Spatiotemporally Coupled Electron–Hole Dynamics in Two Dimensional Heterostructures

Coulomb interactions play a crucial role in low-dimensional semiconductor materials, e.g., 2D layered semiconductors, dictating their electronic and optical properties. However, fundamental questions remain as to whether and how Coulomb interactions affect the charge or energy flow in 2D heterostructures, which is essential for their light-electricity conversions. Herein, using ultrafast spectroscopy, we report real space coupled electron-hole dynamics in 2D heterostructures. We show in (WSe₂/)WS₂/MoTe₂ with a controlled energy gradient for the hole and a near flat band for electron transfer, the fate of the electron is controlled by the hole in coupled dynamics. The interfacial electron transfer from WS₂ to MoTe₂ follows the hole closely and can be facilitated or suppressed by dynamic Coulomb interaction. In parallel to the band alignment, this study reveals the critical role of Coulomb interactions on the fate of photogenerated charges in 2D heterostructures, providing experimental evidence for coupled electron-hole dynamics and a new knob for steering nanoscale charge or energy transfer process.