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Tungsten trioxide is a versatile material with widespread applicationsranging from electrochromic and optoelectronic devices to water splitting andcatalysis of chemical reactions. For technological applications, thin films ofWO3 are particularly appealing, taking advantage from high surface-to-volumeratio and tunable physical properties. However, the growth of stoichiometric,crystalline thin films is challenging because the deposition conditions arevery sensitive to the formation of oxygen vacancies. In this work, we show howbackground oxygen pressure during pulsed laser deposition can be used to tunethe structural and electronic properties of WO3 thin films. By performing X-raydiffraction and low-temperature transport measurements, we find changes in WO3lattice volume up to 10%, concomitantly with an insulator-to-metal transitionas a function of increased level of electron doping. We use advanced ab initiocalculations to describe in detail the properties of the oxygen vacancy defectstates, and their evolution in terms of excess charge concentration. Ourresults depict an intriguing scenario where structural, electronic, optical,and transport properties of WO3 single-crystal thin films can all be purposelytuned by a suited control of oxygen vacancies formation during growth.

Charge doping and large lattice expansion in oxygen-deficient heteroepitaxial WO3