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Ordered mesoscale structures in 2D materials induced by small misorientationshave opened pathways for a wide variety of novel electronic, ferroelectric, andquantum phenomena. Until now, the only mechanism to induce this periodicordering was via mechanical rotations between the layers, with the periodicityof the resulting moir\'e pattern being directly related to twist angle. Here wereport a fundamentally new mechanism for emergence of mesoscopic periodicpatterns in multilayer sulfur-containing metal phosphorous trichalcogenide,MnPS$_{3}$, induced by the electron beam. The formation under the beam ofperiodic hexagonal patterns with several characteristic length scales,nucleation and transitions between the phases, and local dynamics aredemonstrated. The associated mechanisms are attributed to the relativecontraction of the layers caused by beam-induced sulphur vacancy formation withsubsequent ordering and lattice parameter change. As a result, the plasmonicresponse of the system is locally altered, suggesting an element of controlover plasmon resonances by electron beam patterning. We pose that harnessingthis phenomenon provides both insight into fundamental physics of quantummaterials and opens a pathway towards device applications by enablingcontrolled periodic potentials on the atomic scale.

Electron-beam induced emergence of mesoscopic ordering in layered MnPS$_{3}$