The intrinsic in-plane isotropy of high-symmetry two-dimensional(2D)transition metal dichalcogenides(TMDs)limits their applicability in polarization-sensitive optoelectronic devices.Conventional strategies such as het...The intrinsic in-plane isotropy of high-symmetry two-dimensional(2D)transition metal dichalcogenides(TMDs)limits their applicability in polarization-sensitive optoelectronic devices.Conventional strategies such as heterointerface and strain engineering can break rotational symmetry and induce anisotropy,yet they suffer from lattice-matching constraints and limited strain tunability.Here,we present a dual-modulation approach that integrates bilayer WS_(2) with the anisotropic van der Waals crystal CrOCl and applies externally engineered holeinduced stress.The in-plane lattice anisotropy of CrOCl induces interfacial symmetry breaking in WS_(2),while hole geometry generates controllable stress gradients.This synergy yields a pronounced optical anisotropy,with excitonic linear polarization reaching up to 59%.Furthermore,external magnetic fields can effectively modulate exciton anisotropy,whereas the anisotropy remains stable across various temperatures.First-principles calculations reveal that interfacial charge redistribution,induced by lattice distortion,underlies the observed optical anisotropy.Our results demonstrate a multi-field tuning platform—mechanical,magnetic,and thermal—for tailoring anisotropic light-matter interactions in 2D semiconductors,advancing the development of next-generation directional optoelectronic and quantum devices.展开更多
基金support from the National Natural Science Foundation of China(No.52373311)the Innovation Program for Quantum Science and Technology(No.2021ZD0301605)+3 种基金support from the National Natural Science Foundation of China(Nos.92263202 and 12374020)the National Key Research and Development Program of China(No.2020YFA0711502)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB33000000)support from the Australian Research Council(Discovery Project,No.DP180102976).
文摘The intrinsic in-plane isotropy of high-symmetry two-dimensional(2D)transition metal dichalcogenides(TMDs)limits their applicability in polarization-sensitive optoelectronic devices.Conventional strategies such as heterointerface and strain engineering can break rotational symmetry and induce anisotropy,yet they suffer from lattice-matching constraints and limited strain tunability.Here,we present a dual-modulation approach that integrates bilayer WS_(2) with the anisotropic van der Waals crystal CrOCl and applies externally engineered holeinduced stress.The in-plane lattice anisotropy of CrOCl induces interfacial symmetry breaking in WS_(2),while hole geometry generates controllable stress gradients.This synergy yields a pronounced optical anisotropy,with excitonic linear polarization reaching up to 59%.Furthermore,external magnetic fields can effectively modulate exciton anisotropy,whereas the anisotropy remains stable across various temperatures.First-principles calculations reveal that interfacial charge redistribution,induced by lattice distortion,underlies the observed optical anisotropy.Our results demonstrate a multi-field tuning platform—mechanical,magnetic,and thermal—for tailoring anisotropic light-matter interactions in 2D semiconductors,advancing the development of next-generation directional optoelectronic and quantum devices.