Intermediate order in tetrahedrally coordinated silicon: evidence for chainlike objects

In this report, we describe the nature of intermediate order in silicon as determined by recent measurements on thin films using transmission electron microscopy (TEM) and Raman scattering. The TEM images show in addition to the expected continuous random network (CRN), the presence of highly ordered quasi-one-dimensional “chain-like objects” (CLO's) that are 1–2 nm wide and tens of nm long that meander and show some evidence of cross-linking with each other. The presence of these objects correlate to a Raman feature centered at 490 cm⁻¹ whose width is 35–40 cm⁻¹, and is used to quantify the heterogeneity in terms of the CLO and CRN (=475 cm⁻¹ scattering) concentrations. The 490 and 35 cm⁻¹ values are consistent with bond angle deviations approaching 0°, and thus reinforces an association with the CLOs. We find that in reference quality a-Si:H (made using pure SiH₄), the CLO concentration is about 5 vol%, while in state-of-the-art material using high H₂ levels of dilution during processing, it increases to about 15%. Increased stability of such material to light-soaking is thus not mediated by a direct volumetric replacement of poor with high-quality components. Rather, an important characteristic of intermediate order in silicon is the low-dimensional aspect of its order, which allows it to influence more total volume than which it is itself composed. Consistent with these and other recent findings, we propose a tensegrity model of amorphous silicon.