Advancing next-generation electronics necessitates precise control of dielectric properties in 2D materials. Here, the first synthesis of novel 2D quasi-van der Waals (vdW) europium oxysulfur (Eu2SOx) compounds, comprising hexagonal Eu₂SO₂ and tetragonal Eu₂SO₆ phases, with composition-tunable dielectric properties, is presented. Using a homodiffusive-controlled epitaxial growth method, materials are achieved with complementary characteristics: the hexagonal Eu₂SO₂ phase exhibits a high dielectric constant (≈30) paired with a moderate bandgap (≈4.56 eV), while the tetragonal Eu₂SO₆ phase offers a wider bandgap (≈5.62 eV) but a lower dielectric constant (≈20). The potential of these materials is demonstrated by integrating ultrathin Eu₂SO₂ nanoplates with molybdenum disulfide (MoS₂) field-effect transistors (FETs) via vdW forces. The resulting devices achieve a near-ideal Ion/Ioff ratio (≈10⁸), minimal hysteresis (≈5.3 mV), a low subthreshold slope (≈63.5 mV dec⁻¹), and ultralow leakage current (≈10⁻¹⁴ A). These results highlight the capacity of europium oxysulfur compounds to address the trade-off between dielectric constant and bandgap, offering tailored solutions for diverse 2D electronic applications. This work underscores the potential of composition engineering to expand the family of rare-earth oxysulfur compounds for nanoelectronics, paving the way for innovative gate dielectrics in next-generation devices.
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