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The polar interface between LaAlO$_{3}$ and SrTiO$_{3}$ has shown promise as a field effect transistor, with reduced (nanoscale) feature sizes and potentially added functionality over conventional semiconductor systems. However, the mobility of the interfacial two-dimensional electron gas (2DEG) is lower than desirable. Therefore to progress, the highly debated origin of the 2DEG must be understood. Here we present a case for surface redox reactions as the origin of the 2DEG, in particular surface O vacancies, using a model supported by first principles calculations that describes the redox formation. In agreement with recent spectroscopic and transport measurements, we predict a stabilization of such redox processes (and hence Ti 3$d$ occupation) with film thickness beyond a critical value, which can be smaller than the critical thickness for 2D electronic conduction, since the surface defects generate trapping potentials that will affect the interface electron mobility. Several other recent experimental results, such as lack of core level broadening and shifts, find natural explanation. Pristine systems will likely require changed growth conditions or modified materials with a higher vacancy free energy.
Empowering conventional materials with unexpected magnetoelectric properties is appealing to the multi-functionalization of existing devices and the exploration of future electronics. Recently, owing to its unique effect in modulating a matters prope
We investigate the effect of low-coordinated surface atoms on the defect-induced magnetism in MgO nanocrystallites using hybrid density functional theory calculations. It has been demonstrated that when Mg vacancies are introduced at the corners of c
The needs for efficient heat removal and superior thermal conduction in nano/micro devices have triggered tremendous studies in low-dimensional materials with high thermal conductivity. Hexagonal boron nitride (h-BN) is believed to be one of the cand
In the quest for topological insulators with large band gaps, heterostructures with Rashba spin-orbit interactions come into play. Transition metal oxides with heavy ions are especially interesting in this respect. We discuss the design principles fo
The interfacial behavior of quantum materials leads to emergent phenomena such as two dimensional electron gases, quantum phase transitions, and metastable functional phases. Probes for in situ and real time surface sensitive characterization are cri