Modelling the defect processes of materials for energy applications

The technological requirement for ever more efficient materials for the energy and electronics sectors has led to the consideration of numerous compositionally and structurally complicated systems. These systems include solid solutions that are difficult to model using electronic structure calculations because of the numerous possibilities in the arrangement of atoms in supercells. The plethora of such possible arrangements leads to extensive and large numbers of potential supercells, and this renders the investigation of defect properties practically intractable. We consider recent advances in oxide interfaces where studies have demonstrated that it is feasible to tune their defect processes effectively. In this review, we aim to contribute to the ongoing discussion in the community on simple, efficient and tractable ways to realise research in solid solutions and oxide interfaces. The review considers the foundations of relevant thermodynamic models to extract point defect parameters and the special quasirandom structures method to model the supercell of solid solutions. Examples of previous work are given to highlight these methodologies. The review concludes with future directions, systems to be considered and a brief assessment of the relevant methodologies

Effect of tin doping on oxygen- and carbon-related defects in Czochralski silicon

Experimental and theoretical techniques are used to investigate the impact of tin doping on the formation and the thermal stability of oxygen- and carbon-related defects in electron-irradiated Czochralski silicon. The results verify previous reports that Sn doping reduces the formation of the VO defect and suppresses its conversion to the VO2 defect. Within experimental accuracy, a small delay in the growth of the VO2 defect is observed. Regarding carbon-related defects, it is determined that Sn doping leads to a reduction in the formation of the CiOi, CiCs, and CiOi(SiI) defects although an increase in their thermal stability is observed. The impact of strain induced in the lattice by the larger tin substitutional atoms, as well as their association with intrinsic defects and carbon impurities, can be considered as an explanation to account for the above observations. The density functional theory calculations are used to study the interaction of tin with lattice vacancies and oxygen- and carbon-related clusters. Both experimental and theoretical results demonstrate that tin co-doping is an efficient defect engineering strategy to suppress detrimental effects because of the presence of oxygen- and carbon-related defect clusters in devices

Atomistic Simulations of the Defect Chemistry and Self-Diffusion of Li-ion in LiAlO2

Lithium aluminate, LiAlO2, is a material that is presently being considered as a tritium breeder material in fusion reactors and coating material in Li-conducting electrodes. Here, we employ atomistic simulation techniques to show that the lowest energy intrinsic defect process is the cation anti-site defect (1.10 eV per defect). This was followed closely by the lithium Frenkel defect (1.44 eV per defect), which ensures a high lithium content in the material and inclination for lithium diffusion from formation of vacancies. Li self-diffusion is three dimensional and exhibits a curved pathway with a migration barrier of 0.53 eV. We considered a variety of dopants with charges +1 (Na, K and Rb), +2 (Mg, Ca, Sr and Ba), +3 (Ga, Fe, Co, Ni, Mn, Sc, Y and La) and +4 (Si, Ge, Ti, Zr and Ce) on the Al site. Dopants Mg2+ and Ge4+ can facilitate the formation of Li interstitials and Li vacancies, respectively. Trivalent dopants Fe3+, Ni3+ and Mn3+ prefer to occupy the Al site with exoergic solution energies meaning that they are candidate dopants for the synthesis of Li (Al, M) O2 (M = Fe, Ni and Mn) compounds

The CiCs(SiI)n defect in silicon from a density functional theory perspective

Carbon is an important defect in silicon (Si) as it can interact with intrinsic point defects and affect the operation of devices. In heavily irradiated Si containing carbon the initially produced carbon interstitial - carbon substitutional (CiCs) defect can associate with self-interstitials (SiI’s) to form, in the course of irradiation, the CiCs(SiI) defect and further to form larger complexes namely CiCs(SiI)n defects by the sequential trapping of self-interstitials defects. In the present study, we use density functional theory to clarify the structure and energetics of the CiCs(SiI)n defects. Here we report that the lowest energy CiCs(SiI) and CiCs(SiI)2 defects are strongly bound with -2.77 eV and -5.30 eV, respectively