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At least 109 records · Page 6

Heterogeneous Morphologies and Hardness of Co-Sputtered Thin Films of Concentrated Cu-Mo-W Alloys

Heterogeneous microstructures in Cu-Mo-W alloy thin films formed by magnetron co-sputtering immiscible elements with concentrated compositions are characterized using scanning transmission electron microscopy (STEM) and nanoindentation. In this work, we modified the phase separated structure of a Cu-Mo immiscible system by adding W, which impedes surface diffusion during film growth. The heterogeneous microstructures in the Cu-Mo-W ternary system exhibited bicontinuous matrices and agglomerates composed of Mo(W)-rich phase. This is unique, as these are the slower-diffusing species, contrasting past reports of binary Cu-Mo thin films that exhibited Cu-rich agglomerates. The bicontinuous matrices comprised of Cu-rich and Mo(W)-rich phases exhibited bilayer thicknesses of less than 5 nm. The hardness of these thin films measured using nanoindentation is reported and compared to similar multilayers and nanocomposites in binary systems.

36 MATERIALS SCIENCE↗

Growth of Crystallographically Aligned PbSe Films of Controlled Thickness on Amorphous Substrates

Lead selenide (PbSe) has extensively been investigated due to its thermoelectric and photoconductive properties. More recently, predictions of emergent properties have focused synthetic efforts on preparing ultra-smooth layers of crystallographically aligned PbSe layers with a thickness equal to an integer number of monolayers. While rough films are typically formed through Volmer-Weber growth on heated substrates, we report the data presented herein indicates that a crystallographically aligned, ultrathin layer with a defined number of PbSe layers forms on mostly amorphous Mo-Se and V-Se coated Si substrates during nominally room temperature deposition. Since the films are uniform in thickness, the number of PbSe bilayers formed depends on the amount of Pb (or Se) deposited. If the amount of Pb deposited is close to that required for an integral number of unit cells and there is sufficient Se, Laue oscillations are present in the as-deposited samples. The Laue oscillations reflect the quality and uniformity of the crystalline PbSe domains. This study demonstrates that the substrate does not need to be crystalline to form uniform, crystallographically aligned, integer monolayer thick PbSe films. These results suggest that tuning the strength of interactions be-tween substrate and growing film is necessary to form smooth, crystallographically aligned layers. The substrate does not need to be crystalline for these interactions to be strong enough to enable growth of crystallographically aligned films.

36 MATERIALS SCIENCE↗

Superconductivity in Ruddlesden–Popper nickelates: a review of recent progress, focusing on thin films

The discovery of superconductivity with Tc ∼ 80 K in the nickelate Ruddlesden-Popper bilayer La3Ni2O7 at high pressure has opened a new platform for unconventional superconductivity, followed by the subsequent observation of superconductivity in trilayer La4Ni3O10, also at high pressure. Remarkably, ambient-pressure superconductivity was also observed recently in La3Ni2O7 ultra-thin films when grown on substrates that provide compressive strain. This discovery significantly extends the type of experimental techniques that can be used in nickelates, previously limited due to the high-pressure constraint. Discussing the similarities and differences among these nickel oxides will provide new insights into understanding the mechanism of high-Tc superconductivity in correlated electron systems. In this paper, we review the experimental and theoretical progress on Ruddlesden–Popper nickelates, with emphasis on thin films, and discuss future perspectives and research directions.

Zhang, Yang [ORNL] (ORCID:0000000336235883)↗

Reducing the Strain Required for Ambient‐Pressure Superconductivity in Ruddlesden‐Popper Bilayer Nickelates

ABSTRACT The discovery of high‐temperature superconductivity in pressurized bulk Ruddlesden‐Popper (RP) bilayer nickelates has prompted the conjecture that epitaxial compressive strain might mimic essential aspects of hydrostatic pressure. The realization of superconductivity in films on SrLaAlO 4 (001) (SLAO) supports this correspondence, yet it remains unclear whether the pressure–temperature phase diagram of RP bilayer nickelates can be systematically mapped (and studied at ambient pressure) as a function of epitaxial strain. To this end, experimental access near the elusive edge of the superconducting phase boundary would provide invaluable insight into the nature of the superconducting state and the ground state from which it emerges. Here we report superconducting RP bilayer nickelates grown on LaAlO 3 (001) (LAO), where the compressive strain required for ambient‐pressure superconductivity is nearly halved to −1.2%. These films exhibit a superconducting onset above 10 K and reach zero resistance at 3 K, with normal‐state transport properties differing from those of films grown on SLAO. Our comparative study shows that strain–rather than interfacial structure is the primary factor governing the superconductivity and normal‐state properties. This work offers a new opportunity to probe emergent phenomena near the superconducting phase boundary in the strain–temperature phase diagram of RP bilayer nickelates.

Tarn, Yaoju [Department of Applied Physics Stanfor↗

Tuning electrical and interfacial thermal properties of bilayer MoS2 via electrochemical intercalation

Layered two-dimensional (2D) materials such as MoS 2 have attracted much attention for nano- and opto-electronics. Recently, intercalation (e.g. of ions, atoms, or molecules) has emerged as an effective technique to modulate material properties of such layered 2D films reversibly. We probe both the electrical and thermal properties of Li-intercalated bilayer MoS 2 nanosheets by combining electrical measurements and Raman spectroscopy. Furthermore, we demonstrate reversible modulation of carrier density over more than two orders of magnitude (from 0.8 × 10 12 to 1.5 × 10 14 cm -2 ), and we simultaneously obtain the thermal boundary conductance between the bilayer and its supporting SiO 2 substrate for an intercalated system for the first time. This thermal coupling can be reversibly modulated by nearly a factor of eight, from 14 ± 4.0 MW m -2 K -1 before intercalation to 1.8 ± 0.9 MW m -2 K -1 when the MoS 2 is fully lithiated. These results reveal electrochemical intercalation as a reversible tool to modulate and control both electrical and thermal properties of 2D layers.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Coherent Electronic Band Structure of TiTe 2 /TiSe 2 Moiré Bilayer

Here, a van der Waals bonded moiré bilayer formed by sequential growth of TiSe 2 and TiTe 2 monolayers exhibits emergent electronic structure as evidenced by angle-resolved photoemission band mapping. The two monolayers adopt the same lattice orientation but incommensurate lattice constants. Despite the lack of translational symmetry, sharp dispersive bands are observed. The dispersion relations appear distinct from those for the component monolayers alone. Theoretical calculations illustrate the formation of composite bands by coherent electronic coupling despite the weak interlayer bonding, which leads to band renormalization and energy shifts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Sequential Infiltration Synthesis of Bilayer Porous Alumina Nanostructures for Broad-Angle, Broadband Antireflective Coatings

Antireflective coatings (ARCs) are thin films engineered to reduce light reflections. Delivering broadband, wide-angle performance is essential for photovoltaics, imaging, and sensing, yet truly omnidirectional antireflection remains difficult due to angle-dependent optical paths and a narrow palette of suitable refractive indices. Here, in this study, we systematically investigate an emerging class of multilayer inorganic ARCs based on conformally coated nanoporous alumina templated by intrinsically microporous polymers (PIMs) and block copolymers (BCPs). We establish a design framework that maps thickness reflectance relationships to identify thickness pairs minimizing reflection across wavelength and incidence angle. We show that deliberately separating the local reflectance minima of the top and bottom layers in bilayer nanostructures broadens the antireflective bandwidth and angular range. We show that 235-nm single-side bilayer porous alumina nanostructures achieves under 2 % reflectance from 380–750 nm for incidence angles up to 45° with less than 0.6% reflectance for incidence angles under 20°. The approach is readily extensible to additional layers or materials with refractive indices tuned via templated nanoporosity and composition, enabling practical, etch-free ARC fabrication without HF or fluorinated precursors and advancing straightforward design of broadband, wide-angle (quasi-omnidirectional) ARCs for next-generation optical systems.

antireflective coatings↗

Carrier properties of Bi(111) grown on mica and Si(111)

A comparison is presented between properties of Bi(111) films grown by Stranski-Krastanov epitaxy on Si(111) 7 × 7 and by van der Waals epitaxy on mica substrates. Thin film morphologies and electronic transport properties of Bi(111) films of variable thickness are investigated for each growth method. Atomic force micrographs for Bi(111) films on mica reveal clearly defined triangular regions consisting of layered steps with height 0.4 nm, corresponding to the Bi(111) bilayer height. Variable-temperature electronic transport measurements show the existence of a quantum confinement-induced energy gap in the film interiors, resulting in a semimetal-to-semiconductor transition. Magnetotransport analysis in a three-carrier model including metallic electrons in surface states and electrons and holes in the films' interiors provides a detailed study of densities, mobilities, and mean-free paths of the three carrier types. Further, improved electronic transport properties are found in Bi(111) films of higher thickness on mica compared to on Si(111), a likely result of the largely strain-free van der Waals epitaxial growth.

36 MATERIALS SCIENCE↗

Effect of grafting density on the two-dimensional assembly of nanoparticles

Employing grazing-incidence small-angle X-ray scattering (GISAXS) and X-ray reflectivity (XRR), we demonstrate that films composed of polyethylene glycol (PEG)-grafted silver nanoparticles (AgNPs) and gold nanoparticles (AuNPs), as well as their binary mixtures, form highly stable hexagonal structures at the vapor–liquid interface. These nanoparticles exhibit remarkable stability under varying environmental conditions, including changes in pH, mixing concentration, and PEG chain length. Short-chain PEG grafting produces dense, well-ordered films, while longer chains produce more complex, less dense quasi-bilayer structures. AuNPs exhibit higher grafting densities than AgNPs, leading to more ordered in-plane arrangements. In binary mixtures, AuNPs dominate the population at the surface, while AgNPs integrate into the system, expanding the lattice without forming a distinct binary superstructure. In conclusion, these results offer valuable insights into the structural behavior of PEG-grafted nanoparticles and provide a foundation for optimizing binary nanoparticle assemblies for advanced nanotechnology applications.

36 MATERIALS SCIENCE↗

Design of 3D Oxide–Metal Hybrid Metamaterial for Tailorable Light–Matter Interactions in Visible and Near-Infrared Region

Dielectric–metallic hybrid metamaterials exhibit extraordinary optical properties due to the light–matter interactions at the dielectric–metallic interfaces. The ability in precision control of the light–matter interactions in nanoscale is key to tailor the optical properties of hybrid metamaterials. In this work, a complex 3D framework of multilayered self-assembled BaTiO 3 (BTO)-Au hybrid thin films is demonstrated with such precision control of the light–matter interaction in nanoscale. Here, unique “bamboo-like” Au nanostructures are formed via the bilayer and trilayer stacking of BTO-Au hybrid layers with interlayers of SrTiO 3 , CeO 2 , or MgO. Different film strain states introduced by the three interlayers result in variable diameter and density of Au nanopillars. Both simulated and experimental optical data demonstrate the localized surface plasmon resonance change and hyperbolic dispersion wavelength shift in visible to near-infrared because of the effective tuning of the Au nanopillar aspect ratio and free electron density. The highly tunable optical properties along with the ferroelectric behavior and thermal robustness of the 3D hybrid film enable it to be a great candidate for multifunctional applications. This study demonstrates a unique 3D approach for precision optical property tuning and combined functionalities in oxide–metal metamaterial systems toward future integrated photonic and electronic devices.

36 MATERIALS SCIENCE↗

Exchange bias switching in an antiferromagnet/ferromagnet bilayer driven by spin-orbit torque

Here the electrical manipulation of magnetization and exchange bias in antiferromagnet/ferromagnet thin films could be of use in the development of the next generation of spintronic devices. Current-controlled magnetization switching can be driven by spin-orbit torques generated in an adjacent heavy metal layer, but these structures are difficult to integrate with exchange bias switching and tunnelling magnetoresistance measurements. Here, we report the current-induced switching of the exchange bias field in a perpendicularly magnetized IrMn/CoFeB bilayer structure using a spin-orbit torque generated in the antiferromagnetic IrMn layer. By manipulating the current direction and amplitude, independent and repeatable switching of the magnetization and exchange bias field below the blocking temperature can be achieved. The critical current density for the exchange bias switching is found to be larger than that for CoFeB magnetization reversal. X-ray magnetic circular dichroism, polarized neutron reflectometry measurements and micromagnetic simulations show that a small net magnetization within the IrMn interface plays a crucial role in these phenomena.

42 ENGINEERING↗

Interfacial magnetic vortex formation in exchange-coupled hard-soft magnetic bilayers

The exchange coupling between a hard magnetic layer MnBi and a soft magnetic layer Co-Fe has been found to significantly improve the maximum energy product. In this work, the spin structure of exchange coupled MnBi:Co-Fe bilayers is experimentally investigated by X-ray magnetic circular dichroism (XMCD) and polarized neutron reflectometry (PNR). We find that the out-of-plane magnetization reversal process of the MnBi:Co-Fe bilayer structure involves formation of a curling-type twisting of the magnetization in the film plane at low or intermediate reversal fields. Additionally, micromagnetic simulations are further performed to provide a detailed view of the spins at the curling center. Reminiscent of chiral spin structures known as spin bobbers, this curling in the exchange-coupled hard-soft magnetic bilayers is a new type of skyrmionic spin structure and worth further investigation.

36 MATERIALS SCIENCE↗

Supercurrent diode effect and finite-momentum superconductors

When both inversion and time-reversal symmetries are broken, the critical current of a superconductor can be nonreciprocal. In this work, we show that, in certain classes of two-dimensional superconductors with antisymmetric spin–orbit coupling, Cooper pairs acquire a finite momentum upon the application of an in-plane magnetic field, and, as a result, critical currents in the direction parallel and antiparallel to the Cooper pair momentum become unequal. This supercurrent diode effect is also manifested in the polarity dependence of in-plane critical fields induced by a supercurrent. These nonreciprocal effects may be found in polar SrTiO 3 film, few-layer MoTe 2 in the Td phase, and twisted bilayer graphene in which the valley degree of freedom plays a role analogous to spin.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The growth and nanothermite reaction of 2Al/3NiO multilayer thin films

Nanothermite NiO–Al is a promising material system for low gas emission heat sources; still, its reactive properties are highly dependent on material processing conditions. In the current study, sputter deposition is used to fabricate highly controlled nanolaminates comprised of alternating NiO and Al layers. Films having an overall stoichiometry of 2Al to 3NiO were produced with different bilayer thicknesses to investigate how ignition and self-sustained, high temperature reactions vary with changes to nanometer-scale periodicity and preheat conditions. Ignition studies were carried out with both hot plate and laser irradiation and compared to slow heating studies in hot-stage x-ray diffraction. Ignition behavior has bilayer thickness and heating rate dependencies. The 2Al/3NiO with λ ≤ 300 nm ignited via solid/solid diffusion mixing (activation energy, E a = 49 ± 3 kJ/mole). Multilayers having λ ≥ 500 nm required a more favorable mixing kinetics of solid/liquid dissolution into molten Al (E a = 30 ± 4 kJ/mole). This solid/liquid dissolution E a is a factor of 5 lower than that of the previously reported powder compacts due to the elimination of a passivating Al oxide layer present on the powder. The reactant mixing mechanism between 300 and 500 nm bilayer thicknesses was dependent on the ignition source's heating rate. The self-propagating reaction velocities of 2Al/3NiO multilayers varied from 0.4 to 2.5 m/s. Pre-heating nanolaminates to temperatures below the onset reaction temperatures associated with forming intermediate nickel aluminides at multilayer interfaces led to increased propagation velocities, whereas pre-heating samples above the onset temperatures inhibited subsequent attempts at laser ignition.

36 MATERIALS SCIENCE↗

Ultrafast measurements of the interfacial spin Seebeck effect in Au and rare-earth iron-garnet bilayers

We investigate picosecond spin-currents across Au/iron-garnet interfaces in response to ultrafast laser heating of the electrons in the Au film. In the picoseconds after optical heating, interfacial spin currents occur due to an interfacial temperature difference between electrons in the metal and magnons in the insulator. We report measurements of this interfacial longitudinal spin Seebeck effect between Au and rare-earth iron-garnet insulators, i.e. RE 3 Fe 5 O 12 , where RE is Y, Eu, Tb, Tm. By systematically varying the rare-earth element, we modify the total magnetic moment of the iron-garnet. We use time domain thermoreflectance (TDTR) measurements to characterize the thermal response of the bilayer to ultrafast optical heating. We use time-resolved magneto-optic Kerr effect (TR-MOKE) measurements of the Au layer to measure the time-evolution of spin accumulation in the Au film. Replacing Y with other rare-earths enhances the electron-magnon conductance G e-m at the Au iron-garnet interface by as much as a factor of three. The electron-magnon conductance does not follow the trend of either the total magnetization of the iron garnet or the magnetic moment of the rare-earth.

36 MATERIALS SCIENCE↗

Ultrafast Light-Induced Magnetoelectric Effect in van der Waals Magnetic Semiconductor Heterostructures

Atomic-scale heterostructures of van der Waals (vdW) magnets and semiconductors provide a unique environment for exploring magnetic dynamics. In contrast to typical photothermal excitation of precessional magnetization dynamics by a pump laser pulse, we find that ultrafast optical excitation of a WS2/CrGeTe3 (CGT) bilayer produces an opposite sign of magnetic torque compared to an isolated CGT film. Experimental observations by time-resolved magneto-optic Kerr effect (TR-MOKE) and theoretical analysis by density functional theory (DFT) and Landau-Lifshitz-Gilbert (LLG) simulations support a mechanism in which charge transfer of photoexcited carriers across the interface alters the perpendicular magnetic anisotropy, which in turn generates a torque on the magnetic layer to trigger precessional magnetization dynamics. These results provide new avenues for ultrafast manipulation of magnetization in vdW heterostructures with type-II band alignments. Lastly, we show that optically-generated spin currents from WS2 into CGT can also trigger precessional dynamics via angular momentum transfer.

Zhou, Wenyi [The Ohio State University]↗

Influence of oxygen on the optical and electrical properties of magnetron-sputtered indium tin oxide thin films at ambient temperature

Indium Tin Oxide (ITO) thin films are commonly used as transparent conductive layers in the production of solar cells. ITO films are typically heat-treated at temperatures exceeding 200 °C after magnetron sputtering to optimize the physical, optical, and electrical characteristics for photovoltaic devices. Here, this high temperature heating procedure greatly limits the use of potential substrates, particularly those comprised of low-temperature-rated polymers. Herein, we examine the physical, optical, and electrical transport effects of oxygen:argon plasmas during radio frequency magnetron sputtering of ITO on glass and flexible polymer surfaces without subsequent heat treatment. ITO thin films were characterized via sheet resistance testing, UV-Vis spectroscopy, X-ray diffraction, and scanning electron microscopy imaging. Sheet resistance measurements revealed an increase in surface resistance with increasing oxygen concentration during sputtering. UV-Vis optical transmittance measurements demonstrated an improvement in optical transmittance with an increase in oxygen concentration reaching a maximum transmittance at an oxygen concentration of 1-2 %. Most importantly, it was discovered that producing bilayers of ITO with pure argon sputtered plasmas followed by oxygen:argon plasmas produced ITO thin films with suitable resistance and transmittance without the need for high temperature post annealing. These results highlight a methodology for the deposition of ITO thin films on temperature sensitive substrates for flexible photovoltaics and low-cost module production.

36 MATERIALS SCIENCE↗

Cationic Ordering and Its Influence on the Magnetic Properties of Co-Rich Cobalt Ferrite Thin Films Prepared by Reactive Solid Phase Epitaxy on Nb-Doped SrTiO 3 (001)

Here, we present the (element-specific) magnetic properties and cation ordering for ultrathin Co-rich cobalt ferrite films. Two Co-rich Co x Fe 3-x O 4 films with different stoichiometry (x=1.1 and x=1.4) have been formed by reactive solid phase epitaxy due to post-deposition annealing from epitaxial CoO/Fe 3 O 4 bilayers deposited before on Nb-doped SrTiO 3 (001). The electronic structure, stoichiometry and homogeneity of the cation distribution of the resulting cobalt ferrite films were verified by angle-resolved hard X-ray photoelectron spectroscopy. From X-ray magnetic circular dichroism measurements, the occupancies of the different sublattices were determined using charge-transfer multiplet calculations. For both ferrite films, a partially inverse spinel structure is found with increased amount of Co 3+ cations in the low-spin state on octahedral sites for the Co 1.4 Fe 1.6 O 4 film. These findings concur with the results obtained by superconducting quantum interference device measurements. Further, the latter measurements revealed the presence of an additional soft magnetic phase probably due to cobalt ferrite islands emerging from the surface, as suggested by atomic force microscope measurements.

36 MATERIALS SCIENCE↗