Scalable fabrication of vertically arranged Bi2Se3 crossbar arrays for memristive device applications

Despite the unique advantages of the memristive switching devices based on two-dimensional (2D) transition metal dichalcogenides, scalable growth technologies of such 2D materials and wafer-level fabrication remain challenging. In this work, we present the gold-assisted large-area physical vapor deposition (PVD) growth of Bi2Se3 features for the scalable fabrication of 2D-material-based crossbar arrays of memristor devices. This work indicates that gold layers, prepatterned by photolithography processes, can catalyze PVD growth of few-layer Bi2Se3 with 100-folds larger crystal grain size in comparison with that grown on bare Si/SiO2 substrates. We also present a fluid-guided growth strategy to improve growth selectivity of Bi2Se3 on Au layers. Through the experimental and computational analyses, we identify two key processing parameters, i.e., the distance between Bi2Se3 powder and the target substrate and the distance between the leading edges of the substrate and the substrate holder with a hollow interior, which plays a critical role in realizing large-scale growth. By optimizing these growth parameters, we have successfully demonstrated cm-scale highly-selective Bi2Se3 growth on crossbar-arrayed structures with an in-lab yield of 86%. The whole process is etch- and plasma-free, substantially minimizing the damage to the crystal structure and also preventing the formation of rough 2D-material surfaces. Furthermore, we also preliminarily demonstrated memristive devices, which exhibit reproducible resistance switching characteristics (over 50 cycles) and a retention time of up to 106 s. This work provides a useful guideline for the scalable fabrication of vertically arranged crossbar arrays of 2D-material-based memristive devices, which is critical to the implementation of such devices for practical neuromorphic applications.