holes reach the multiplication region (InAlAs p-i-n structure) and trigger the avalanche process. As a result, a large number of e-h pairs are created, and the holes move toward the cathode. Holes created by the avalanche process gain large kinetic energy through the electric field, and are considered hot. These hot holes are cooled as they travel across a p -InAlAs low field region, and are eventually blocked by energy barriers formed by the InGaAsP/ InAlAs heterojunctions. The composition of the InGaAsP alloy was chosen to have an 80 meV valance band offset with InAlAs, which is high enough to hinder the transport of the already cooled holes. Being stopped by the energy barrier, holes are accumulated at the junctions to shield the electric field, resulting in a decrease of the electric field in the multiplication region. Because the impact ionization rate is extremely sensitive to the magnitude of the electric field, the field-screening effect drastically reduces the impact ionization rate and quenches the output signals. After the avalanche pulse signal is self-quenched, the accumulated holes at the InGaAsP/ InAlAs interface escape the energy barrier through thermal excitation and tunneling and finally leave the device. The device is thus reset and ready for subsequent photon detection. This recovery time is controlled by the height of the energy barrier and the hole-cooling rate.

Zhao, Kai↗
DOE OSTI2021

Epitaxy, exfoliation, and strain-induced magnetism in rippled Heusler membranes

Single-crystalline membranes of functional materials enable the tuning of properties via extreme strain states; however, conventional routes for producing membranes require the use of sacrificial layers and chemical etchants, which can both damage the membrane and limit the ability to make them ultrathin. Here we demonstrate the epitaxial growth of the cubic Heusler compound GdPtSb on graphene-terminated Al 2 O 3 substrates. Despite the presence of the graphene interlayer, the Heusler films have epitaxial registry to the underlying sapphire, as revealed by x-ray diffraction, reflection high energy electron diffraction, and transmission electron microscopy. The weak Van der Waals interactions of graphene enable mechanical exfoliation to yield free-standing GdPtSb membranes, which form ripples when transferred to a flexible polymer handle. Whereas unstrained GdPtSb is antiferromagnetic, measurements on rippled membranes show a spontaneous magnetic moment at room temperature, with a saturation magnetization of 5.2 bohr magneton per Gd. First-principles calculations show that the coupling to homogeneous strain is too small to induce ferromagnetism, suggesting a dominant role for strain gradients. Our membranes provide a novel platform for tuning the magnetic properties of intermetallic compounds via strain (piezomagnetism and magnetostriction) and strain gradients (flexomagnetism).

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Unraveling the electronic structure and magnetic transition evolution across monolayer, bilayer, and multilayer ferromagnetic Fe 3 GeTe 2

Two-dimensional (2D) van der Waals (vdW) magnets have sparked widespread attention due to their potential in spintronic applications as well as in fundamental physics. Ferromagnetic vdW compound Fe 3 GeTe 2 (FGT) and its Ga variants have garnered significant interest due to their itinerant magnetism, correlated states, and high magnetic transition temperature. Experimental studies have demonstrated the tunability of FGT’s Curie temperature, T C , through adjustments in quintuple layer numbers (QL) and carrier concentrations, n. However, the underlying mechanism remains elusive. In this study, we employ molecular beam epitaxy (MBE) to synthesize 2D FGT films down to 1 QL with precise layer control, facilitating an exploration of the band structure and the evolution of itinerant carrier density. Angle-resolved photoemission spectroscopy (ARPES) reveals significant band structure changes at the ultra-thin limit, while first-principles calculations elucidate the band evolution from 1 QL to bulk, largely governed by interlayer coupling. Additionally, we find that n is intrinsically linked to the number of QL and temperature, with a critical value triggering the magnetic phase transition. Our findings underscore the pivotal role of band structure and itinerant electrons in governing magnetic phase transitions in such 2D vdW magnetic materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Controlling selective nucleation and growth of dysprosium islands on graphene by metal intercalation

We report metal intercalation is an effective method to modify the physical and chemical properties of low-dimensional systems such as epitaxial graphene. Here, we show that the nucleation and growth of metal nanostructures on epitaxial graphene on SiC(0001) can be dramatically changed by metal intercalation. Using scanning tunneling microscopy experiments, we demonstrate that dysprosium (Dy) metal islands are selectively nucleated on the area with Dy intercalation under both graphene and carbon buffer layers, while the adjacent area with only buffer layer intercalated remains relatively bare. Using first-principles calculations based on density functional theory, we show that adsorption of Dy adatom on the preferred nucleation area is energetically more favorable than on other areas. Moreover, changes in the electronic structure and the interlayer spacing upon Dy intercalation obtained from our calculations are also consistent with experimental observations. Our results indicate that metal intercalation is a promising way to manipulate the interaction between graphene and deposited adatoms.

2-dimensional systems↗
DOE OSTI2020

Massive Suppression of Proximity Pairing in Topological ( Bi 1 - x Sb x ) 2 Te 3 Films on Niobium

Interfacing bulk conducting topological Bi 2 Se 3 films with s-wave superconductors initiates strong superconducting order in the nontrivial surface states. Yet, bulk insulating topological (Bi 1-x Sb x ) 2 Te 3 films on bulk Nb instead exhibit a giant attenuation of surface superconductivity, even for films only two-layers thick. This massive suppression of proximity pairing is shown by ultrahigh-resolution band mappings and by contrasting quantified superconducting gaps with those of heavily n-doped topological Bi 2 Se 3 /Nb. The results underscore the limitations of using superconducting proximity effects to realize topological superconductivity in nearly intrinsic systems.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Tuning the Chern number in quantum anomalous Hall insulators

A quantum anomalous Hall (QAH) state is a two-dimensional topological insulating state that has a quantized Hall resistance of h/(Ce 2 ) and vanishing longitudinal resistance under zero magnetic field (where h is the Planck constant, e is the elementary charge, and the Chern number C is an integer). The QAH effect has been realized in magnetic topological insulators and magic-angle twisted bilayer graphene. However, the QAH effect at zero magnetic field has so far been realized only for C = 1. Here we realize a well quantized QAH effect with tunable Chern number (up to C = 5) in multilayer structures consisting of alternating magnetic and undoped topological insulator layers, fabricated using molecular beam epitaxy. The Chern number of these QAH insulators is determined by the number of undoped topological insulator layers in the multilayer structure. Moreover, we demonstrate that the Chern number of a given multilayer structure can be tuned by varying either the magnetic doping concentration in the magnetic topological insulator layers or the thickness of the interior magnetic topological insulator layer. We develop a theoretical model to explain our experimental observations and establish phase diagrams for QAH insulators with high, tunable Chern number. Furthermore, the realization of such insulators facilitates the application of dissipationless chiral edge currents in energy-efficient electronic devices, and opens up opportunities for developing multi-channel quantum computing and higher-capacity chiral circuit interconnects.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Surface triggered stabilization of metastable charge-ordered phase in SrTiO 3

Charge ordering (CO), characterized by a periodic modulation of electron density and lattice distortion, has been a fundamental topic in condensed matter physics, serving as a potential platform for inducing novel functional properties. The charge-ordered phase is known to occur in a doped system with high d-electron occupancy, rather than low occupancy. Here, we report the realization of the charge-ordered phase in electron-doped (100) SrTiO 3 epitaxial thin films that have the lowest d-electron occupancy i.e., d 1 -d 0 . Theoretical calculation predicts the presence of a metastable CO state in the bulk state of electron-doped SrTiO 3 . Atomic scale analysis reveals that (100) surface distortion favors electron-lattice coupling for the charge-ordered state, and triggering the stabilization of the CO phase from a correlated metal state. This stabilization extends up to six unit cells from the top surface to the interior. Our approach offers an insight into the means of stabilizing a new phase of matter, extending CO phase to the lowest electron occupancy and encompassing a wide range of 3d transition metal oxides.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Surface photovoltage spectroscopy observes junctions and carrier separation in gallium nitride nanowire arrays for overall water-splitting

Gallium nitride (GaN) nanowire arrays on silicon are able to drive the overall water-splitting reaction with up to 3.3% solar-to-hydrogen efficiency. Photochemical charge separation is key to the operation of these devices, but details are difficult to observe experimentally because of the number of components and interfaces. Here, we use surface photovoltage spectroscopy to study charge transfer in i-, n-, and p-GaN nanowire arrays on n+ -Si wafers in the presence and absence of Rh/Cr 2 O 3 co-catalysts. The effect of the space charge layer and sub-bandgap defects on majority and minority carrier transport can be clearly observed, and estimates of the built-in potential of the junctions can be made. Transient illumination of the p-GaN/n + -Si junction generates up to -1.4 V surface photovoltage by carrier separation along the GaN nanowire axis. This process is central to the overall water-splitting function of the n + -Si/p-GaN/Rh/Cr 2 O 3 nanowire array. Overall, these results improve our understanding of photochemical charge transfer and separation in group III–V semiconductor nanostructures for the conversion of solar energy into fuels.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Engineering new limits to magnetostriction through metastability in iron-gallium alloys

Magnetostrictive materials transduce magnetic and mechanical energies and when combined with piezoelectric elements, evoke magnetoelectric transduction for high-sensitivity magnetic field sensors and energy-efficient beyond-CMOS technologies. The dearth of ductile, rare-earth-free materials with high magnetostrictive coefficients motivates the discovery of superior materials. Fe 1- x Ga x alloys are amongst the highest performing rare-earth-free magnetostrictive materials; however, magnetostriction becomes sharply suppressed beyond x = 19% due to the formation of a parasitic ordered intermetallic phase. Here, we harness epitaxy to extend the stability of the BCC Fe 1- x Ga x alloy to gallium compositions as high as x = 30% and in so doing dramatically boost the magnetostriction by as much as 10x relative to the bulk and 2x larger than canonical rare-earth based magnetostrictors. A Fe 1- x Ga x - [Pb(Mg 1/3 Nb 2/3 )O 3 ] 0.7 -[PbTiO 3 ] 0.3 (PMN-PT) composite magnetoelectric shows robust 90° electrical switching of magnetic anisotropy and a converse magnetoelectric coefficient of 2.0 × 10 -5 s m -1 . When optimally scaled, this high coefficient implies stable switching at ~80 aJ per bit.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Orientation-dependent structural properties during growth and growth mechanism of CoO films

The orientation-dependent local structural properties of CoO films on sapphire substrates during growth were investigated through linearly-polarized extended X-ray absorption fine structure (EXAFS) measurements. Specifically, CoO(1 1 1) and (100) crystals with a rock-salt structure (Fm3m) were epitaxially grown on alpha-Al2O3(0001) and (1012) substrates, respectively, at 700 degrees C using a radio-frequency sputtering system. The local structural properties of CoO films in the in-plane and out-of-plane orientations were quantitatively determined using linearly-polarized EXAFS at the Co K-edge during growth. The EXAFS analysis revealed that during the initial stages of growth, the local structural properties exhibit significant differences compared to thick films, with short atomic distances and large (small) Debye-Waller factors observed in the out-of-plane (in-plane) orientations. The local structural strain mostly diminished when approximately 20 CoO layers accumulated on the substrate. Density functional theory (DFT) calculations further supported these findings by confirming that cobalt atoms initially form stable bonds with the sapphire surface, leading to the simultaneous growth of oxygen and cobalt layers in a coordinated manner through layer-by-layer growth.

36 MATERIALS SCIENCE↗
DOE OSTI2023

From Stoner to local moment magnetism in atomically thin Cr2Te3

Abstract The field of two-dimensional (2D) ferromagnetism has been proliferating over the past few years, with ongoing interests in basic science and potential applications in spintronic technology. However, a high-resolution spectroscopic study of the 2D ferromagnet is still lacking due to the small size and air sensitivity of the exfoliated nanoflakes. Here, we report a thickness-dependent ferromagnetism in epitaxially grown Cr 2 Te 3 thin films and investigate the evolution of the underlying electronic structure by synergistic angle-resolved photoemission spectroscopy, scanning tunneling microscopy, x-ray absorption spectroscopy, and first-principle calculations. A conspicuous ferromagnetic transition from Stoner to Heisenberg-type is directly observed in the atomically thin limit, indicating that dimensionality is a powerful tuning knob to manipulate the novel properties of 2D magnetism. Monolayer Cr 2 Te 3 retains robust ferromagnetism, but with a suppressed Curie temperature, due to the drastic drop in the density of states near the Fermi level. Our results establish atomically thin Cr 2 Te 3 as an excellent platform to explore the dual nature of localized and itinerant ferromagnetism in 2D magnets.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Effect of correlated oxide electrodes on disorder pinning and thermal roughening of ferroelectric domain walls in epitaxial PbZr 0.2 Ti 0.8 O 3 thin films

We report the competing effects of disorder pinning and thermal roughening on ferroelectric domain walls as a function of temperature in epitaxial PbZr 0.2 Ti 0.8 O 3 thin films deposited on (001) SrTiO 3 substrates buffered by three types of correlated oxide electrodes, La 0.67 Sr 0.33 MnO 3 , LaNiO 3 , and SrIrO 3 . Piezo-response force microscopy studies show that the 50 nm PbZr 0.2 Ti 0.8 O 3 films are uniformly polarized in the as-grown states, with the patterned domain structures persisting above 700 °C. For all three types of films, the domain wall roughness is dominated by 2D random bond disorder at room temperature, and transitions to 1D thermal roughening upon heating. The roughness exponent ζ increases progressively from 0.3 to 0.5 within a temperature window that depends on the bottom conducting oxide type, from which we extracted the distribution of disorder pinning energy. Lastly, we discuss the possible origins of the disorder pinning and the effect of the correlated oxide electrodes on the energy landscape of DW motion.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Controlled Nucleation and Stabilization of Ferroelectric Domain Wall Patterns in Epitaxial (110) Bismuth Ferrite Heterostructures

Ferroelectric domain walls, topological entities separating domains of uniform polarization, are promising candidates as active elements for nanoscale memories. In such applications, controlled nucleation and stabilization of domain walls are critical. In this work, using in situ transmission electron microscopy and phase-field simulations, a controlled nucleation of vertically oriented 109° domain walls in (110)-oriented BiFeO 3 (BFO) thin films is reported. In the switching experiment, reversed domains that are nucleated preferentially at the nanoscale edges of the “crest and sag” pattern-like electrode under external bias subsequently grow into a stable stripe configuration. In addition, when triangular pockets (with an in-plane polarization component) are present, these domain walls are pinned to form stable flux-closure domains. Phase field simulations show that i) field enhancement at the edges of the electrode causes site-specific domain nucleation, and ii) the local electrostatics at the domain walls drives the formation of flux closure domains, thus stabilizing the striped pattern, irrespective of the initial configuration. The results demonstrate how flux closure pinning can be exploited in conjunction with electrode patterning and substrate orientation to achieve a desired topological defect configuration. These insights constitute critical advancements in exploiting domain walls in next generation ferroelectronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Axion insulator state in hundred-nanometer-thick magnetic topological insulator sandwich heterostructures

Abstract An axion insulator is a three-dimensional (3D) topological insulator (TI), in which the bulk maintains the time-reversal symmetry or inversion symmetry but the surface states are gapped by surface magnetization. The axion insulator state has been observed in molecular beam epitaxy (MBE)-grown magnetically doped TI sandwiches and exfoliated intrinsic magnetic TI MnBi 2 Te 4 flakes with an even number layer. All these samples have a thickness of ~ 10 nm, near the 2D-to-3D boundary. The coupling between the top and bottom surface states in thin samples may hinder the observation of quantized topological magnetoelectric response. Here, we employ MBE to synthesize magnetic TI sandwich heterostructures and find that the axion insulator state persists in a 3D sample with a thickness of ~ 106 nm. Our transport results show that the axion insulator state starts to emerge when the thickness of the middle undoped TI layer is greater than ~ 3 nm. The 3D hundred-nanometer-thick axion insulator provides a promising platform for the exploration of the topological magnetoelectric effect and other emergent magnetic topological states, such as the high-order TI phase.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Magnetic Texture in Insulating Single Crystal High Entropy Oxide Spinel Films

Magnetic insulators are important materials for a range of next-generation memory and spintronic applications. Structural constraints in this class of devices generally require a clean heterointerface that allows effective magnetic coupling between the insulating layer and the conducting layer. However, there are relatively few examples of magnetic insulators that can be synthesized with surface qualities that would allow these smooth interfaces and precisely tuned interfacial magnetic exchange coupling, which might be applicable at room temperature. In this work, we demonstrate an example of how the configurational complexity in the magnetic insulator layer can be used to realize these properties. The entropy-assisted synthesis is used to create single-crystal (Mg 0.2 Ni 0.2 Fe 0.2 Co 0.2 Cu 0.2 )Fe 2 O 4 films on substrates spanning a range of strain states. These films show smooth surfaces, high resistivity, and strong magnetic responses at room temperature. Furthermore, local and global magnetic measurements further demonstrate how strain can be used to manipulate the magnetic texture and anisotropy. These findings provide insight into how precise magnetic responses can be designed using compositionally complex materials that may find application in next-generation magnetic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Challenges in atomic layer etching of gallium nitride using surface oxidation and ligand-exchange

Two atomic layer etching (ALE) methods were studied for crystalline GaN, based on oxidation, fluorination, and ligand exchange. Etching was performed on unintentionally doped GaN grown by hydride vapor phase epitaxy. For the first step, the GaN surfaces were oxidized using either water vapor or remote O 2 -plasma exposure to produce a thin oxide layer. Removal of the surface oxide was addressed using alternating exposures of hydrogen fluoride (HF) and trimethylgallium (TMG) via fluorination and ligand exchange, respectively. Several HF and TMG super cycles were implemented to remove the surface oxide. Each ALE process was monitored in situ using multiwavelength ellipsometry. X-ray photoelectron spectroscopy was employed for the characterization of surface composition and impurity states. Additionally, the thermal and plasma-enhanced ALE methods were performed on patterned wafers and transmission electron microscopy (TEM) was used to measure the surface change. The x-ray photoelectron spectroscopy measurements indicated that F and O impurities remained on etched surfaces for both ALE processes. Ellipsometry indicated a slight reduction in thickness. TEM indicated a removal rate that was less than predicted. In conclusion, we suggest that the etch rates were reduced due to the ordered structure of the oxide formed on crystalline GaN surfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Characterization of Nb films for superconducting qubits using phase boundary measurements

Continued advances in superconducting qubit performance require more detailed understandings of the many sources of decoherence. Within these devices, two-level systems arise due to defects, interfaces, and grain boundaries and are thought to be a major source of qubit decoherence at millikelvin temperatures. In addition to Al, Nb is a commonly used metallization layer in superconducting qubits. Consequently, a significant effort is required to develop and qualify processes that mitigate defects in Nb films. As the fabrication of complete superconducting qubits and their characterization at millikelvin temperatures is a time and resource intensive process, it is desirable to have measurement tools that can rapidly characterize the properties of films and evaluate different treatments. Here, we show that measurements of the variation of the superconducting critical temperature T c with an applied external magnetic field H (of the phase boundary T c – H⁠) performed with very high-resolution show features that are directly correlated with the structure of the Nb films. In combination with x-ray diffraction measurements, we show that one can even distinguish variations in the size and crystal orientation of the grains in a Nb film by small but reproducible changes in the measured superconducting phase boundary.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Proximity Magnetism in Mn(Bi,Sb) 2 Te 4 –(Bi,Sb) 2 Te 3 /MnTe Natural Heterostructures

Magnetic topological insulators and their heterostructures provide significant opportunities to couple band topology with a nontrivial spin configuration for enhanced spintronic device performance, as well as designing magnetoelectric systems and functionalities. We find that Mn interdiffusion from MnTe when interfaced with (Bi,Sb) 2 Te 3 stabilizes as self-organized Mn(Bi,Sb) 2 Te 4 septuple lamellae among alternating (Bi,Sb) 2 Te 3 quintuple layers, as observed using scanning transmission electron microscopy and depth-sensitive polarized neutron reflectometry. We further demonstrate a valuable combination of magnetic and topological orders in these naturally formed Mn(Bi,Sb) 2 Te 4 –(Bi,Sb) 2 Te 3 heterostructures, which are exchange-coupled with MnTe. Magnetotransport experiments and quantum magnetism simulations reveal that, above its own Néel temperature T N ∼ 20 K, Mn(Bi,Sb) 2 Te 4 mediates the exchange field leading to an anomalous Hall effect at the (Bi,Sb) 2 Te 3 /MnTe interface, with an enhanced interfacial T N exceeding 200 K, approaching that of the bulk MnTe. This magnetic interface, in turn, allows a robust and deterministic spin–orbit torque switching without an external magnetic field at a low critical current density of 3 × 10 5 A cm –2 . The antiferromagnetically coupled architecture of Mn(Bi,Sb) 2 Te 4 –(Bi,Sb) 2 Te 3 /MnTe, featuring magnetic and topological proximity effects across a chalcogenide backbone, is rich in fundamental interface physics and holds the potential for practical applications in spintronics.

magnetic topological insulator↗