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Lattice deformation via substrate‐driven mechanical straining of 2D materials can profoundly modulate their bandgap by altering the electronic band structure. However, such bandgap modulation is typically short‐lived and weak due to substrate slippage, which restores lattice symmetry and limits strain transfer. Here, it is shown that a non‐volatile thermomechanical strain induced during hot‐press synthesis results in giant modulation of the inherent bandgap in quasi‐2D tellurium nanoflakes (TeNFs). By leveraging the thermal expansion coefficient (TEC) mismatch and maintaining a pressure‐enforced non‐slip condition between TeNFs and the substrate, a non‐volatile and anisotropic compressive strain is attained with ε = −4.01% along zigzag lattice orientation and average biaxial strain of −3.46%. This results in a massive permanent bandgap modulation of 2.3 eV at a rate S (ΔEg) of up to 815 meV/% (TeNF/ITO), exceeding the highest reported values by 200%. Furthermore, TeNFs display long‐term strain retention and exhibit robust band‐to‐band blue photoemission featuring an intrinsic quantum efficiency of 80%. The results show that non‐volatile thermomechanical straining is an efficient substrate‐based bandgap modulation technique scalable to other 2D semiconductors and van der Waals materials for on‐demand nano‐optoelectronic properties. 

Abstract Chalcogenide-based nonvolatile phase change materials (PCMs) have a long history of usage, from bulk disk memory to all-optic neuromorphic computing circuits. Being able to perform uniform phase transitions over a subwavelength scale makes PCMs particularly suitable for photonic applications. For switching between nonvolatile states, the conventional chalcogenide phase change materials are brought to a melting temperature to break the covalent bonds. The cooling rate determines the final state. Reversible polymorphic layered materials provide an alternative atomic transition mechanism for low-energy electronic (small domain size) and photonic nonvolatile memories (which require a large effective tuning area). The small energy barrier of breaking van der Waals force facilitates low energy, fast-reset, and melting-free phase transitions, which reduces the chance of element segregation-associated device failure. The search for such material families starts with polymorphic In₂Se₃, which has two layered structures that are topologically similar and stable at room temperature. In this perspective, we first review the history of different memory schemes, compare the thermal dynamics of phase transitions in amorphous-crystalline and In₂Se₃, detail the device implementations for all-optical memory, and discuss the challenges and opportunities associated with polymorphic memory.