Realizing Optoelectronic Devices from Crumpled Two-Dimensional Material Heterostructures

Due to their high in-plane stiffness and low flexural rigidity, two-dimensional (2D) materials are excellent candidates for engineering three-dimensional (3D) nanostructures using crumpling. An important new direction is to integrate 2D materials into crumpled heterostructures, which can have much more complex device geometries. Here, we demonstrate phototransistors from crumpled 2D heterostructures formed from graphene contacts to a monolayer transition-metal dichalcogenide (MoS₂, WSe₂) channel and quantify the membrane morphology and optoelectronic performance. First, we examined the morphology of folds in the heterostructure and constituent monolayers under uniaxial compression. The 2D membranes relieve the stress by delaminating from the substrate and creating nearly periodic folds whose spacing depends on the membrane type. The matched mechanical stiffness of the constituting layers allows the 2D heterostructure to maintain a conformal interface through large deformations. Next, we examined the optoelectronic performance of a biaxially crumpled graphene-WSe₂ phototransistor. Photoluminescence (PL) spectroscopy shows that the optical band gap of WSe₂ shifts by less than 2 meV between flat and 15% biaxial crumpling, corresponding to a change in strain of less than 0.05%. The photoresponsivity scaled as P^-0.38 and reached 20 A/W under an illumination power density of 4 μW/cm² at 20 V bias, a performance comparable to flat photosensors. Using photocurrent microscopy, we observe that the photoresponsivity increases by only 20% after crumpling. Both the PL and photoresponse confirm that crumpling and delamination prevent the buildup of compressive strain leading to highly deformed materials and devices with similar performance to their flat analogs. These results set a foundation for crumpled all-2D heterostructure devices and circuitry for flexible and stretchable electronic applications.