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  1. Abstract

    Chalcogen vacancies in the semiconducting monolayer transition-metal dichalcogenides (TMDs) have frequently been invoked to explain a wide range of phenomena, including both unintentional p-type and n-type conductivity, as well as sub-band gap defect levels measured via tunneling or optical spectroscopy. These conflicting interpretations of the deep versus shallow nature of the chalcogen vacancies are due in part to shortcomings in prior first-principles calculations of defects in the semiconducting two-dimensional TMDs that have been used to explain experimental observations. Here we report results of hybrid density functional calculations for the chalcogen vacancy in a series of monolayer TMDs, correctly referencing the thermodynamic charge transition levels to the fundamental band gap (as opposed to the optical band gap). We find that the chalcogen vacancies are deep acceptors and cannot lead to n-type or p-type conductivity. Both the (0/−1) and (−1/−2) transition levels occur in the gap, leading to paramagnetic charge statesS=1/2andS = 1, respectively, in a collinear-spin representation. We discuss trends in terms of the band alignments between the TMDs, which can serve as a guide to future experimental studies of vacancy behavior.

     
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  2. Free, publicly-accessible full text available September 12, 2024
  3. The oxides of platinum group metals are promising for future electronics and spintronics due to the delicate interplay of spin-orbit coupling and electron correlation energies. However, their synthesis as thin films remains challenging due to their low vapour pressures and low oxidation potentials. Here we show how epitaxial strain can be used as a control knob to enhance metal oxidation. Using Ir as an example, we demonstrate the use of epitaxial strain in engineering its oxidation chemistry, enabling phase-pure Ir or IrO2 films despite using identical growth conditions. The observations are explained using a density-functional-theory-based modified formation enthalpy framework, which highlights the important role of metal-substrate epitaxial strain in governing the oxide formation enthalpy. We also validate the generality of this principle by demonstrating epitaxial strain effect on Ru oxidation. The IrO2 films studied in our work further revealed quantum oscillations, attesting to the excellent film quality. The epitaxial strain approach we present could enable growth of oxide films of hard-to-oxidize elements using strain engineering. 
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    Free, publicly-accessible full text available May 22, 2024
  4. Abstract Germanium-based oxides such as rutile GeO 2 are garnering attention owing to their wide band gaps and the prospects of ambipolar doping for application in high-power devices. Here, we present the use of germanium tetraisopropoxide (GTIP), a metal-organic chemical precursor, as a source of germanium for the demonstration of hybrid molecular beam epitaxy for germanium-containing compounds. We use Sn 1- x Ge x O 2 and SrSn 1- x Ge x O 3 as model systems to demonstrate our synthesis method. A combination of high-resolution X-ray diffraction, scanning transmission electron microscopy, and X-ray photoelectron spectroscopy confirms the successful growth of epitaxial rutile Sn 1- x Ge x O 2 on TiO 2 (001) substrates up to x  = 0.54 and coherent perovskite SrSn 1- x Ge x O 3 on GdScO 3 (110) substrates up to x  = 0.16. Characterization and first-principles calculations corroborate that germanium occupies the tin site, as opposed to the strontium site. These findings confirm the viability of the GTIP precursor for the growth of germanium-containing oxides by hybrid molecular beam epitaxy, thus providing a promising route to high-quality perovskite germanate films. 
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