Micro-tip manipulated origami for robust twisted few-layer graphene

Twisted few-layer graphene (tFLG) has emerged as an ideal model system for investigating novel strongly correlated and topological phenomena. However, the experimental construction of tFLG with high structural stability is still challenging. Here, we introduce a highly accessible method for fabricating robust tFLG by polymer micro-tip manipulated origami. Through using a self-prepared polymer micro-tip—which is composed of multiple dimethylpolysiloxane, poly(vinyl chloride), and graphite sheets—to fold graphene layers, we fabricated tFLG with different twist angles (0°–30°) and various layers, including twisted bilayers (1 + 1), twisted double-bilayers (2 + 2), twisted double-trilayers (3 + 3), and thicker layers. Even ABC-stacked tFLG were created, such as twisted ABC/ABC and ABC/ABA graphene coexisting in an ABC-ABA domain wall region. We found that the origami-fabricated tFLG exhibits high stability against thermal and mechanical perturbations including heating and transferring, which could be attributed to its special folding and tearing structures. Moreover, based on the rich types of samples, we revealed twist-angle- and stacking-order-dependent Raman characteristics of tFLG, which are valuable for understanding stacking-modulated phonon spectroscopy. Our experiments provide a simple and efficient approach to construct structurally robust tFLG, paving the way for the study of highly stable twisted van der Waals heterostructures.