Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses

The ultrafast formation of strongly bound excitons in two-dimensional semiconductors provides a rich platform for studying fundamental physics as well as developing novel optoelectronic technologies. While extensive research has explored the excitonic coherence, many-body interactions, and nonlinear optical properties, the potential to study these phenomena by directly controlling their coherent polarization dynamics has not been fully realized. In this work, we use a sub-10 fs pulse shaper to study how temporal control of coherent exciton polarization affects the generation of four-wave mixing in monolayer WSe2\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${\rm{WS}}{{\rm{e}}}_{2}$$\end{document} under ambient conditions. By tailoring multiphoton pathway interference, we tune the nonlinear response from destructive to constructive interference, resulting in a 2.6-fold enhancement over the four-wave mixing generated by a transform-limited pulse. This demonstrates a general method for nonlinear enhancement by shaping the pulse to counteract the temporal dispersion experienced during resonant light-matter interactions. Our method allows us to excite both 1s and 2s states, showcasing a selective control over the resonant state that produces nonlinearity. By comparing our results with theory, we find that exciton-exciton interactions dominate the nonlinear response, rather than Pauli blocking. This capability to manipulate exciton polarization dynamics in atomically thin crystals lays the groundwork for exploring a wide range of resonant phenomena in condensed matter systems and opens up new possibilities for precise optical control in advanced optoelectronic devices.