Ultrafast Coulomb blockade in an atomic-scale quantum dot (2412.13718v1)

Abstract: Controlling electron dynamics at optical clock rates is a fundamental challenge in lightwave-driven nanoelectronics. Here, we demonstrate ultrafast charge-state manipulation of individual selenium vacancies in monolayer and bilayer tungsten diselenide (WSe$_2$) using picosecond terahertz (THz) source pulses, focused onto the picocavity of a scanning tunneling microscope (STM). Using THz pump--THz probe time-domain sampling of the defect charge population, we capture atomic-scale snapshots of the transient Coulomb blockade, a signature of charge transport via quantized defect states. We identify back tunneling of localized charges to the tip electrode as a key challenge for lightwave-driven STM when probing electronic states with charge-state lifetimes exceeding the pulse duration. However, we show that back tunneling can be mitigated by the Franck-Condon blockade, which limits accessible vibronic transitions and promotes unidirectional charge transport. Our rate equation model accurately reproduces the time-dependent tunneling process across the different coupling regimes. This work builds on recent progress in imaging coherent lattice and quasiparticle dynamics with lightwave-driven STM and opens new avenues for exploring ultrafast charge dynamics in low-dimensional materials, advancing the development of lightwave-driven nanoscale electronics.