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Abstract Realizing nonlinear optical response in the low photon density limit in solid-state systems has been a long-standing challenge. Semiconductor microcavities in the strong coupling regime hosting exciton-polaritons have emerged as attractive candidates in this context. However, the weak interaction between these quasiparticles has been a hurdle in this quest. Dipolar excitons provide an attractive strategy to overcome this limitation but are often hindered by their weak oscillator strength. The interlayer dipolar excitons in naturally occurring homobilayer MoS 2 alleviates this issue owing to their formation via hybridization of interlayer charge transfer exciton with intralayer B exciton. Here we demonstrate the formation of dipolar exciton polaritons in bilayer MoS 2 resulting in unprecedented nonlinear interaction strengths. A ten-fold increase in nonlinearity is observed for the interlayer dipolar excitons compared to the conventional A excitons. These highly nonlinear dipolar polaritons will likely be a frontrunner in the quest for solid-state quantum nonlinear devices. 

Hybrid organic–inorganic semiconductors feature complex lattice dynamics due to the ionic character of the crystal and the softness arising from non-covalent bonds between molecular moieties and the inorganic network. Here we establish that such dynamic structural complexity in a prototypical two dimensional lead iodide perovskite gives rise to the coexistence of diverse excitonic resonances, each with a distinct degree of polaronic character. By means of high-resolution resonant impul- sive stimulated Raman spectroscopy, we identify vibrational wavepacket dynamics that evolve along different configurational coordinates for distinct excitons and photocarriers. Employing density functional theory calculations, we assign the observed coherent vibrational modes to various low-frequency (≲50 cm−1) optical phonons involving motion in the lead iodide layers. We thus conclude that different excitons induce specific lattice reorganizations, which are signatures of polaronic binding. This insight into the energetic/configurational landscape involving globally neutral primary photoexcitations may be relevant to a broader class of emerging hybrid semiconductor materials.