Evidence of Noncollinear Spin Texture in Magnetic Moiré Superlattices

Abstract

Moiré magnetism, parallel with moiré electronics that has led to novel correlated and topological electronic states, emerges as a new venue to design and control exotic magnetic phases in twisted magnetic two-dimensional(2D) crystals. Here, we report direct evidence of noncollinear spin texture in 2D twisted double bilayer (tDB) magnet chromium triiodide (CrI${}_3$). Using magneto-optical spectroscopy in tDB CrI${}_3$, we revealed the presence of a net magnetization, unexpected from the composing antiferromagnetic bilayers with compensated magnetizations, and the emergence of noncollinear spins, originated from the moiré exchange coupling-induced spin frustrations. Exploring the twist angle dependence, we demonstrated that both features are present in tDB CrI${}_3$ with twist angles from 0.5${}^o$ to 5${}^o$, but are most prominent in the 1.1${}^o$ tDB CrI${}_3$. Focusing on the temperature dependence of the 1.1${}^o$ tDB CrI${}_3$, we resolved the dramatic suppression in the net magnetization onset temperature and the significant softening of noncollinear spins, as a result of the moiré induced frustration. Our results demonstrate the power of moiré superlattices in introducing novel magnetic phenomena that are absent in natural 2D magnets.

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