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  1. To enable greater control over thermal atomic layer deposition (ALD) of molybdenum disulfide (MoS 2 ), here we report studies of the reactions of molybdenum hexafluoride (MoF 6 ) and hydrogen sulfide (H 2 S) with metal oxide substrates from nucleation to few-layer films. In situ quartz crystal microbalance experiments performed at 150, 200, and 250 °C revealed temperature-dependent nucleation behavior of the MoF 6 precursor, which is attributed to variations in surface hydroxyl concentration with temperature. In situ Fourier transform infrared spectroscopy coupled with ex situ x-ray photoelectron spectroscopy (XPS) indicated the presence of molybdenum oxide and molybdenum oxyfluoride species during nucleation. Density functional theory calculations additionally support the formation of these species as well as predicted metal oxide to fluoride conversion. Residual gas analysis revealed reaction by-products, and the combined experimental and computational results provided insights into proposed nucleation surface reactions. With additional ALD cycles, Fourier transform infrared spectroscopy indicated steady film growth after ∼13 cycles at 200 °C. XPS revealed that higher deposition temperatures resulted in a higher fraction of MoS 2 within the films. Deposition temperature was found to play an important role in film morphology with amorphous films obtained at 200 °C and below, while layered films withmore »vertical platelets were observed at 250 °C. These results provide an improved understanding of MoS 2 nucleation, which can guide surface preparation for the deposition of few-layer films and advance MoS 2 toward integration into device manufacturing.« less
    Free, publicly-accessible full text available December 1, 2023
  2. Free, publicly-accessible full text available September 1, 2023
  3. Nanoarchitectural control of matter is crucial for next-generation technologies. DNA origami templates are harnessed to accurately position single molecules; however, direct single molecule evidence is lacking regarding how well DNA origami can control the orientation of such molecules in three-dimensional space, as well as the factors affecting control. Here, we present two strategies for controlling the polar (θ) and in-plane azimuthal (ϕ) angular orientations of cyanine Cy5 single molecules tethered on rationally-designed DNA origami templates that are physically adsorbed (physisorbed) on glass substrates. By using dipolar imaging to evaluate Cy5′s orientation and super-resolution microscopy, the absolute spatial orientation of Cy5 is calculated relative to the DNA template. The sequence-dependent partial intercalation of Cy5 is discovered and supported theoretically using density functional theory and molecular dynamics simulations, and it is harnessed as our first strategy to achieve θ control for a full revolution with dispersion as small as ±4.5°. In our second strategy, ϕ control is achieved by mechanically stretching the Cy5 from its two tethers, being the dispersion ±10.3° for full stretching. These results can in principle be applied to any single molecule, expanding in this way the capabilities of DNA as a functional templating material for single-molecule orientation control.more »The experimental and modeling insights provided herein will help engineer similar self-assembling molecular systems based on polymers, such as RNA and proteins.« less
    Free, publicly-accessible full text available July 1, 2023
  4. Mid-infrared photonic integrated circuits (PICs) that combine on-chip light sources with other optical components constitute a key enabler for applications such as chemical sensing, light detection, ranging, and free-space communications. In this paper, we report the monolithic integration of interband cascade lasers emitting at 3.24 µm with passive, high-index-contrast waveguides made of chalcogenide glasses. Output from the chalcogenide waveguides exhibits pulsed peak power up to 150 mW (without roll-over), threshold current density 280 A/cm2, and slope efficiency 100 mW/A at 300 K, with a lower bound of 38% efficiency for coupling between the two waveguides. These results represent an important step toward the realization of fully integrated mid-infrared PICs.

  5. 3D photonics promises to expand the reach of photonics by enabling the extension of traditional applications to nonplanar geometries and adding novel functionalities that cannot be attained with planar devices. Available material options and device geometries are, however, limited by current fabrication methods. In this work, we pioneer a method that allows for placement of integrated photonic device arrays at arbitrary predefined locations in 3D using a fabrication process that capitalizes on the buckling of a 2D pattern. We present theoretical and experimental validation of the deterministic buckling process, thus demonstrating implementation of the technique to realize what we believe to be the first fully packaged 3D integrated photonics platform. Application of the platform for mechanical strain sensing is further demonstrated.

  6. The extraordinary optical properties of single-layer graphene have spurred the development of a variety of photonic components. We have previously demonstrated a scalable and versatile platform to facilitate the integration of graphene and other 2-D materials with chalcogenide glass-based planar photonics. In this paper, we detail the design criteria and optimization guidelines towards high-performance graphene-integrated thermo-optic (TO) switches based on the chalcogenide glass-on-graphene platform. Notably, absorption loss of graphene can be reduced to < 20 dB/cm when it is sandwiched inside photonic structures capitalizing on the anisotropic absorption property of graphene. We quantify energy efficiency of the TO switch, showing that the choice of cladding materials plays a critical role in improving device efficiency. Furthermore, we report a record TO switching efficiency of 10 nm/mW via judicious engineering of the overlap between optical mode and thermal profile.

  7. Abstract

    The DNA hypomethylating agents decitabine and 5-azacytidine are the only two drugs approved for treatment of all subtypes of the myeloid malignancy myelodysplastic syndromes (MDS). The key to drug activity is incorporation into target cell DNA, however, a practical method to measure this incorporation is un-available. Here, we report a sensitive and specific LC-MS/MS method to simultaneously measure decitabine incorporation and DNA hypomethylation. A stable heavy isotope of 2′-deoxycytidine was used as an internal standard and one-step multi-enzyme digestion was used to release the DNA bound drug. Enzyme-released decitabine along with other mononucleosides were separated by a reverse-phase C18column and quantified by mass spectrometry using multiple-reaction-monitoring (MRM) mode, with a lower limit of quantitation at 1.00 nM.In vitrostudies demonstrated dosage and time-dependent incorporation of decitabine into myeloid leukemia cell DNA that correlated with extent of DNA hypomethylation. When applied to clinical samples serially collected from MDS patients treated with decitabine, the method again demonstrated correlation between decitabine DNA-incorporation and DNA hypomethylation. This novel assay to measure the intended molecular pharmacodynamic effect of decitabine therapy can therefore potentially provide insights into mechanisms underlying sensitivity versus resistance to therapy.