Two-dimensional superconductor (2DSC) monolayers with non-centrosymmetry exhibit unconventional Ising pair superconductivity and an enhanced upper critical field beyond the Pauli paramagnetic limit, driving intense research interest. However, they are often susceptible to structural disorder and environmental oxidation, which destroy electronic coherence and provide technical challenges in the creation of artificial van der Waals heterostructures (vdWHs) for devices. Herein, we report a general and scalable synthesis of highly crystalline 2DSC monolayers via a mild electrochemical exfoliation method using flexible organic ammonium cations solvated with neutral solvent molecules as co-intercalants. Using NbSe₂ as a model system, we achieved a high yield (>75%) of large-sized single-crystal monolayers up to 300 µm. The as-fabricated, twisted NbSe₂ vdWHs demonstrate high stability, good interfacial properties and a critical current that is modulated by magnetic field when one flux quantum fits to an integer number of moiré cells. Additionally, formulated 2DSC inks can be exploited to fabricate wafer-scale 2D superconducting wire arrays and three-dimensional superconducting composites with desirable morphologies.

具有非中心对称性的二维超导体（2DSC）单层表现出非常规的Ising对超导性和超出Pauli顺磁极限的增强的上临界场，从而引起了强烈的研究兴趣。但是，它们通常易受结构紊乱和环境氧化的影响，这会破坏电子相干性，并在创建用于设备的人工范德华力异质结构（vdWH）时带来技术挑战。本文中，我们报告了一种温和的电化学剥落方法，该方法使用与中性溶剂分子溶剂化的柔性有机铵阳离子作为共嵌入剂，通过温和的电化学剥落方法合成了高度结晶的2DSC单层膜，该方法具有可扩展性。使用NbSe ₂作为模型系统，我们实现了高达300 µm的大型单晶单层的高产率（> 75％）。扭曲的NbSe ₂ vdWHs制备后显示出高稳定性，良好的界面特性以及当一个通量量子适合整数个莫尔面单元时由磁场调制的临界电流。另外，可以利用配制的2DSC油墨来制造晶圆级2D超导线材阵列和具有所需形貌的三维超导复合材料。