Ultrafast, Kinetically Limited, Ambient Synthesis of Vanadium Dioxides through Laser Direct Writing on Ultrathin Chalcogenide Matrix.

Abstract

Vanadium dioxide (VO₂) is a strongly correlated electronic material and has attracted significant attention due to its metal-to-insulator transition and diverse smart applications. Traditional synthesis of VO₂ usually requires minutes or hours of global heating and low oxygen partial pressure to achieve thermodynamic control of the valence state. Further patterning of VO₂ through a series of lithography and etching processes may inevitably change its surface valence, which poses a great challenge for the assembly of micro- and nanoscale VO₂-based heterojunction devices. Herein, we report an ultrafast method to simultaneously synthesize and pattern VO₂ on the time scale of seconds under ambient conditions through laser direct writing on a V₅S₈ "canvas". The successful ambient synthesis of VO₂ is attributed to the ultrafast local heating and cooling process, resulting in controlled freezing of the intermediate oxidation phase during the relatively long kinetic reaction. A Mott memristor based on a V₅S₈-VO₂-V₅S₈ lateral heterostructure can be fabricated and integrated with a MoS₂ channel, delivering a transistor with abrupt switching transfer characteristics. The other device with a VS<i>_x</i>O<i>_y</i> channel exhibits a large negative temperature coefficient of approximately 4.5%/K, which is highly desirable for microbolometers. The proposed approach enables fast and efficient integration of VO₂-based heterojunction devices and is applicable to other intriguing intermediate phases of oxides.