Femtosecond-Nanometer Visualization of Exciton Dynamics in MoSe$_2$

TL;DR

This study employs femtosecond-resolved photoemission micrographs to visualize exciton dynamics in MoSe$_2$ with nanometer and femtosecond resolution, revealing layer-dependent lifetimes and exciton resonance tuning in real space and time.

Contribution

It introduces a novel imaging technique combining two-photon photoemission and tunable near-IR excitation to directly observe exciton behavior in 2D materials at nanometer and femtosecond scales.

Findings

Exciton lifetimes in multilayer MoSe$_2$ are ~24 times longer than in monolayers.

Tuning near-IR excitation reveals nm-scale variations in exciton resonances.

The method enables real-space, real-time tracking of exciton dynamics not possible with conventional microscopy.

Abstract

Femtosecond (fs)-resolved photoemission electron micrographs of single and few-layer MoSe$_2$ track exciton dynamics in this model 2D quantum material system with joint nanometer (nm)-fs resolution. We illustrate the latter using two-photon photoemission following 400 nm fs irradiation to probe and tunable near-IR excitation (770-840 nm) to populate the lowest accessible A-exciton states in MoSe$_2$. Through distinct imaging contrasts in single/few-layer regions, we spatio-temporally visualize exciton lifetimes in multilayers that are ~24 times longer than their monolayer analogs. We also find that tuning the near-IR excitation source allows us to track exciton resonances that vary on the nm scale. In effect, our approach allows us to track exciton resonances and dynamics in real-space and in real-time, which is not currently possible (or at least trivially implemented) using conventional all-optical, nano-optical, and all-electron-based microscopies.