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Colloidal ultrathin 2D MoS2 nanoplatelets and nanosheets provide a toolbox for future spin- and valleytronic applications. Colloidal chemistry offers innovative strategies to tune the materials' optoelectronic properties from metallic to semiconducting.

2D metal monochalcogenides have recently attracted interest for photoelectrochemical (PEC) applications in aqueous electrolytes. Their optical bandgap in the visible and near-infrared spectral region is adequate for energy conversion and photodetection/sensing. Their large surface-to-volume ratio guarantees that the charge carriers are photogenerated at the material/electrolyte interface, where redox reactions occur, minimizing recombination processes. However, solution-processed photoelectrodes based on these materials exhibit energy conversion efficiencies that are far from the current state of the art expressed by established technologies. This work reports a systematic morphological, spectroscopic, and PEC characterization of solution-processed films of photoactive InSe flakes for PEC-type photodetectors. By optimizing the thickness and hybridizing InSe flakes with electrically conductive Sn:In2O3(ITO) nanocrystals, photoanodes with a significant photoanodic response in both acidic and alkaline media are designed, reaching responsivity up to 60.0 mA W−1(external quantum efficiency = 16.4%) at +0.4 V versus RHE under visible illumination. In addition, a strategy based on the use of sacrificial agents (i.e., 2-propanol and Na2SO3) is proposed to improve the stability of the InSe and ITO/InSe photodetectors. Our data confirm the potential of 2D InSe for PEC energy conversion and sensing applications, remarking the challenges related to InSe stability during anodic operation.

Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have a thickness-tunable band gap in the semiconducting crystal phase and – in monolayer form – exhibit a direct band gap. TMDCs are highly promising for spin- and valleytronics and show an ultrafast response to external (optical) stimuli, an essential feature for optoelectronics. However, up to now, colloidal synthesis routes for ultrathin TMDCs typically yield different shapes and crystal phases and a thorough understanding of the product guiding reaction mechanism is missing. We investigate the colloidal synthesis of ultrathin MoS2 nanoplatelets (8 nm ± 4 nm) and nanosheets (22 nm ± 9 nm) in terms of the evolution of crystal phase and shape over the course of their formation. The reaction is followed by X-ray photoelectron spectroscopy, showing that a mixture of the semiconducting 2H and the metallic 1T crystal phase is formed initially, regardless of the molybdenum oleate precursor concentration used for the reaction. A low precursor concentration however leads to the formation of MoS2 nanoplatelets, while a high concentration yields laterally larger MoS2 nanosheets. Both structures have undergone a full transition to the semiconducting 2H crystal phase by the end of the reaction. Phase pure semiconducting MoS2 nanoplatelets with a lateral size approaching the MoS2 exciton Bohr radius exhibit strong additional lateral quantum confinement leading to a drastically shortened decay of the B-exciton, which we characterize by ultrafast transient absorption spectroscopy. Our results offer a straight-forward synthesis strategy to phase pure semiconducting 2D MoS2 and represent an important starting point for chemically exploring upcoming colloidal TMDC heterostructures for optical applications.

α-RuCl

2D magnets represent material systems in which magnetic order and topological phase transitions can be observed. Based on these phenomena, novel types of computing architectures and magnetoelectronic devices can be envisaged. Unlike conventional magnetic films, their magnetism is independent of the substrate and interface qualities, and 2D magnetic properties manifest even in formally bulk single crystals. However, 2D magnetism in layered materials is rarely reported often due to weak exchange interactions and magnetic anisotropy, and low magnetic transition temperatures. Here, the electron spin resonance (ESR) properties of a layered antiferromagnetic CrSBr single crystal are reported. The W-like shape angular dependence of the ESR linewidth provides a signature for room temperature spin–spin correlations and for the XY spin model. By approaching the Néel temperature the arising of competing intralayer ferromagnetic and interlayer antiferromagnetic interactions might lead to the formation of vortex and antivortex pairs. This argument is inferred by modeling the temperature dependence of the ESR linewidth with the topological Berezinskii-Kosterlitz-Thouless phase transition. These findings together with the chemical stability and semiconducting properties, make CrSBr a promising layered magnet for future magneto- and topological-electronics.

Magnetic van der Waals (vdW) materials offer a fantastic platform to investigate and exploit rich spin configurations stabilized in reduced dimensions. One tantalizing magnetic order is the interlayer antiferromagnetism in A-type vdW antiferromagnet, which may be effectively modified by the magnetic field, stacking order and thickness scaling. However, atomically revealing the interlayer spin orientation in the vdW antiferromagnet is highly challenging, because most of the material candidates exhibit an insulating ground state or instability in ambient conditions. Here, we report the layer-dependent interlayer antiferromagnetic reorientation in air-stable semiconductor CrSBr using magnetotransport characterization and first-principles calculations. We reveal a pronounced odd-even layer effect of interlayer reorientation, which originates from the competitions among interlayer exchange, magnetic anisotropy energy and extra Zeeman energy of uncompensated magnetization. Furthermore, we quantitatively constructed the layer-dependent magnetic phase diagram with the help of a linear-chain model. Our work uncovers the layer-dependent interlayer antiferromagnetic reorientation engineered by magnetic field in the air-stable semiconductor, which could contribute to future vdW spintronic devices.