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InSe, a member of the layered materials family, is a superior electronic andoptical material which retains a direct bandgap feature from the bulk toatomically thin few-layers and high electronic mobility down to a single layerlimit. We, for the first time, exploit strain to drastically modify the bandgapof two-dimensional (2D) InSe nanoflakes. We demonstrated that we could decreasethe bandgap of a few-layer InSe flake by 160 meV through applying an in-planeuniaxial tensile strain to 1.06% and increase the bandgap by 79 meV throughapplying an in-plane uniaxial compressive strain to 0.62%, as evidenced byphotoluminescence (PL) spectroscopy. The large reversible bandgap change of ~239 meV arises from a large bandgap change rate (bandgap strain coefficient) offew-layer InSe in response to strain, ~ 154 meV/% for uniaxial tensile strainand ~ 140 meV/% for uniaxial compressive strain, representing the mostpronounced uniaxial strain-induced bandgap strain coefficient experimentallyreported in two-dimensional materials.We developed a theoretical understandingof the strain-induced bandgap change through first-principles DFT and GWcalculations. We also confirmed the bandgap change by photoconductivitymeasurements using excitation light with different photon energies. The highlytunable bandgap of InSe in the infrared regime should enable a wide range ofapplications, including electro-mechanical, piezoelectric and optoelectronicdevices.

Ultrasensitive Tunability of the Direct Bandgap of Two-dimensional InSe Flakes via Strain Engineering