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Hellman, F.

Publications and source records attributed to Hellman, F..

Structural tunability and origin of two-level systems in amorphous silicon

Amorphous silicon films prepared by electron-beam evaporation have systematically and substantially greater atomic density for higher thickness, higher growth temperature, and slower deposition rate, reaching the density of crystalline Si when films of thickness greater than ~300 nm are grown at 425 °C and at <1 Å/s. Here, a combination of spectroscopic techniques provide insight into atomic disorder, local strains, dangling bonds, and nanovoids. Electron diffraction shows that the short-range order of the amorphous silicon is similar at all growth temperatures, but fluctuation electron microscopy shows that films grown above room temperature show a form of medium-range order not previously observed in amorphous silicon. Atomic disorder and local strain obtained from Raman spectroscopy are reduced with increasing growth temperature and show a nonmonotonic dependence on thickness. Dangling bond density decreases with increasing growth temperature and is only mildly dependent on thickness. Positron annihilation Doppler broadening spectroscopy and electron energy loss spectroscopy show that nanovoids, and not density variations within the network, are responsible for reduced atomic density. Specific heat and mechanical loss measurements, which quantify the density of tunneling two-level systems, in combination with the structural data, suggest that two-level systems in amorphous silicon films are associated with nanovoids and their surroundings, which are in essence loosely bonded regions where atoms are less constrained.

36 MATERIALS SCIENCE↗

Coexistence of soft and hard magnetic phases in single layer amorphous Tb–Co thin films

Amorphous, ferrimagnetic Tb-Co thin films prepared with a thin Ta underlayer and either a Ta or a Pt overlayer show evidence of both soft and hard magnetic phases. At room temperature, the films exhibit conventional ferromagnetism, but low temperature magnetometry measurements reveal the decoupling of the two magnetic phases with decreasing temperature due to increased anisotropy energy of the hard layer at lower temperatures. Decreasing the film thickness to 2 nm, slightly above the superparamagnetic limit found at 1 nm, a soft, low-density phase was isolated and found to be present in all the films as confirmed with x-ray reflectivity and Rutherford backscattering spectrometry measurements. For greater thicknesses, the bottom layer retains its soft magnetic nature, while the remainder of the film is denser and has strong perpendicular magnetic anisotropy, leading to the exchange-spring behavior when the anisotropy becomes large, either at low temperatures or via a Pt overlayer that adds a strong interfacial anisotropy to the layer. Micromagnetic simulations of a soft/hard bilayer model with the experimentally determined anisotropy and magnetization parameters into a soft/hard bilayer model reproduced the experimental hysteretic behavior very well. These findings demonstrate how the magnetic state and the response of a-Tb-Co films to external fields can be controlled, providing a high degree of tunability that is promising for high-performance nanoscale devices.

36 MATERIALS SCIENCE↗

Origin of mechanical and dielectric losses from two-level systems in amorphous silicon

Amorphous silicon contains tunneling two-level systems, which are the dominant energy loss mechanisms for amorphous solids at low temperatures. These two-level systems affect both mechanical and electromagnetic oscillators and are believed to produce thermal and electromagnetic noise and energy loss. However, it is unclear whether the two-level systems that dominate mechanical and dielectric losses are the same; the former relies on the coupling between phonons and two-level systems, with an elastic field coupling constant γ while the latter depends on a two-level systems dipole moment p0, which couples to the electromagnetic field. Mechanical and dielectric loss measurements as well as structural characterization were performed on amorphous silicon thin films grown by electron beam deposition with a range of growth parameters. Samples grown at 425 °C show a large reduction of mechanical loss (34 times) and a far smaller reduction of dielectric loss (2.3 times) compared to those grown at room temperature. Additionally, mechanical loss shows lower loss for thicker films, while dielectric loss shows lower loss for thinner films. Overall, analysis of these results indicate that mechanical loss correlates with atomic density, while dielectric loss correlates with dangling-bond density, suggesting a different origin for these two energy dissipation processes in amorphous silicon.

36 MATERIALS SCIENCE↗

Influence of dislocations and twin walls in BaTiO 3 on the voltage-controlled switching of perpendicular magnetization

In this work, we investigate the influence of dislocations and twin walls in BaTiO 3 on its ferroelectric response and the resulting effect on the perpendicular magnetic anisotropy (PMA) of a strain-coupled [Co\Ni] n film. A dense twinned structure in conjunction with a high dislocation density significantly reduces the converse piezoelectric effect of BaTiO 3 by hindering the propagation of newly nucleated domains with an applied electric field. This, in turn, results in a modest reduction of the PMA of the ferromagnetic layer. On the other hand, the ferroelectric polarization reorients from [100] to [001] direction in a dislocation-free BaTiO 3 , inducing the maximum achievable in-plane compressive strain of 1.1%. A large fraction of this uniaxial strain is transferred to the magnetoelastically coupled ferromagnetic layers whose magnetization switches to in plane via the inverse magnetostriction effect. This work reveals the critical role of the interplay between twin walls and dislocations within a ferroelectric substrate in the performance of multiferroic heterostructures and provides insight into the development of highly energy-efficient magnetoelectric devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Unexpected dependence of the anomalous Hall angle on the Hall conductivity in amorphous transition metal thin films

The anomalous Hall effect (AHE), and magnetic and electronic transport properties were investigated in a series of amorphous transition metal thin films— Fe x S i –x , Fe x Ge 1-x , Co x Ge 1–x , Co x Si 1–x , and Fe 1–y Co y Si. The experimental results are compared with density functional theory calculations of the density of Berry curvature and intrinsic anomalous Hall conductivity. In all samples, the longitudinal conductivity (σ xx ), magnetization (M), and Hall resistivity (ρ xy ) increase with increasing transition metal concentration; due to the structural disorder σ xx is lower in all samples than a typical crystalline metal. In the systems with Fe as the transition metal (including Fe 1–y Co y Si), the magnetization and AHE are large and in some cases greater than the crystalline analog. In all samples, the AHE is dominated by the intrinsic mechanism, arising from a nonzero, locally derived Berry curvature. The anomalous Hall angle (AHA) (= σ xy /σ xx ) is as large as 5% at low temperature. These results are compared with the AHAs reported in a broad range of crystalline and amorphous materials. Previous work has shown that in a typical crystalline ferromagnet the Hall conductivity (σ xy ) and σ xx are correlated and are usually either both large or both small, resulting in an AHA that decreases with increasing σ xy . By contrast, the AHA increases linearly with increasing σ xy in the amorphous systems. This trend is attributed to a generally low σ xx , while σ xy varies and can be large. In the amorphous systems, σ xx and σ xy are not coupled, and there may thus exist the potential to further increase the AHA by increasing σ xy .

36 MATERIALS SCIENCE↗

Two-level systems and growth-induced metastability in hydrogenated amorphous silicon

Specific heat measurements from 2 to 300 K of hydrogenated amorphous silicon prepared by hot-wire chemical vapor deposition show a large excess specific heat at low temperature, significantly larger than the Debye specific heat calculated from the measured sound velocity. The as-prepared films have a Schottky anomaly that is associated with metastable hydrogen in the amorphous network, as well as large linear and excess cubic term commonly associated with tunneling two-level systems in amorphous solids. Annealing at 200 °C, a temperature that enables hydrogen mobility but not evaporation, irreversibly reduces the heat capacity, eliminating the Schottky anomaly and leaving a reduced linear heat capacity. A non-monotonic dependence on growth temperature and H content is observed in all effects, except for sound velocity, which suggests that the tunneling two-level systems and the Schottky anomaly are associated with atomic hydrogen and require low density regions to form, while sound velocity is associated with the silicon network and increases with increasing growth temperature.

36 MATERIALS SCIENCE↗

Itinerant ferromagnetism and intrinsic anomalous Hall effect in amorphous iron-germanium

The amorphous iron-germanium system ( a - Fe x Ge 1 - x ) lacks long-range structural order and hence lacks a significant Brillouin zone. The magnetization of a - Fe x Ge 1 - x is well explained by the Stoner model for Fe concentrations x above the onset of magnetic order around x = 0.4 , indicating that the local order of the amorphous structure preserves the spin-split density of states of the Fe- 3 d states sufficiently to polarize the electronic structure despite k being a bad quantum number. Measurements reveal an enhanced anomalous Hall resistivity ρ x y AH relative to crystalline FeGe; this ρ x y AH is compared to density-functional theory calculations of the anomalous Hall conductivity to resolve its underlying mechanisms. The intrinsic mechanism, typically understood as the Berry curvature integrated over occupied k states but shown here to be equivalent to the density of curvature integrated over occupied energies in aperiodic materials, dominates the anomalous Hall conductivity of a - Fe x Ge 1 - x ( 0.38 ≤ x ≤ 0.61 ). The density of curvature is the sum of spin-orbit correlations of local orbital states and can hence be calculated with no reference to k space. This effect and the accompanying Stoner-like model for the intrinsic anomalous Hall conductivity establish a unified understanding of the underlying physics of the anomalous Hall effect in both crystalline and disordered systems.

36 MATERIALS SCIENCE↗