An official website of the United States government
Abstract Semiconductor excitations can hybridize with cavity photons to form exciton-polaritons (EPs) with remarkable properties, including light-like energy flow combined with matter-like interactions. To fully harness these properties, EPs must retain ballistic, coherent transport despite matter-mediated interactions with lattice phonons. Here we develop a nonlinear momentum-resolved optical approach that directly images EPs in real space on femtosecond scales in a range of polaritonic architectures. We focus our analysis on EP propagation in layered halide perovskite microcavities. We reveal that EP–phonon interactions lead to a large renormalization of EP velocities at high excitonic fractions at room temperature. Despite these strong EP–phonon interactions, ballistic transport is maintained for up to half-exciton EPs, in agreement with quantum simulations of dynamic disorder shielding through light-matter hybridization. Above 50% excitonic character, rapid decoherence leads to diffusive transport. Our work provides a general framework to precisely balance EP coherence, velocity, and nonlinear interactions.
more »
« less
This content will become publicly available on September 28, 2026
Static disorder-induced renormalization of polariton group velocity
Molecular exciton-polaritons exhibit long-range, ultrafast propagation, yet recent experiments have reported far slower propagation than expected. In this work, we implement a nonperturbative approach to quantify how static energetic disorder renormalizes polariton group velocity in strongly coupled microcavities. The method requires no exact diagonalization or master equation propagation and depends only on measurable parameters: the mean exciton energy and its probability distribution, the microcavity dispersion, and the Rabi splitting. Using parameters corresponding to recently probed organic microcavities, we show that exciton inhomogeneous broadening slows both lower and upper polaritons, particularly when the mean exciton energy fluctuation approaches the collective light–matter coupling strength. A detailed discussion and interpretation of these results is provided using perturbation theory in the limit of weak resonance scattering. The magnitude of the effects examined in this work supports the conclusion that most of the reported polaritonic slowdown arises from dynamical (phonon-assisted) disorder, with static energetic disorder contributing only secondarily.
more »
« less
- Award ID(s):
- 2340746
- PAR ID:
- 10650762
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 163
- Issue:
- 12
- ISSN:
- 0021-9606
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Exciton–polaritons have become an emerging platform for implementing non-Hermitian physics. The implementation commonly requires control of both the real and imaginary parts of the eigenmodes of the system. We present an experimental method to achieve this purpose using microcavities with sub-wavelength gratings as reflectors. The reflectivity and reflection phase of the grating can be changed by its geometric parameters, and they determine the energy and linewidth of the polariton modes. We demonstrate that this method allows a wide range of possible polariton energy and linewidth, suitable for implementing non-Hermitian polariton systems with coupled modes.more » « less
-
Abstract Exciton‐polaritons in organic microcavities are applied in devices including lasers, light‐emitting devices, and photodetectors, as well as in structures capable of tuning exciton kinetics and energy transfer. To enable a broader tailoring of polariton properties, it is important to develop means to better control molecular orientation and tune the intensity of the exciton–photon interaction. Vapor‐processed, glassy organic thin films are previously shown to have tunable molecular orientation as evidenced by phenomena including birefringence and transition dipole moment (TDM) alignment. Here, this tunability in TDM orientation with thin film processing conditions is exploited to continuously vary the interaction between the exciton and confined cavity photon mode. By embedding a thin film of 4,4′‐bis[(N‐carbazole)styryl]biphenyl (BSB‐Cz) in a metal‐reflector microcavity, ultrastrong coupling and hybridization of multiple electronic transitions of BSB‐Cz are demonstrated with a common cavity mode. Increasing the temperature during BSB‐Cz deposition tunes the TDM orientation from predominantly in‐plane to random to slightly vertical. This leads to a corresponding ≈30% variation in the associated Rabi splitting, consistent with theoretical predictions. This work demonstrates a means to continuously tune coupling strength from a materials perspective while also providing a handle to tune orientation disorder in thin film.more » « less
-
null (Ed.)Non-fullerene acceptors (NFAs) are highly promising materials for organic photovoltaics (OPVs). Exciton diffusion in NFAs is crucial to their photovoltaic performance, but is not yet well understood. Here we systematically examine exciton diffusion in a fused-ring electron acceptor (IDIC) based on a first-principles framework. We discover that low-energy excitons in disordered IDIC are charge-separated with electrons and holes residing on neighboring molecules, yielding long exciton lifetimes. With low energetic disorder, high exciton density of states (DOS) and long lifetimes, the disordered IDIC is predicted to exhibit large exciton diffusion lengths and high quantum efficiency. The temperature and energy dependences of exciton diffusion are explored and the manner in which various materials properties (exciton energy, DOS, energetic disorder, and phonon frequency) conspire to influence exciton diffusion is elucidated. Finally, we show that dilation could be an effective strategy to increase the exciton diffusion length in IDIC.more » « less
-
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
