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2D magnetic materials hold promise for quantum and spintronic applications. 2D antiferromagnetic materials are of particular interest due to their relative insensitivity to external magnetic fields and higher switching speeds compared to 2D ferromagnets. However, their lack of macroscopic magnetization impedes detection and control of antiferromagnetic order, thus motivating magneto‐electrical measurements for these purposes. Additionally, many 2D magnetic materials are ambient‐reactive and electrically insulating or highly resistive below their magnetic ordering temperatures, which imposes severe constraints on electronic device fabrication and characterization. Herein, these issues are overcome via a fabrication protocol that achieves electrically conductive devices from the ambient‐reactive 2D antiferromagnetic semiconductor NiI₂. The resulting gate‐tunable transistors show band‐like electronic transport below the antiferromagnetic and multiferroic transition temperatures of NiI₂, revealing a Hall mobility of 15 cm² V⁻¹ s⁻¹at 1.7 K. These devices also allow direct electrical probing of the thickness‐dependent multiferroic phase transition temperature of NiI₂from 59 K (bulk) to 28 K (monolayer).

 

Mixed-dimensional van der Waals heterojunctions involve interfacing materials with different dimensionalities, such as a 2D transition metal dichalcogenide and a 0D organic semiconductor. These heterojunctions have shown unique interfacial properties not found in either individual component. Here, we use femtosecond transient absorption to reveal photoinduced charge transfer and interlayer exciton formation in a mixed-dimensional type-II heterojunction between monolayer MoS2 and vanadyl phthalocyanine (VOPc). Selective excitation of the MoS2 exciton leads to hole transfer from the MoS2 valence band to VOPc highest occupied molecular orbit in ∼710 fs. On the contrary, selective photoexcitation of the VOPc layer leads to instantaneous electron transfer from its excited state to the conduction band of MoS2 in less than 100 fs. This light-initiated ultrafast separation of electrons and holes across the heterojunction interface leads to the formation of an interlayer exciton. These interlayer excitons formed across the interface lead to longer-lived charge-separated states of up to 2.5 ns, longer than in each individual layer of this heterojunction. Thus, the longer charge-separated state along with ultrafast charge transfer times provide promising results for photovoltaic and optoelectronic device applications.

 

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. 

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.