Spontaneous Polarization Suppression of Exciton-Exciton Annihilation in 3R-Stacked MoS$_2$ Bilayers

Abstract

Rapid exciton-exciton annihilation (EEA) in two-dimensional semiconductors limits access to high-density excitonic regimes essential for efficient optoelectronic operation under strong excitation. Here, we show that EEA is suppressed by repulsive dipole-dipole interactions between interlayer excitons polarized by the spontaneous polarization intrinsic to rhombohedral (3R)-stacked MoS$_2$ bilayers. Using ultrafast pump-probe spectroscopy, we measure an EEA rate of $\gamma_{\rm EEA}=(5.03\pm0.99)\times10^{-3}$ cm$^2$ s$^{-1}$ in 3R bilayers, which is approximately 18.2-fold smaller than that in monolayers and 2.9-fold smaller than that in nonpolar 2H bilayers. Despite the higher exciton diffusivity recently reported for 3R relative to 2H bilayers, the reduced EEA rate in 3R indicates a rate-limited regime governed by the close-encounter annihilation probability rather than diffusion. A rate-limited annihilation model incorporating a dipole-dipole repulsive potential captures the observed ratio $\gamma_{{\rm EEA},3{\rm R}}/\gamma_{{\rm EEA},2{\rm H}}\approx0.35$ for an exciton-exciton encounter distance of $\sim$1.3 nm, consistent with the bilayer exciton Bohr radius. These results show that spontaneous polarization in 3R-stacked bilayers suppresses nonlinear excitonic losses and provides a route toward high-density excitonics.