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. 
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                            Asymmetric 3D Elastic–Plastic Strain‐Modulated Electron Energy Structure in Monolayer Graphene by Laser Shocking
                        
                    
    
            Abstract Graphene has a great potential to replace silicon in prospective semiconductor industries due to its outstanding electronic and transport properties; nonetheless, its lack of energy bandgap is a substantial limitation for practical applications. To date, straining graphene to break its lattice symmetry is perhaps the most efficient approach toward realizing bandgap tunability in graphene. However, due to the weak lattice deformation induced by uniaxial or in‐plane shear strain, most strained graphene studies have yielded bandgaps <1 eV. In this work, a modulated inhomogeneous local asymmetric elastic–plastic straining is reported that utilizes GPa‐level laser shocking at a high strain rate (dε/dt) ≈ 106–107s−1, with excellent formability, inducing tunable bandgaps in graphene of up to 2.1 eV, as determined by scanning tunneling spectroscopy. High‐resolution imaging and Raman spectroscopy reveal strain‐induced modifications to the atomic and electronic structure in graphene and first‐principles simulations predict the measured bandgap openings. Laser shock modulation of semimetallic graphene to a semiconducting material with controllable bandgap has the potential to benefit the electronic and optoelectronic industries. 
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                            - Award ID(s):
- 1810280
- PAR ID:
- 10461477
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 31
- Issue:
- 19
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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