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Uniaxial strain has been widely used as a powerful tool for investigating and controlling the properties of quantum materials. However, existing strain techniques have so far mostly been limited to use with bulk crystals. Although recent progress has been made in extending the application of strain to two-dimensional van der Waals (vdW) heterostructures, these techniques have been limited to optical characterization and extremely simple electrical device geometries. Here, we report a piezoelectric-based in situ uniaxial strain technique enabling simultaneous electrical transport and optical spectroscopy characterization of dual-gated vdW heterostructure devices. Critically, our technique remains compatible with vdW heterostructure devices of arbitrary complexity fabricated on conventional silicon/silicon dioxide wafer substrates. We demonstrate a large and continuously tunable strain of up to −0.15% at millikelvin temperatures, with larger strain values also likely achievable. We quantify the strain transmission from the silicon wafer to the vdW heterostructure, and further demonstrate the ability of strain to modify the electronic properties of twisted bilayer graphene. Our technique provides a highly versatile new method for exploring the effect of uniaxial strain on both the electrical and optical properties of vdW heterostructures and can be easily extended to include additional characterization techniques. 

Abstract The interplay between a multitude of electronic, spin, and lattice degrees of freedom underlies the complex phase diagrams of quantum materials. Layer stacking in van der Waals (vdW) heterostructures is responsible for exotic electronic and magnetic properties, which inspires stacking control of two-dimensional magnetism. Beyond the interplay between stacking order and interlayer magnetism, we discover a spin-shear coupling mechanism in which a subtle shear of the atomic layers can have a profound effect on the intralayer magnetic order in a family of vdW antiferromagnets. Using time-resolved X-ray diffraction and optical linear dichroism measurements, interlayer shear is identified as the primary structural degree of freedom that couples with magnetic order. The recovery times of both shear and magnetic order upon optical excitation diverge at the magnetic ordering temperature with the same critical exponent. The time-dependent Ginzburg-Landau theory shows that this concurrent critical slowing down arises from a linear coupling of the interlayer shear to the magnetic order, which is dictated by the broken mirror symmetry intrinsic to the monoclinic stacking. Our results highlight the importance of interlayer shear in ultrafast control of magnetic order via spin-mechanical coupling. 

ABSTRACT Magnetoelastic coupling in van der Waals (vdW) magnetic materials enables a unique interplay between the spin and lattice degrees of freedom. Characterizing the elastic responses with atomic and femtosecond resolution across the magnetic transition is essential for guiding the design of magnetically tunable actuators and strain‐mediated spintronic devices. Here, ultrafast X‐ray diffraction employed at a free‐electron laser reveals that the atomic displacements, wave vectors, and dispersion relations of acoustic phonon modes in a vdW antiferromagnet FePS₃are coupled with the magnetic order, by tracking both in‐plane and out‐of‐plane Bragg peaks upon optical excitation across the Néel temperature (T_N). One transverse mode shows that a quasi‐out‐of‐plane atomic displacement undergoes a significant directional change acrossT_N. Its quasi‐in‐plane wave vector is derived by comparing the measured sound velocity and the first‐principles calculations. The other transverse mode is an interlayer shear acoustic mode whose amplitude is strongly enhanced in the antiferromagnetic phase, exhibiting eight times stronger amplitude than the longitudinal acoustic mode belowT_N. The atomically resolved characterization of acoustic phonon dynamics that couple with magnetic ordering opens opportunities for harnessing unique magnetoelastic coupling in vdW magnets on ultrafast timescales.