Tuning the electronic structure of 2D materials is a very powerful asset toward tailoring their properties to suit the demands of future applications in optoelectronics. Strain engineering is one of the most promising methods in this regard. We demonstrate that even very small out-of-plane axial compression readily modifies the electronic structure of monolayer MoS2. As we show through in situ resonant and nonresonant Raman spectroscopy and photoluminescence measurements combined with theoretical calculations, the transition from direct to indirect band gap semiconductor takes place at ∼0.5 GPa, and the transition to a semimetal occurs at stress smaller than 3 GPa.

§Department of Physical and Macromolecular Chemistry Faculty of Science Charles University Prague Hlavova 2030 Prague 2 128 43 Czech Republic

†J Heyrovsky Institute of Physical Chemistry of the AS CR v v i Dolejskova 2155 3 182 23 Prague 8 Czech Republic

‡Departamento de Química Física 1 Facultad de Ciencias Químicas Universidad Complutense de Madrid Madrid 28040 Spain

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