The influence of hydrogen on the chemical, mechanical, optical/electronic, and electrical transport properties of amorphous hydrogenated boron carbide

Because of its high electrical resistivity, low dielectric constant (kappa), high thermal neutron capture cross section, and robust chemical, thermal, and mechanical properties, amorphous hydrogenated boron carbide (a-BxC:H-y) has garnered interest as a material for low-kappa dielectric and solid-state neutron detection applications. Herein, we investigate the relationships between chemical structure (atomic concentration B, C, H, and O), physical/mechanical properties (density, porosity, hardness, and Young's modulus), electronic structure [band gap, Urbach energy (E-U), and Tauc parameter (B-1/2)], optical/dielectric properties (frequency-dependent dielectric constant), and electrical transport properties (resistivity and leakage current) through the analysis of a large series of a-BxC: Hy thin films grown by plasma-enhanced chemical vapor deposition from ortho-carborane. The resulting films exhibit a wide range of properties including H concentration from 10% to 45%, density from 0.9 to 2.3 g/cm(3), Young's modulus from 10 to 340 GPa, band gap from 1.7 to 3.8 eV, Urbach energy from 0.1 to 0.7 eV, dielectric constant from 3.1 to 7.6, and electrical resistivity from 10(10) to 10(15) Omega cm. Hydrogen concentration is found to correlate directly with thin-film density, and both are used to map and explain the other material properties. Hardness and Young's modulus exhibit a direct power law relationship with density above similar to 1.3 g/cm(3) (or below similar to 35% H), below which they plateau, providing evidence for a rigidity percolation threshold. An increase in band gap and decrease in dielectric constant with increasing H concentration are explained by a decrease in network connectivity as well as mass/electron density. An increase in disorder, as measured by the parameters EU and B-1/2, with increasing H concentration is explained by the release of strain in the network and associated decrease in structural disorder. All of these correlations in a-BxC: Hy are found to be very similar to those observed in amorphous hydrogenated silicon (a-Si: H), which suggests parallels between the influence of hydrogenation on their material properties and possible avenues for optimization. Finally, an increase in electrical resistivity with increasing H at <35 at. % H concentration is explained, not by disorder as in a-Si: H, but rather by a lower rate of hopping associated with a lower density of sites, assuming a variable range hopping mechanism interpreted in the framework of percolation theory. (C) 2015 AIP Publishing LLC.