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  1. We present a comprehensive study of the inhomogeneous mixed-valence compound, EuPd3S4, by electrical transport, X-ray diffraction, time-domain151Eu synchrotron Mössbauer spectroscopy, and X-ray absorption spectroscopy measurements under high pressure. Electrical transport measurements show that the antiferromagnetic ordering temperature,TN, increases rapidly from 2.8 K at ambient pressure to 23.5 K at ~19 GPa and plateaus between ~19 and ~29 GPa after which no anomaly associated withTNis detected. A pressure-induced first-order structural transition from cubic to tetragonal is observed, with a rather broad coexistence region (~20 GPa to ~30 GPa) that corresponds to theTNplateau. Mössbauer spectroscopy measurements show a clear valence transition from approximately 50:50 Eu2+:Eu3+to fully Eu3+at ~28 GPa, consistent with the vanishing of the magnetic order at the same pressure. X-ray absorption data show a transition to a fully trivalent state at a similar pressure. Our results show that pressure first greatly enhancesTN, most likely via enhanced hybridization between the Eu 4fstates and the conduction band, and then, second, causes a structural phase transition that coincides with the conversion of the europium to a fully trivalent state.

     
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    Free, publicly-accessible full text available December 19, 2024
  2. Microwave loss in superconducting TiN films is attributed to two-level systems in various interfaces arising in part from oxidation and microfabrication-induced damage. Atomic layer etching (ALE) is an emerging subtractive fabrication method which is capable of etching with angstrom-scale etch depth control and potentially less damage. However, while ALE processes for TiN have been reported, they either employ HF vapor, incurring practical complications, or the etch rate lacks the desired control. Furthermore, the superconducting characteristics of the etched films have not been characterized. Here, we report an isotropic plasma-thermal TiN ALE process consisting of sequential exposures to molecular oxygen and an SF6/H2 plasma. For certain ratios of SF6:H2 flow rates, we observe selective etching of TiO2 over TiN, enabling self-limiting etching within a cycle. Etch rates were measured to vary from 1.1 Å/cycle at 150°C to 3.2 Å/cycle at 350°C using ex situ ellipsometry. We demonstrate that the superconducting critical temperature of the etched film does not decrease beyond that expected from the decrease in film thickness, highlighting the low-damage nature of the process. These findings have relevance for applications of TiN in microwave kinetic inductance detectors and superconducting qubits. 
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    Free, publicly-accessible full text available September 26, 2024
  3. Free, publicly-accessible full text available October 20, 2024
  4. We report the isotropic plasma atomic layer etching (ALE) of aluminum nitride using sequential exposures of SF6 plasma and trimethylaluminum [Al(CH3)3]. ALE was observed at temperatures greater than 200 °C, with a maximum etch rate of 1.9 Å/cycle observed at 300 °C as measured using ex situ ellipsometry. After ALE, the etched surface was found to contain a lower concentration of oxygen compared to the original surface and exhibited a ∼35% decrease in surface roughness. These findings have relevance for applications of AlN in nonlinear photonics and wide bandgap semiconductor devices. 
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    Free, publicly-accessible full text available May 2, 2024
  5. The previously unreported layered compounds IrTe 2 I and RhTe 2 I were prepared by a high-pressure synthesis method. Single crystal X-ray and powder X-ray diffraction studies find that the compounds are isostructural, crystallizing in a layered orthorhombic structure in the non-centrosymmetric, non-symmorphic space group Pca 2 1 (#29). Characterization reveals diamagnetic, high resistivity, semiconducting behavior for both compounds, consistent with the +3 chemical valence and d 6 electronic configurations for both iridium and rhodium and the Te–Te dimers seen in the structural study. Electronic band structures are calculated for both compounds, showing good agreement with the experimental results. 
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  6. null (Ed.)
    The optical conductivity of single layer graphene (SLG) can be significantly and reversibly modified when the Fermi level is tuned by electrical gating. However, so far this interesting property has rarely been applied to free-space two-dimensional (2D) photonic devices because the surface-incident absolute absorption of SLG is limited to 1%–2%. No significant change in either reflectance or transmittance would be observed even if SLG is made transparent upon gating. To achieve significantly enhanced surface-incident optical absorption in SLG in a device structure that also allows gating, here we embed SLG in an optical slot-antenna-coupled cavity (SAC) framework, simultaneously enhancing SLG absorption by up to 20 times and potentially enabling electrical gating of SLG as a step towards tunable 2D photonic surfaces. This framework synergistically integrates near-field enhancement induced by ultrahigh refractive index semimetal slot-antenna with broadband resonances in visible and infrared regimes, ~ 3 times more effective than a vertical cavity structure alone. An example of this framework consists of self-assembled, close-packed Sn nanodots separated by ~ 10 nm nanogaps on a SLG/SiO2/Al stack, which dramatically increases SLG optical absorption to 10%-25% at λ = 600–1,900 nm. The enhanced SLG absorption spectrum can also be controlled by the insulator thickness. For example, SLG embedded in this framework with a 150 nm-thick SiO2 insulating layer displays a distinctive red color in contrast to its surrounding regions without SLG on the same sample under white light illumination. This opens a potential path towards gate-tunable spectral reflectors. Overall, this work initiates a new approach towards tunable 2D photonic surfaces. 
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  7. Cryogenic electron microscopy (cryo-EM) has become one of the most powerful techniques to reveal the atomic structures and working mechanisms of biological macromolecules. New designs of the cryo-EM grids—aimed at preserving thin, uniform vitrified ice and improving protein adsorption—have been considered a promising approach to achieving higher resolution with the minimal amount of materials and data. Here, we describe a method for preparing graphene cryo-EM grids with up to 99% monolayer graphene coverage that allows for more than 70% grid squares for effective data acquisition with improved image quality and protein density. Using our graphene grids, we have achieved 2.6-Å resolution for streptavidin, with a molecular weight of 52 kDa, from 11,000 particles. Our graphene grids increase the density of examined soluble, membrane, and lipoproteins by at least 5-fold, affording the opportunity for structural investigation of challenging proteins which cannot be produced in large quantity. In addition, our method employs only simple tools that most structural biology laboratories can access. Moreover, this approach supports customized grid designs targeting specific proteins, owing to its broad compatibility with a variety of nanomaterials.

     
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