Mixed-dimensional van der Waals (vdW) heterostructures, integrated two-dimensional (2D) atomic crystals with three-dimensional (3D) functional materials, offer a powerful means to manipulating physical properties and generating unprecedented functionalities. Understanding interfacial couplings at those hetero (homo)-interfaces is indispensable for exploring new optical and electronic devices. Herein, we investigated dynamically phase-transition-driven strain coupling across a vdW heterointerface through integrating 2D layered 2H-MoS2 nanoflakes onto 3D phase-change VO2 epitaxial thin films. The Raman peak positions of the in-plane and out-of-plane vibration modes E2g1 and A1g from the 2H-MoS2 nanoflakes show a phonon softening and reversible hysteresis loop as a function of temperature in this mixed-dimensional vdW 2H-MoS2/(1¯11)-VO2/(11¯02)-Al2O3 heterostructure, originating from the co-action of temperature-dependent anharmonicity in 2H-MoS2 and reversible structural phase transition (SPT)-induced in-plane tensile strain from the VO2 thin film. Accordingly, the integrated Raman scattering intensity of these two feature peaks of the 2H-MoS2 nanoflakes increased (decreased) as the temperature increased (decreased), exhibiting a hysteresis loop in the SPT and metal–insulator transition region of VO2. Additionally, the peak integrated intensity enhancement ratio of the E2g1 and A1g vibration modes was approximately 2.3 and 2.8, respectively. These results indicate that the dynamically SPT-driven in-plane tensile strain from the bottom VO2 layer interfacially couples with the adjacent 2H-MoS2 nanoflakes and results in a reduction in the electronic transition energy, leading to an enhancement in the Raman scattering intensity of 2H-MoS2. Our work holds promise for dynamic strain control of lattice dynamics and electron–phonon interaction of 2D materials for functional electronic and photoelectronic devices.
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