Phonon-enhanced strain sensitivity of quantum dots in two-dimensional semiconductors

Abstract

Two-dimensional semiconductors have attracted considerable interest for integration into emerging quantum photonic networks. Strain engineering of monolayer transition-metal dichalcogenides (ML-TMDs) enables the tuning of light-matter interactions and associated optoelectronic properties, and generates new functionalities, including the formation of quantum dots (QDs). Here, we combine spatially resolved micro-photoluminescence ($\hat{I}¼$-PL) spectroscopy from cryogenic (4$\text{-}$94 K) to room temperature with micro-Raman spectroscopy at room temperature to investigate the strain-dependent emission energies of thousands of individual QDs in ML-WS${}_2$ and ML-WSe${}_2$, integrated across multiple heterostructures and a piezoelectric device. Compared with delocalized excitons, QDs in both materials exhibit enhanced strain sensitivities of their emission energies $-$ approximately fourfold in WS${}_2$ and twofold in WSe${}_2$ $-$ leading to pronounced broadening of the ensemble emission linewidth. Temperature-dependent $\hat{I}¼$-PL spectroscopy combined with dynamic strain tuning experiments further reveal that the enhanced strain sensitivity of individual QDs originates from strengthened interactions with low-energy phonons induced by quantum confinement. Our results demonstrate a versatile strain-engineering approach with potential for spectral matching across solid-state, atomic, and hybrid quantum photonic networks, and provide new insights into phonon-QD interactions in two-dimensional semiconductors.

17 pages, 5 figures, methods, supporting information