The large-scale synthesis of high-quality thin films with extensive tunability derived from molecular building blocks will advance the development of artificial solids with designed functionalities. We report the synthesis of two-dimensional (2D) porphyrin polymer films with wafer-scale homogeneity in the ultimate limit of monolayer thickness by growing films at a sharp pentane/water interface, which allows the fabrication of their hybrid superlattices. Laminar assembly polymerization of porphyrin monomers could form monolayers of metal-organic frameworks with Cu2+ linkers or covalent organic frameworks with terephthalaldehyde linkers. Both the lattice structures and optical properties of these 2D films were directly controlled by the molecular monomers and polymerization chemistries. The 2D polymers were used to fabricate arrays of hybrid superlattices with molybdenum disulfide that could be used in electrical capacitors.

The emergence of two-dimensional (2D) magnetic crystals and moiré engineering of van der Waals materials has opened the door for devising new magnetic ground states via competing interactions in moiré superlattices 1-9 . Although a suite of interesting phenomena, including multi-flavor magnetic states 10 , noncollinear magnetic states 10-13 , moiré magnon bands and magnon networks 14 , has been predicted in twisted bilayer magnetic crystals, nontrivial magnetic ground states have yet to be realized. Here, by utilizing the stacking-dependent interlayer exchange interactions in CrI3 (Ref. 15, 16 ), we demonstrate in small-twist-angle CrI3 bilayers a noncollinear magnetic ground state. It consists of antiferromagnetic (AF) and ferromagnetic (FM) domains and is a result of the competing interlayer AF coupling in the monoclinic stacking regions of the moiré superlattice and the energy cost for forming AF-FM domain walls. Above a critical twist angle of ~ 𝟑°, the noncollinear state transitions to a collinear FM ground state. We further show that the noncollinear magnetic state can be controlled by electrical gating through the doping-dependent interlayer AF interaction. Our results demonstrate the possibility of engineering new magnetic ground states in twisted bilayer magnetic crystals, as well as gate-voltage-controllable high-density magnetic memory storage.Moiré superlattices built on twisted bilayers of van der Waals materials have presented an exciting platform for studying correlated states of matter with unprecedented controllability [7][8][9] . In addition to graphene and transition metal dichalcogenide moiré materials 17 , recent theoretical studies have predicted the emergence of new magnetic ground states in twisted bilayers of 2D magnetic crystals [10][11][12][13][14] . These states are originated from the stacking-dependent interlayer exchange interactions in magnetic moiré superlattices. Two-dimensional CrI3 (similarly CrBr3 18 and CrCl3 19 ), in which stackingdependent interlayer magnetic ground states have been demonstrated by recent experiments 15, 16 , is a good candidate for exploring moiré magnetism.

The densification of integrated circuits requires thermal management strategies and high thermal conductivity materials1–3. Recent innovations include the development of materials with thermal conduction anisotropy, which can remove hotspots along the fast-axis direction and provide thermal insulation along the slow axis4,5. However, most artificially engineered thermal conductors have anisotropy ratios much smaller than those seen in naturally anisotropic materials. Here we report extremely anisotropic thermal conductors based on large-area van der Waals thin films with random interlayer rotations, which produce a room-temperature thermal anisotropy ratio close to 900 in MoS2, one of the highest ever reported. This is enabled by the interlayer rotations that impede the through-plane thermal transport, while the long-range intralayer crystallinity maintains high in-plane thermal conductivity. We measure ultralow thermal conductivities in the through-plane direction for MoS2 (57 ± 3 mW m−1 K−1) and WS2 (41 ± 3 mW m−1 K−1) films, and we quantitatively explain these values using molecular dynamics simulations that reveal one-dimensional glass-like thermal transport. Conversely, the in-plane thermal conductivity in these MoS2 films is close to the single-crystal value. Covering nanofabricated gold electrodes with our anisotropic films prevents overheating of the electrodes and blocks heat from reaching the device surface. Our work establishes interlayer rotation in crystalline layered materials as a new degree of freedom for engineering-directed heat transport in solid-state systems.

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Quantum computing based on superconducting qubits requires the understanding and control of the materials, device architecture, and operation. However, the materials for the central circuit element, the Josephson junction, have mostly been focused on using the AlO x tunnel barrier. Here, we demonstrate Josephson junctions and superconducting qubits employing two-dimensional materials as the tunnel barrier. We batch-fabricate and design the critical Josephson current of these devices via layer-by-layer stacking N layers of MoS2 on the large scale. Based on such junctions, MoS2 transmon qubits are engineered and characterized in a bulk superconducting microwave resonator for the first time. Our work allows Josephson junctions to access the diverse material properties of two-dimensional materials that include a wide range of electrical and magnetic properties, which can be used to study the effects of different material properties in superconducting qubits and to engineer novel quantum circuit elements in the future.

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The emergence of two-dimensional (2D) magnetic crystals and moiré engineering of van der Waals materials has opened the door for devising new magnetic ground states via competing interactions in moiré superlattices. Although a suite of interesting phenomena, including multi-flavor magnetic states, noncollinear magnetic states, moiré magnon bands and magnon networks, has been predicted in twisted bilayer magnetic crystals, nontrivial magnetic ground states have yet to be realized. Here, by utilizing the stacking-dependent interlayer exchange interactions in CrI3, we demonstrate in small-twist-angle CrI3 bilayers a noncollinear magnetic ground state. It consists of antiferromagnetic (AF) and ferromagnetic (FM) domains and is a result of the competing interlayer AF coupling in the monoclinic stacking regions of the moiré superlattice and the energy cost for forming AF-FM domain walls. Above a critical twist angle of ~ 3°, the noncollinear state transitions to a collinear FM ground state. We further show that the noncollinear magnetic state can be controlled by electrical gating through the doping-dependent interlayer AF interaction. Our results demonstrate the possibility of engineering new magnetic ground states in twisted bilayer magnetic crystals, as well as gate-voltage-controllable high-density magnetic memory storage.

This is an Accepted Manuscript for the Microscopy and Microanalysis 2020 Proceedings. This version may be subject to change during the production process.