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Jarillo-Herrero, Pablo

The single-particle and many-body properties of twisted bilayer graphene (TBG) can be dramatically 1 different from those of a single graphene layer, in particular when the two layers are rotated relative 2 to each other by a small angle ��≈��∘1–6. Here, we probe for the first time collective excitations of TBG 3 graphene with 20 nanometer spatial resolution, by applying mid-infrared (MIR) near-field optical 4 microscopy. We unveil a propagating plasmon mode in charge-neutral TBG with ��=��.��−��.��∘, which 5 is dramatically different from the ordinary single-layer graphene intraband plasmon7,8. We interpret it 6 as an interband plasmon associated with the optical transitions between minibands originating from 7 the moiré superlattice9,10. The details of the plasmon dispersion are directly related to the motion of 8 electrons in the moiré superlattice and offer invaluable insight into a plethora of physical properties, 9 such as the band nesting between flat band and remote band10, local interlayer coupling, losses etc. We 10 find a strongly reduced interlayer coupling in the regions with AA-stacking, pointing at screening due 11 to electron-electron (e-e) interactions. Optical nano-imaging studies of TBG pave the way to spatially 12 probe interactions effects at the nanoscale11, it could potentially elucidate the contribution of collective excitations to many-body ground states12, and it unveils itself as a new platform for strong light-matter 14 interactions and quantum plasmonic studies and devices13.

Following the recent isolation of monolayer CrI3 [1], there has been a surge of new two-dimensional van der Waals magnetic materials [2-12], whose incorporation in van der Waals heterostructures offers a new platform for spintronics [5-9], proximity magnetism [13], and quantum spin liquids [14]. A primary question in this burgeoning field is how exfoliating crystals to the few-layer limit influences their magnetism. Studies on CrI3 have shown a different magnetic ground state for ultrathin exfoliated films [1,5,6] but the origin is not yet understood. Here, we use electron tunneling through few-layer crystals of the layered antiferromagnetic insulator CrCl3 to probe its magnetic order, finding a ten-fold enhancement in the interlayer exchange compared to bulk crystals. Moreover, temperature- and polarization-dependent Raman spectroscopy reveal that the crystallographic phase transition of bulk crystals does not occur in exfoliated films. This results in a different low temperature stacking order and, we hypothesize, increased interlayer exchange. Our study provides new insight into the connection between stacking order and interlayer interactions in novel two-dimensional magnets, which may be relevant for correlating stacking faults and mechanical deformations with the magnetic ground states of other more exotic layered magnets, such as RuCl3 [14].

Following the recent isolation of monolayer CrI3, many more two-dimensional van der Waals magnetic materials have been isolated. Their incorporation in van der Waals heterostructures offers a new platform for spintronics proximity magnetism and quantum spin liquids. A primary question in this field is how exfoliating crystals to the few-layer limit influences their magnetism. Studies of CrI3 have shown a different magnetic ground state for ultrathin exfoliated films compared with the bulk, but the origin is not yet understood. Here, we use electron tunnelling through few-layer crystals of the layered antiferromagnetic insulator CrCl3 to probe its magnetic order and find a tenfold enhancement of the interlayer exchange compared with bulk crystals. Moreover, temperature- and polarization-dependent Raman spectroscopy reveals that the crystallographic phase transition of bulk crystals does not occur in exfoliated films. This results in a different low-temperature stacking order and, we hypothesize, increased interlayer exchange. Our study provides insight into the connection between stacking order and interlayer interactions in two-dimensional magnets, which may be relevant for correlating stacking faults and mechanical deformations with the magnetic ground states of other more exotic layered magnets such as RuCl3.