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Inter-twisted bilayers of two-dimensional (2D) materials can host low-energyflat bands, which offer opportunity to investigate many intriguing physicsassociated with strong electron correlations. In the existing systems,ultra-flat bands only emerge at very small twist angles less than a fewdegrees, which poses challenge for experimental study and practicalapplications. Here, we propose a new design principle to achieve low-energyultra-flat bands with increased twist angles. The key condition is to have a 2Dsemiconducting material with large energy difference of band edges controlledby stacking. We show that the interlayer interaction leads to defect-likestates under twisting, which forms a flat band in the semiconducting band gapwith dispersion strongly suppressed by the large energy barriers in the moiresuperlattice even for large twist angles. We explicitly demonstrate our idea inbilayer alpha-In2Se3 and bilayer InSe. For bilayer alpha-In2Se3, we show that atwist angle -13.2 degree is sufficient to achieve the band flatness comparableto that of twist bilayer graphene at the magic angle -1.1 degree. In addition,the appearance of ultra-flat bands here is not sensitive to the twist angle asin bilayer graphene, and it can be further controlled by external gate fields.Our finding provides a new route to achieve ultra-flat bands other thanreducing the twist angles and paves the way towards engineering such flat bandsin a large family of 2D materials.

Designing Ultra-Flat Bands in Twisted Bilayer Materials at Large Twist Angles without specific degree