Quadrupolar and Dipolar Excitons in Bilayer <math display=

Shun Feng; Aidan J. Campbell; Bibi Mary Francis; Hyeonjun Baek; Takashi Taniguchi; Kenji Watanabe; Iann C. Gerber; Brian D. Gerardot; Mauro Brotons-Gisbert

doi:10.1103/physrevlett.134.166901

Journal article Quadrupolar and Dipolar Excitons in Bilayer $2 H − {MoSe}_{2}$

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Shun Feng, Aidan J. Campbell, Bibi Mary Francis, Hyeonjun Baek, Takashi Taniguchi, Kenji Watanabe, Iann C. Gerber, Brian D. Gerardot, Mauro Brotons-Gisbert. Quadrupolar and Dipolar Excitons in Bilayer

2 H − {MoSe}_{2}

. Physical Review Letters. 2025, 134 (16), 166901. https://doi.org/10.1103/physrevlett.134.166901

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We report the experimental observation of quadrupolar exciton states in the reflectance contrast spectrum of 2H-stacked bilayer MoSe2. The application of a vertical electric field results in a quadratic energy redshift of these quadrupolar excitons, in contrast to the linear energy splitting observed in the coexisting dipolar excitons within the bilayer MoSe2. We perform helicity-resolved reflectance contrast measurements to investigate the spin and valley configurations of the quadrupolar exciton states as a function of applied vertical electric and magnetic fields. Comparing our results with a phenomenological coupled-oscillator model indicates that the electric- and magnetic-field dependence of the quadrupolar exciton states can be attributed to the intravalley and intervalley hybridization of spin-triplet interlayer excitons with opposite permanent dipole moments, mediated by interlayer hole tunneling. These results position naturally stacked MoSe2 bilayers as a promising platform to explore electric-field-tunable many-body exciton phenomena.

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