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Using four-wave mixing microscopy, we measure the coherent response and ultrafast dynamics of excitons and trions in MoSe 2 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.

A time-resolved observation of coherent interlayer longitudinal acoustic phonons in thin layers of 2H-MoSe2 is reported. A femtosecond pump-probe technique is used to investigate the evolution of the energy loss of these vibrational modes in a wide selection of MoSe2 flakes with different thicknesses ranging from bilayer up to the bulk limit. By directly analysing the temporal decay of the modes, we can clearly distinguish an abrupt crossover related to the acoustic mean free path of the phonons in a layered system, and the constraints imposed on the acoustic decay channels when reducing the dimensionality. For thicker samples, the main acoustic attenuation mechanism is attributed to the scattering of the acoustic modes with thermal phonons. For samples thinner than ∼20 molecular layers, the predominant damping mechanism is ascribed to the effects of surface asperity. Losses intrinsic to the low dimensionality of single or few layer materials impose critical limitations for their use in optomechanical and optoelectronic devices.

Monolayer transition metal dichalcogenides, known for exhibiting strong excitonic resonances, constitute a very interesting and versatile platform for the investigation of light-matter interactions. In this work, we report on a strong coupling regime between excitons in monolayer WSe2 and photons confined in an open, voltage-tunable dielectric microcavity. The tunability of our system allows us to extend the exciton-polariton state over a wide energy range and, in particular, to bring the excitonic component of the lower polariton mode into resonance with other excitonic transitions in monolayer WSe2. We can retain up to 40% of initial circular polarization of the laser or loose it completely if polariton modes are brought into resonances with low energy excitonic modes.