Coherent imaging and dynamics of excitons in MoSe2 monolayers epitaxially grown on hexagonal boron nitride

Using four-wave mixing microscopy, we measure the coherent response and ultrafast dynamics of excitons and trions in MoSe2 monolayers grown by molecular beam epitaxy on thin films of hexagonal boron nitride. We assess inhomogeneous and homogeneous broadenings in the transition spectral lineshape. The impact of phonons on the homogeneous dephasing is inferred via the temperature dependence of the dephasing. Four-wave mixing mapping, combined with atomic force microscopy, reveals spatial correlations between exciton oscillator strength, inhomogeneous broadening and the sample morphology. The quality of the coherent optical response of epitaxially grown transition metal dichalcogenides now becomes comparable to the samples produced by mechanical exfoliation, enabling the coherent nonlinear spectroscopy of innovative materials, like magnetic layers or Janus semiconductors.

Automated summary

Using four-wave mixing microscopy, the coherent response and ultrafast dynamics of excitons and trions in MoSe2 monolayers grown by molecular beam epitaxy on thin films of hexagonal boron nitride are measured. The inhomogeneous and homogeneous broadenings in the transition spectral lineshape are evaluated. The impact of phonons on the homogeneous dephasing is inferred through the temperature dependence of the dephasing. Four-wave mixing mapping combined with atomic force microscopy reveals spatial correlations between exciton oscillator strength, inhomogeneous broadening, and the sample morphology. The quality of the coherent optical response of epitaxially grown transition metal dichalcogenides is now comparable to mechanically exfoliated samples, enabling the coherent nonlinear spectroscopy of innovative materials such as magnetic layers or Janus semiconductors.