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Van der Waals materials with long-range magnetic order show a range of correlated phenomena that could be of use in the development of optoelectronic and spintronic applications. Magnetically ordered van der Waals semiconductors with spin-polarized currents are, in particular, sensitive to external stimuli such as strain, electrostatic fields, magnetic fields and electromagnetic radiation. Their combination of two-dimensional magnetic order, semiconducting band structure and weak dielectric screening means that these materials could be used to create novel atomically thin opto-spintronic devices. Here we explore the development of van der Waals opto-spintronics. We examine the interplay between optical, magnetic and electronic excitations in van der Waals magnetic semiconductors, and explore the control of their magnetization via external stimuli. We consider fabrication and passivation strategies for the practical handling and design of opto-spintronic devices. We also explore potential opto-spintronic device architectures and applications, which include magnonics, quantum transduction, neuromorphic computing and non-volatile memory. 

α-RuCl3 is a layered transition metal halide that possesses a range of exotic magnetic, optical, and electronic properties including fractional excitations indicative of a proximate Kitaev quantum spin liquid (QSL). While previous reports have explored these properties on idealized single crystals or mechanically exfoliated samples, the scalable production of α-RuCl3 nanosheets has not yet been demonstrated. Here, we perform liquid-phase exfoliation (LPE) of α-RuCl3 through an electrochemically assisted approach, which yields ultrathin, electron-doped α-RuCl3 nanosheets that are then assembled into electrically conductive large-area thin films. The crystalline integrity of the α-RuCl3 nanosheets following LPE is confirmed through a wide range of structural and chemical analyses. Moreover, the physical properties of the LPE α-RuCl3 nanosheets are investigated through electrical, optical, and magnetic characterization methods, which reveal a structural phase transition at 230 K that is consistent with the onset of Kitaev paramagnetism in addition to an antiferromagnetic transition at 2.6 K. Intercalated ions from the electrochemical LPE protocol favorably alter the optical response of the α-RuCl3 nanosheets, enabling large-area Mott insulator photodetectors that operate at telecommunications-relevant infrared wavelengths near 1.55 μm. These photodetectors show a linear photocurrent response as a function of incident power, which suggests negligible trap-mediated recombination or photothermal effects, ultimately resulting in a photoresponsivity of ≈2 mA/W. 

Abstract Transition metal dichalcogenides (TMDs) are known for their layered structure and tunable functional properties. However, a unified understanding on other transition metal chalcogenides (i.e. M 2 X) is still lacking. Here, the relatively new class of copper-based chalcogenides Cu 2 X (X = Te, Se, S) is thoroughly reported. Cu 2 X are synthesized by an unusual vapor–liquid assisted growth on a Al 2 O 3 /Cu/W stack. Liquid copper plays a significant role in synthesizing these layered systems, and sapphire assists with lateral growth and exfoliation. Similar to traditional TMDs, thickness dependent phonon signatures are observed, and high-resolution atomic images reveal the single phase Cu 2 Te that prefers to grow in lattice-matched layers. Charge transport measurements indicate a metallic nature at room temperature with a transition to a semiconducting nature at low temperatures accompanied by a phase transition, in agreement with band structure calculations. These findings establish a fundamental understanding and thrust Cu 2 Te as a flexible candidate for wide applications from photovoltaics and sensors to nanoelectronics. 

Two-dimensional (2D) materials have attracted attention for quantum information science due to their ability to host single-photon emitters (SPEs). Although the properties of atomically thin materials are highly sensitive to surface modification, chemical functionalization remains unexplored in the design and control of 2D material SPEs. Here, we report a chemomechanical approach to modify SPEs in monolayer WSe₂through the synergistic combination of localized mechanical strain and noncovalent surface functionalization with aryl diazonium chemistry. Following the deposition of an aryl oligomer adlayer, the spectrally complex defect-related emission of strained monolayer WSe₂is simplified into spectrally isolated SPEs with high single-photon purity. Density functional theory calculations reveal energetic alignment between WSe₂defect states and adsorbed aryl oligomer energy levels, thus providing insight into the observed chemomechanically modified quantum emission. By revealing conditions under which chemical functionalization tunes SPEs, this work broadens the parameter space for controlling quantum emission in 2D materials.