Abstract

Transition metal oxides offer functional properties beyond conventional semiconductors. Bridging the gap between the fundamental research frontier in oxide electronics and their realization in commercial devices demands a wafer-scale growth approach for high-quality transition metal oxide thin films. Such a method requires excellent control over the transition metal valence state to avoid performance deterioration, which has been proved challenging. Here we present a scalable growth approach that enables a precise valence state control. By creating an oxygen activity gradient across the wafer, a continuous valence state library is established to directly identify the optimal growth condition. Single-crystalline VO2 thin films have been grown on wafer scale, exhibiting more than four orders of magnitude change in resistivity across the metal-to-insulator transition. It is demonstrated that ‘electronic grade' transition metal oxide films can be realized on a large scale using a combinatorial growth approach, which can be extended to other multivalent oxide systems.

Highlights

  • Transition metal oxides offer functional properties beyond conventional semiconductors

  • Phase pure epitaxial VO2 films have been grown by pulsed laser deposition (PLD)[20,21,22], sputtering[23,24,25], molecular beam epitaxy (MBE)[26,27] and chemical solution deposition technique[28], the growth of high-quality VO2 thin films has been found very demanding[21,26], attributed to the complex and rich structural phase diagram of vanadium oxide[5]

  • This approach has been successfully utilized to optimize the bandgap of III–V semiconductor nanowires[38], discover new luminescent materials[33], study the composition variance of metallic glasses[34], increasing the Curie temperature of the ferromagnetic semiconductor GaMnAs37 and exploring the effect of LaAlO3 cation stoichiometry on electrical properties of the twodimensional electron gas at the LaAlO3/SrTiO3 interface[35]

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Summary

Introduction

Transition metal oxides offer functional properties beyond conventional semiconductors. Such a combinatorial strategy requires (1) precise and direct control of a spatially varying fluxes; (2) two or more sources to independently supply the elements of interest; (3) a favourable deposition geometry, that is, a sufficiently large substrate compared with the flux density profile at sample position to create a sufficiently steep flux gradient; (4) large inelastic mean free path to avoid unintentional gas phase reactions This approach has been successfully utilized to optimize the bandgap of III–V semiconductor nanowires[38], discover new luminescent materials[33], study the composition variance of metallic glasses[34], increasing the Curie temperature of the ferromagnetic semiconductor GaMnAs37 and exploring the effect of LaAlO3 cation stoichiometry on electrical properties of the twodimensional electron gas at the LaAlO3/SrTiO3 interface[35]

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