ZnO has emerged as a promising candidate for optoelectronic and microelectronic applications, whose development requires greater understanding and control of their electronic contacts. The rapid pace of ZnO research over the past decade has yielded considerable new information on the nature of ZnO interfaces with metals. Work on ZnO contacts over the past decade has now been carried out on high quality material, nearly free from complicating factors such as impurities, morphological and native point defects. Based on the high quality bulk and thin film crystals now available, ZnO exhibits a range of systematic interface electronic structure that can be understood at the atomic scale. Here we provide a comprehensive review of Schottky barrier and ohmic contacts including work extending over the past half century. For Schottky barriers, these results span the nature of ZnO surface charge transfer, the roles of surface cleaning, crystal quality, chemical interactions, and defect formation. For ohmic contacts, these studies encompass the nature of metal-specific interactions, the role of annealing, multilayered contacts, alloyed contacts, metallization schemes for state-of-the-art contacts, and their application to n-type versus p-type ZnO. Both ZnO Schottky barriers and ohmic contacts show a wide range of phenomena and electronic behavior, which can all be directly tied to chemical and structural changes on an atomic scale.
Self-compensation, the tendency of a crystal to lower its energy by forming point defects to counter the effects of a dopant, is here quantitatively proven. Based on a new theoretical formalism and several different experimental techniques we demonstrate that the addition of 1.4 x 10 21 -cm -3 Ga donors in ZnO causes the lattice to form 1.7 x 10 20 -cm -3 Zn-vacancy acceptors. The calculated V Zn formation energy of 0.2 eV is consistent with predictions from density functional theory. Our formalism is of general validity and can be used to investigate self-compensation in any degenerate semiconductor material.2
A conversion from ohmic to rectifying behavior is observed for Au contacts on atomically ordered polar ZnO surfaces following remote, room-temperature oxygen plasma treatment. This transition is accompanied by reduction of the “green” deep level cathodoluminescence emission, suppression of the hydrogen donor-bound exciton photoluminescence and a ∼0.75eV increase in n-type band bending observed via x-ray photoemission. These results demonstrate that the contact type conversion involves more than one mechanism, specifically, removal of the adsorbate-induced accumulation layer plus lowered tunneling due to reduction of near-surface donor density and defect-assisted hopping transport.
The covalent functionalization of 2D crystals is an emerging route for tailoring the electronic structure and generating novel phenomena. Understanding the influence of ligand chemistry will enable the rational tailoring of their properties. Through the synthesis of numerous ligand-functionalized germanane crystals, we establish the role of ligand size and electronegativity on functionalization density, framework structure, and electronic structure. Nearly uniform termination only occurs with small ligands. Ligands that are too sterically bulky will lead to partial hydrogen termination of the framework. With a homogeneous distribution of different ligands, the band gaps and Raman shifts are dictated by their relative stoichiometry in a pseudolinear fashion similar to Vegard's law. Larger and more electronegative ligands expand the germanane framework, thereby lowering the band gap and Raman shift. Simply by changing the identity of the organic ligand, the band gap can be tuned by ∼15%, highlighting the power of functionalization chemistry to manipulate the properties of single-atom thick materials.
Electronic Structure of Tantalum Oxynitride Perovskite Photocatalysts. -The absolute conduction and valence band energy levels of MTaO2N (M: Ca, Sr, Ba) and PrTaON2, which are promising candidates for photocatalytic splitting of water under visible light irradiation, are determined by a combination of XPS, Kelvin probe force microscopy, UV/VIS spectroscopy, and depth-resolved cathodoluminescence spectroscopy. All four compounds have conduction band edges that lie above the reduction potential for water and valence band edges which lie near the oxidation potential of water. The position of the conduction band edge is closely linked to the Ta-O/N-Ta bond angles, whereas the position of the valence band edge is more sensitive to the oxygen--to-nitrogen ratio. -(BALAZ*, S.; PORTER, S. H.; WOODWARD, P. M.; BRILLSON, L. J.; Chem. Mater. 25 (2013) 16, 3337-3343,
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