Advanced Synthesis and Characterization Techniques for Ultrahard Film Growth

Anthony Van Buuren (14-ERD-067)

Project Description

Ultrahard materials are relevant to Livermore's National Ignition Facility for ignition targets, the Department of Defense for wear-resistant coatings, and the Defense Advance Research Projects Agency for low-temperature diamond growth. Chemical vapor deposition has attracted significant interest for the preparation of ultrahard coatings, yet characterization has largely been conducted post-synthesis, which restricts understanding of growth mechanisms because the surface environment changes during deposition. Developing a means to deposit ultrahard coatings with high spatial resolution and at low temperature on three-dimensional structures would represent a completely new capability that can be readily integrated into the additive manufacturing effort at Lawrence Livermore. Our research combines unique Laboratory-based, laser-assisted chemical vapor-deposition synthesis with x-ray-based in situ characterization to tackle this problem (see figure). Our synthesis method could provide a versatile approach for ultrahard film synthesis with precise control over the location of deposition, and the in situ method enables a comprehensive characterization of the film structure at all stages of growth.

We expect to establish an x-ray-based in situ diagnostic for coating process control and rapid prototyping of ultrahard coatings. By rapidly exploring chemical and structural properties of candidate ultrahard materials with our laser-assisted diagnostic cell for chemical vapor deposition, we expect to achieve a better understanding of these materials over short time periods. We will develop a predictive understanding of coating growth and resulting film structure and robustness, and produce spatially selective coatings of ultrahard materials. We are confident that the research will attract the interest of the oil and gas service sector in the ability to produce designer coatings of materials such as diamond, boron carbide, and boron carbon nitride for diverse applications such as high-wear parts in pumps, drill bits and other mechanical surfaces, materials that experience extreme chemical or thermal environments, and mission-critical parts.

Mission Relevance

Our new laser-assisted chemical vapor-deposition capability and in situ diagnostics expertise supports the Laboratory's additive manufacturing efforts to produce unique materials. Research into ultrahard, fracture- and corrosion-resistant materials falls squarely in LLNL's advanced materials and manufacturing core competency, especially with regard to development of new materials and partnership building.

FY16 Accomplishments and Results

In FY16 we (1) successfully established laser-assisted chemical vapor-deposition growth of silicon carbide at Livermore, and boron carbide at the University of California, Berkeley Nanolab; (2) discovered that by modifying laser power and precursor gas (tetramethyl silane), growth of silicon carbide films or wires could be obtained; (3) grew boron carbide films using boron trichloride precursors; (4) deployed the portable vapor-deposition system in conjunction with in situ experiments to study the initial growth of silicon carbide films; and (5) initiated in situ experiments during laser-assisted chemical vapor-deposition growth with x-ray absorption spectroscopy at the Canadian Light Source in Saskatoon, and x-ray diffraction at the Advanced Photon Source at Argonne National Laboratory.

We used in situ x-ray diffraction to monitor laser-assisted chemical vapor-deposition growth of boron carbide for our study of ultrahard material films for diverse applications in energy and national security.
We used in situ x-ray diffraction to monitor laser-assisted chemical vapor-deposition growth of boron carbide for our study of ultrahard material films for diverse applications in energy and national security.
 

Publications and Presentations

  • Van Buuren, A., "Structure of carbon nanotube porins in lipid bilayers: An in situ small-angle x-ray scattering (SAXS) study." Nano Lett. 16, 4019 (2016). LLNL-JRNL-679134. http://dx.doi.org/10.1021/acs.nanolett.6