Nanocomposite thin films comprised of metastable metal carbides in a carbon matrix have a wide variety of applications ranging from hard coatings to magnetics and energy storage and conversion. While their deposition using nonequilibrium techniques is established, the understanding of the dynamic evolution of such metastable nanocomposites under thermal equilibrium conditions at elevated temperatures during processing and during device operation remains limited. Here, we investigate sputter-deposited nanocomposites of metastable nickel carbide (Ni3C) nanocrystals in an amorphous carbon (a-C) matrix during thermal postdeposition processing via complementary in situ X-ray diffractometry, in situ Raman spectroscopy, and in situ X-ray photoelectron spectroscopy. At low annealing temperatures (300 °C) we observe isothermal Ni3C decomposition into face-centered-cubic Ni and amorphous carbon, however, without changes to the initial finely structured nanocomposite morphology. Only for higher temperatures (400–800 °C) Ni-catalyzed isothermal graphitization of the amorphous carbon matrix sets in, which we link to bulk-diffusion-mediated phase separation of the nanocomposite into coarser Ni and graphite grains. Upon natural cooling, only minimal precipitation of additional carbon from the Ni is observed, showing that even for highly carbon saturated systems precipitation upon cooling can be kinetically quenched. Our findings demonstrate that phase transformations of the filler and morphology modifications of the nanocomposite can be decoupled, which is advantageous from a manufacturing perspective. Our in situ study also identifies the high carbon content of the Ni filler crystallites at all stages of processing as the key hallmark feature of such metal–carbon nanocomposites that governs their entire thermal evolution. In a wider context, we also discuss our findings with regard to the much debated potential role of metastable Ni3C as a catalyst phase in graphene and carbon nanotube growth.
We report on the optimisation of amorphous molybdenum silicide thin film growth for superconducting nanowire single-photon detector (SNSPD) applications. Molybdenum silicide was deposited via co-sputtering from Mo and Si targets in an Ar atmosphere. The superconducting transition temperature (Tc) and sheet resistance (Rs) were measured as a function of thickness and compared to several theoretical models for disordered superconducting films. Superconducting and optical properties of amorphous materials are very sensitive to short- (up to 1 nm) and medium-range order (∼1–3 nm) in the atomic structure. Fluctuation electron microscopy studies showed that the films assumed an A15-like medium-range order. Electron energy loss spectroscopy indicates that the film stoichiometry was close to Mo83Si17, which is consistent with reports that many other A15 structures with the nominal formula A3B show a significant non-stoichiometry with A:B > 3:1. Optical properties from ultraviolet (270 nm) to infrared (2200 nm) wavelengths were measured via spectroscopic ellipsometry for 5 nm thick MoSi films indicating high long wavelength absorption. We also measured the current density as a function of temperature for nanowires patterned from a 10 nm thick MoSi film. The current density at 3.6 K is 3.6 × 105 A cm−2 for the widest wire studied (2003 nm), falling to 2 × 105 A cm−2 for the narrowest (173 nm). This investigation confirms the excellent suitability of MoSi for SNSPD applications and gives fresh insight into the properties of the underlying materials.
Amorphous superconductors have become attractive candidate materials for superconducting nanowire single-photon detectors due to their ease of growth, homogeneity and competitive superconducting properties. To date the majority of devices have been fabricated using WxSi1−x, though other amorphous superconductors such as molybdenum silicide (MoxSi1−x) offer increased transition temperature. This study focuses on the properties of MoSi thin films grown by magnetron sputtering. We examine how the composition and growth conditions affect film properties. For 100 nm film thickness, we report that the superconducting transition temperature (Tc) reaches a maximum of 7.6 K at a composition of Mo83Si17. The transition temperature and amorphous character can be improved by cooling of the substrate during growth which inhibits formation of a crystalline phase. X-ray diffraction and transmission electron microscopy studies confirm the absence of long range order. We observe that for a range of 6 common substrates (silicon, thermally oxidized silicon, R- and C-plane sapphire, x-plane lithium niobate and quartz), there is no variation in superconducting transition temperature, making MoSi an excellent candidate material for SNSPDs.
We present low temperature nano-optical characterization of a silicon-on-insulator (SOI) waveguide integrated SNSPD. The SNSPD is fabricated from an amorphous Mo 83 Si 17 thin film chosen to give excellent substrate conformity. At 350 mK, the SNSPD exhibits a uniform photoresponse under perpendicular illumination, corresponding to a maximum system detection efficiency of approximately 5% at 1550 nm wavelength. Under these conditions 10 Hz dark count rate and 51 ps full width at half maximum (FWHM) timing jitter is observed. #260601
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