skip to main content


Title: Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2
Abstract Strong optical nonlinearities play a central role in realizing quantum photonic technologies. Exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such interactions is generally not sufficient to reach the regime of quantum nonlinear optics. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities. Here we demonstrate the formation of exciton-polaritons using excited excitonic states in monolayer tungsten diselenide (WSe 2 ) embedded in a microcavity. The realized excited-state polaritons exhibit an enhanced nonlinear response ∼ $${g}_{{pol}-{pol}}^{2s} \sim 46.4\pm 13.9\,\mu {eV}\mu {m}^{2}$$ g p o l − p o l 2 s ~ 46.4 ± 13.9 μ e V μ m 2 which is ∼4.6 times that for the ground-state exciton. The demonstration of enhanced nonlinear response from excited exciton-polaritons presents the potential of generating strong exciton-polariton interactions, a necessary building block for solid-state quantum photonic technologies.  more » « less
Award ID(s):
2116679 1708457
PAR ID:
10334119
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ;
Date Published:
Journal Name:
Nature Communications
Volume:
12
Issue:
1
ISSN:
2041-1723
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. The condensation of half-light half-matter exciton polaritons in semiconductor optical cavities is a striking example of macroscopic quantum coherence in a solid-state platform. Quantum coherence is possible only when there are strong interactions between the exciton polaritons provided by their excitonic constituents. Rydberg excitons with high principal value exhibit strong dipole–dipole interactions in cold atoms. However, polaritons with the excitonic constituent that is an excited state, namely Rydberg exciton polaritons (REPs), have not yet been experimentally observed. Here, we observe the formation of REPs in a single crystal CsPbBr 3 perovskite cavity without any external fields. These polaritons exhibit strong nonlinear behavior that leads to a coherent polariton condensate with a prominent blue shift. Furthermore, the REPs in CsPbBr 3 are highly anisotropic and have a large extinction ratio, arising from the perovskite’s orthorhombic crystal structure. Our observation not only sheds light on the importance of many-body physics in coherent polariton systems involving higher-order excited states, but also paves the way for exploring these coherent interactions for solid-state quantum optical information processing. 
    more » « less
  2. It remains unclear how the collective strong coupling of cavity-confined photons to the electronic transitions of molecular chromophore leverages the distinct properties of the polaritonic constituents for future technologies. In this study, we design, fabricate, and characterize multiple types of Fabry-Pérot (FP) mirco-resonators containing copper(II) tetraphenyl porphyrin (CuTPP) to show how cavity polariton formation affects radiative relaxation processes in the presence of substantial non-Condon vibronic coupling between two of this molecule’s excited electronic states. Unlike the prototypical enhancement of Q state radiative relaxation of CuTPP in a FP resonator incapable of forming polaritons, we find the light emission processes in multimode cavity polariton samples become enhanced for cavity-exciton energy differences near those of vibrations known to mediate non-Condon vibronic coupling. We propose the value of this detuning is consistent with radiative relaxation of Herzberg-Teller polaritons into collective molecular states coupled to the cavity photon coherently. We contrast the feature stemming from light emission from the HT polariton state with those that occur due to polariton-enhanced light absorption. Our results demonstrate the landscape of molecular and photonic interactions enabled by cavity polariton formation using complex chromophores and how researchers can design resonators to leverage these interactions to characterize and control polaritonic properties.

     
    more » « less
  3. 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. 
    more » « less
  4. Topological insulators are a class of electronic materials exhibiting robust edge states immune to perturbations and disorder. This concept has been successfully adapted in photonics, where topologically nontrivial waveguides and topological lasers were developed. However, the exploration of topological properties in a given photonic system is limited to a fabricated sample, without the flexibility to reconfigure the structurein situ. Here, we demonstrate an all-optical realization of the orbital Su–Schrieffer–Heeger model in a microcavity exciton-polariton system, whereby a cavity photon is hybridized with an exciton in a GaAs quantum well. We induce a zigzag potential for exciton polaritons all-optically by shaping the nonresonant laser excitation, and measure directly the eigenspectrum and topological edge states of a polariton lattice in a nonlinear regime of bosonic condensation. Furthermore, taking advantage of the tunability of the optically induced lattice, we modify the intersite tunneling to realize a topological phase transition to a trivial state. Our results open the way to study topological phase transitions on-demand in fully reconfigurable hybrid photonic systems that do not require sophisticated sample engineering.

     
    more » « less
  5. Abstract

    Room temperature stable excitons in layered two‐dimensional (2D) transition metal dichalcogenides (TMDs) offer a unique route for engineering light and matter interactions. Due to the strong optical dispersion near the excitonic transitions, a high refractive index arises in these ultrathin semiconductors.[1,2]Utilizing this behavior, strongly confined Fano type optical resonances in an ultrathin (i.e., ≈12 nm) tungsten disulfide (WS2) photonic crystal (PhC) directly fabricated on a TMD‐on‐glass platform are reported. In this approach, Fano‐type WS2photonic resonances strongly couple to the WS2excitonic dispersion engender self‐resonant exciton‐polaritons with an out‐of‐plane optical confinement exceeding that provided by surface plasmon polaritons in the visible. The large spatial light‐matter overlap endowed by this unique monolithic self‐coupling scheme is utilized for steering of enhanced 2D WSe2excitonic photoluminescence in a truly TMD integrated system. It is envisioned that the strong light matter interaction on the TMD‐on‐glass platform will unfold the prospects of ultrathin exciton‐polaritonic resonators.

     
    more » « less