Electronic localization and optical activity of strain-engineered transition-metal dichalcogenide nanobubbles

Abstract Strain-engineered transition-metal dichalcogenide nanobubbles are promising platforms for quantum emission, as revealed by recent experimental observations. In this work, we present an ab initio investigation of MoS 2 , WS 2 , MoSe 2 , and WSe 2 nanobubbles, linking their structural and electronic properties to predictions of their optical activity. Inflating forces yield tunable geometries with non-uniform, apex-concentrated strain, which is sensitive to material rigidity. Strain modifies band gaps and universally induces non-dispersive valence states, exhibiting composition-dependent wave-function character, as revealed by an in-depth analysis of band structures and orbital contributions. Crucially, transitions from these apex-localized valence states are predominantly dark. This characteristic is attributed to their localization at the Γ -point, inhibiting transitions to the lowest unoccupied states that reside at the K-valley. While revealing that the herein considered sub-10-nm nanobubbles fall short as single-photon emitters, our findings provide essential understanding of the structure-property relations in emerging quantum materials, providing robust design rules to optimize their characteristics for novel quantum applications.