Note: When clicking on a Digital Object Identifier (DOI) number, you will be taken to an external site maintained by the publisher.
Some full text articles may not yet be available without a charge during the embargo (administrative interval).
What is a DOI Number?
Some links on this page may take you to non-federal websites. Their policies may differ from this site.
-
Abstract X-ray diffraction, Amorphous silicon, Multi-objective optimization, Monte Carlo methods. This paper addresses a difficult inverse problem that involves the reconstruction of a three-dimensional model of tetrahedral amorphous semiconductors via inversion of diffraction data. By posing the material-structure determination as a multiobjective optimization program, it has been shown that the problem can be solved accurately using a few structural constraints, but no total-energy functionals/forces, which describe the local chemistry of amorphous networks. The approach yields highly realistic models of amorphous silicon, with no or only a few coordination defects (≤1%), a narrow bond-angle distribution of width 9–11.5°, and an electronic gap of 0.8–1.4 eV. These data-driven information-based models have been found to produce electronic and vibrational properties of a -Si that match accurately with experimental data and rival that of the Wooten-Winer-Weaire models. The study confirms the effectiveness of a multiobjective optimization approach to the structural determination of complex materials, and resolves a long-standing dispute concerning the uniqueness of a model of tetrahedral amorphous semiconductors obtained via inversion of diffraction data.more » « less
-
more » « less
This article presents an ab initio study of hydrogen dynamics inside nanometer‐size voids in amorphous silicon (
a ‐Si) within the framework of the density‐functional theory for a varying hydrogen load of 10–30 atoms per void at the low and high temperature of 400 and 700 K, respectively. Using the local density approximation (LDA) and its generalized‐gradient counterpart (GGA), the dynamics of hydrogen atoms inside the voids are examined with an emphasis on the diffusion of H atoms/molecules, and the resulting nanostructural changes of the void surfaces. The results from simulations suggest that the microstructure of the hydrogen distribution on the void surfaces and the morphology of the voids are characterized by the presence of a significant number of monohydride SiH bonds, along with a few dihydride configurations. The study also reveals that a considerable number (about 10–45 at%) of total H atoms inside a void can appear as H2molecules for a hydrogen load of 10–30 H atoms per void. The approximate shape of the voids is addressed from a knowledge of the positions of the void‐surface atoms using the convex‐hull approximation and the Gaussian broadening of the pseudoatomic surfaces of Si and H atoms. -
more » « less
The structure of the first sharp diffraction peak (FSDP) of amorphous silicon (a‐Si) near 2 Å−1is addressed with particular emphasis on the position, intensity, and width of the diffraction curve. By studying a number of continuous random network (CRN) models of a‐Si, it is shown that the position and intensity of the FSDP are primarily determined by radial atomic correlations in the amorphous network on the length scale of 15 Å. A shell‐by‐shell analysis of the contribution from different radial shells reveals that key contributions to the FSDP originate from the second and fourth radial shells in the network, which are accompanied by a background contribution from the first shell and small residual corrections from the distant radial shells. The results from numerical calculations are complemented by a phenomenological discussion of the relationship between the peaks in the structure factor in the wavevector space and the reduced pair‐correlation function in the real space. An approximate functional relation between the position of the FSDP and the average radial distance of Si atoms in the second radial shell in the network is derived, which is corroborated by numerical calculations.
