Electronic states and total energies in hydrogenated amorphous silicon

Abstract

The effects of bulklike and surfacelike surroundings on the electronic density of states of a variety of Si-H bonding conformations in hydrogenated amorphous silicon are examined using the cluster Bethe-lattice approach. Firstly, we discover that two fundamentally different bonding patterns, with different consequences for the doping mechanism, are consistent with ultraviolet photoemission spectroscopy (UPS) data. These are (1) H atoms bonded in microcrystalline regions and (2) clusters of monohydrides (SiH) in a continuous random network. Our results suggest an experiment in which x-ray photoemission spectroscopy and UPS taken together should distinguish between (1) and (2) and hence contribute toward understanding doping. Secondly, by using the calculated densities of states, the energies of a number of conformations and dehydrogenation reactions are calculated with the use of an empirical bond-strength total-energy scheme. Our results agree with results from annealing experiments. We introduce an improvement in the Bethe-lattice method which permits efficient solution of a second-neighbor tight-binding Hamiltonian, and which is valid for $N\mathrm{th}$-neighbor interactions. We also estimate the Hubbard $U$, Stokes shifts, and electronic states associated with neutral and charged dangling bonds.