Stoffel D. Janssens

Separation of intra- and intergranular magnetotransport properties in nanocrystalline diamond films on the metallic side of the metal-insulator transition

A systematic study on the morphology and electronic properties of thin heavily boron-doped nanocrystalline diamond (NCD)films is presented. The films have nominally the same thickness ( 150nm) and are grown with a fixed B/C ratio (5000ppm) but with different C/H ratios (0.5-5%) in the gas phase. The morphology of the films is investigated by x-ray diffraction and atomic force microscopy measurements, which confirm that lower C/H ratios lead to a larger average grain size. Magnetotransport measurements reveal a decrease in resistivity and a large increase in mobility, approaching the values obtained for single-crystal diamond as the average grain size of the films increases. In all films, the temperature dependence of resistivity decreases with larger grains and the charge carrier density and mobility are thermally activated. It is possible

Heat-Transfer Resistance at Solid–Liquid Interfaces: A Tool for the Detection of Single-Nucleotide Polymorphisms in DNA

In this article, we report on the heat-transfer resistance at interfaces as a novel, denaturation-based method to detect single-nucleotide polymorphisms in DNA. We observed that a molecular brush of double-stranded DNA grafted onto synthetic diamond surfaces does not notably affect the heat-transfer resistance at the solid-to-liquid interface. In contrast to this, molecular brushes of single-stranded DNA cause, surprisingly, a substantially higher heat-transfer resistance and behave like a thermally insulating layer. This effect can be utilized to identify ds-DNA melting temperatures via the switching from low- to high heat-transfer resistance. The melting temperatures identified with this method for different DNA duplexes (29 base pairs without and with built-in mutations) correlate nicely with data calculated by modeling. The method is fast, label-free (without the need for fluorescent or radioactive markers), allows for repetitive measurements, and can also be extended toward array formats. Reference measurements by confocal fluorescence microscopy and impedance spectroscopy confirm that the switching of heat-transfer resistance upon denaturation is indeed related to the thermal on-chip denaturation of DNA.

Direct visualization of boron dopant distribution and coordination in individual chemical vapor deposition nanocrystalline B-doped diamond grains

The boron dopant distribution in individual heavily boron-doped nanocrystalline diamond film grains, with sizes ranging from 100 to 350 nm in diameter, has been studied using a combination of high resolution annular dark field scanning transmission electron microscopy and spatially resolved electron energy-loss spectroscopy. Using these tools, the boron distribution and local boron coordination have been determined. Quantification results reveal embedding of B dopants in the diamond lattice, and a preferential enrichment of boron at defective areas and twin boundaries. Coordination mapping reveals a distinct difference in coordination of the B dopants in “pristine” diamond areas and in defective regions.

Local boron environment in B-doped nanocrystalline diamond films.

Thin films of heavily B-doped nanocrystalline diamond (B:NCD) have been investigated by a combination of high resolution annular dark field scanning transmission electron microscopy and spatially resolved electron energy-loss spectroscopy performed on a state-of-the-art aberration corrected instrument to determine the B concentration, distribution and the local B environment. Concentrations of ~1 to 3 at.% of boron are found to be embedded within individual grains. Even though most NCD grains are surrounded by a thin amorphous shell, elemental mapping of the B and C signal shows no preferential embedding of B in these amorphous shells or in grain boundaries between the NCD grains, in contrast with earlier work on more macroscopic superconducting polycrystalline B-doped diamond films. Detailed inspection of the fine structure of the boron K-edge and comparison with density functional theory calculated fine structure energy-loss near-edge structure signatures confirms that the B atoms present in the diamond grains are substitutional atoms embedded tetrahedrally into the diamond lattice.

Photocurrent Generation in Diamond Electrodes Modified with Reaction Centers

Photoactive reaction centers (RCs) are protein complexes in bacteria able to convert sunlight into other forms of energy with a high quantum yield. The photostimulation of immobilized RCs on inorganic electrodes result in the generation of photocurrent that is of interest for biosolar cell applications. This paper reports on the use of novel electrodes based on functional conductive nanocrystalline diamond onto which bacterial RCs are immobilized. A three-dimensional conductive polymer scaffold grafted to the diamond electrodes enables efficient entrapment of photoreactive proteins. The electron transfer in these functional diamond electrodes is optimized through the use of a ferrocene-based electron mediator, which provides significant advantages such as a rapid electron transfer as well as high generated photocurrent. A detailed discussion of the generated photocurrent as a function of time, bias voltage, and mediators in solution unveils the mechanisms limiting the electron transfer in these functional electrodes. This work featuring diamond-based electrodes in biophotovoltaics offers general guidelines that can serve to improve the performance of similar devices based on different materials and geometries.

Surface plasma pretreatment for enhanced diamond nucleation on AlN

The surface of polycrystalline aluminum nitride (AlN) thin films is exposed to different gas discharge plasmas (N2, O2, and CF4) followed by a water-based colloidal seeding of ultra-dispersed nanodiamond particles. Fluorination of the AlN surface enhances the seeding density, whereas the oxidized surface does not yield any nucleation sites. In the former case, the seeding density improves by almost three orders of magnitude as compared to the untreated and N2 pretreated samples, and allows to grow pinhole-free nanocrystalline diamond film on AlN. Finally, we demonstrate a route towards selective diamond growth on AlN thin films by employing CF4 plasma pretreatment together with photolithography.

Local bond length variations in boron-doped nanocrystalline diamond measured by spatially resolved electron energy-loss spectroscopy

Variations in local bond length and coordination in boron-doped nanocrystalline diamond (NCD) films have been studied through changes in the fine structure of boron and carbon K-edges in electron energy-loss spectra, acquired in a scanning transmission electron microscope. The presence of high concentrations of B in pristine diamond regions and enrichment of B at defects in single NCD grains is demonstrated. Local bond length variations are evidenced through an energy shift of the carbon 1s → σ* edge at B-rich defective regions within single diamond grains, indicating an expansion of the diamond bond length at sites with local high B content.

Ultra-thin nanocrystalline diamond membranes as pressure sensors for harsh environments

Glass and diamond are suitable materials for harsh environments. Here, a procedure for fabricating ultra-thin nanocrystalline diamond membranes on glass, acting as an electrically insulating substrate, is presented. In order to investigate the pressure sensing properties of such membranes, a circular, highly conductive boron-doped nanocrystalline diamond membrane with a resistivity of 38 mΩ cm, a thickness of 150 nm, and a diameter of 555 μm is fabricated in the middle of a Hall bar structure. During the application of a positive differential pressure under the membrane (0–0.7 bar), four point piezoresistive effect measurements are performed. From these measurements, it can be concluded that the resistance response of the membrane, as a function of differential pressure, is highly linear and sensitive.

Thin conductive diamond films as beam intensity monitors for soft x-ray beamlines

Quantitative analysis of X-ray absorption and dichroism data requires knowledge of the beamline photon flux during the measurements. We show that thin conductive (B-doped) diamond thin films can be an alternative to the widely used gold meshes for monitoring the beam intensity of soft X-ray beamlines in situ. Limited by the carbon extended x-ray absorption fine structure oscillations, the diamond films become applicable beginning from about 600 eV photon energy, where the important transition metal edges and the rare-earth edges are found. The 100 nm and 250 nm thick free-standing diamond films were grown and tested against standard gold meshes in real-life dichroism experiments performed at beamline ID08 of the European Synchrotron Radiation Facility, Grenoble, France. Quantitative agreement was found between the two experimental data sets. The films feature an extremely high transmission of about 90% and, at the same time, yield a sufficiently strong and clean reference signal. Furthermore, the thin films do not affect the shape of the transmitted beam. X-rays passing mesh-type monitors are subject to diffraction effects, which widen the beam and become particularly disturbing for small beamsizes in the micrometer range.

Hydrogen termination of CVD diamond films by high-temperature annealing at atmospheric pressure

A high-temperature procedure to hydrogenate diamond films using molecular hydrogen at atmospheric pressure was explored. Undoped and doped chemical vapour deposited (CVD) polycrystalline diamond films were treated according to our annealing method using a H2 gas flow down to ~50 ml∕min (STP) at ~850 °C. The films were extensively evaluated by surface wettability, electron affinity, elemental composition, photoconductivity, and redox studies. In addition, electrografting experiments were performed. The surface characteristics as well as the optoelectronic and redox properties of the annealed films were found to be very similar to hydrogen plasma-treated films. Moreover, the presented method is compatible with atmospheric pressure and provides a low-cost solution to hydrogenate CVD diamond, which makes it interesting for industrial applications. The plausible mechanism for the hydrogen termination of CVD diamond films is based on the formation of surface carbon dangling bonds and carbon-carbon unsaturated bonds at the applied tempera-ture, which react with molecular hydrogen to produce a hydrogen-terminated surface.