Ultrafast Nanoimaging of Electronic Coherence of Monolayer WSe<sub>2</sub>
Wenjin Luo, Benjamin G. Whetten, Vasily Kravtsov, Ashutosh Kumar Singh, Yibo Yang, Di Huang, Xinbin Cheng, Tao Jiang, Alexey Belyanin, Markus B. Raschke
Abstract
Transition-metal dichalcogenides (TMDs) have demonstrated a wide range of novel photonic, optoelectronic, and correlated electron phenomena for more than a decade. However, the coherent dynamics of their excitons, including possibly long dephasing times and their sensitivity to spatial heterogeneities, are still poorly understood. Here we implement adiabatic plasmonic nanofocused four-wave mixing (FWM) to image the coherent electron dynamics in monolayer WSe 2 . We observe nanoscale heterogeneities at room temperature with dephasing ranging from T 2 ≲ 5 to T 2 ≳ 60 fs on length scales of 50–100 nm. We further observe a counterintuitive anticorrelation between FWM intensity and T 2, with the weakest FWM emission at locations of longest coherence. We interpret this behavior as a nonlocal nano-optical interplay between spatial coherence of the nonlinear polarization and disorder-induced scattering. The results highlight the challenges associated with heterogeneities in TMDs limiting their photophysical properties, yet also the potential of their novel nonlinear optical phenomena.