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Electromodulation spectroscopy enables optical absorption characterization of interlayer excitons in two-dimensional heterostructures. 

Exciton polaron is a hypothetical many-body quasiparticle that involves an exciton dressed with a polarized electron-hole cloud in the Fermi sea. It has been evoked to explain the excitonic spectra of charged monolayer transition metal dichalcogenides, but the studies were limited to the ground state. Here we measure the reflection and photoluminescence of monolayer MoSe₂and WSe₂gating devices encapsulated by boron nitride. We observe gate-tunable exciton polarons associated with the 1 s–3 s exciton Rydberg states. The ground and excited exciton polarons exhibit comparable energy redshift (15~30 meV) from their respective bare excitons. The robust excited states contradict the trion picture because the trions are expected to dissociate in the excited states. When the Fermi sea expands, we observe increasingly severe suppression and steep energy shift from low to high exciton-polaron Rydberg states. Their gate-dependent energy shifts go beyond the trion description but match our exciton-polaron theory. Our experiment and theory demonstrate the exciton-polaron nature of both the ground and excited excitonic states in charged monolayer MoSe₂and WSe₂.

 

We report the direct observation of intervalley exciton between the Q conduction valley and Γ valence valley in bilayer WSe2 by photoluminescence. The QΓ exciton lies at ~18 meV below the QK exciton and dominates the luminescence of bilayer WSe2. By measuring the exciton spectra at gate-tunable electric field, we reveal different interlayer electric dipole moments and Stark shifts between QΓ and QK excitons. Notably, we can use the electric field to switch the energy order and dominant luminescence between QΓ and QK excitons. Both QΓ and QK excitons exhibit pronounced phonon replicas, in which two-phonon replicas outshine the one-phonon replicas due to the existence of (nearly) resonant exciton-phonon scatterings and numerous two-phonon scattering paths. We can simulate the replica spectra by comprehensive theoretical modeling and calculations. The good agreement between theory and experiment for the Stark shifts and phonon replicas strongly supports our assignment of QΓ and QK excitons. 

The electronic exciton polaron is a hypothetical many-body quasiparticle formed by an exciton dressed with a polarized electron-hole cloud in the Fermi sea (FS). It is predicted to display rich many-body physics and unusual roton-like dispersion. Exciton polarons were recently evoked to explain the excitonic spectra of doped monolayer transition metal dichalcogenides (TMDs), but these studies are limited to the ground state. Excited-state exciton polarons can exhibit richer many-body physics due to their larger spatial extent, but detection is challenging due to their inherently weak signals. Here we observe gate-tunable exciton polarons for the 1s - 3s excitonic Rydberg series in ultraclean monolayer MoSe2 devices by optical spectroscopy. When the FS expands, we observe increasingly severe suppression and steep energy shift from low to high Rydberg states. Their gate-dependent energy shifts go beyond the trion description but match our exciton-polaron theory. Notably, the exciton-polaron absorption and emission bands are separated with an energy gap, which increases from ground to excited state. Such peculiar characteristics are attributed to the roton-like exciton-polaron dispersion, where energy minima occur at finite momenta. The roton effect increases from ground to excited state. Such exciton-polaron Rydberg series with progressively significant many-body and roton effect shall provide a new platform to explore complex many-body phenomena.