Ultrafast imaging of polariton propagation and interactions
arXiv:2205.01176 · doi:10.1038/s41467-023-39550-x
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.
References in corpus (6)
- Strong light-matter coupling in two-dimensional atomic crystals
- Imaging exciton-polariton transport in MoSe2 waveguides
- Femtosecond photo-switching of interface polaritons in black phosphorus heterostructures
- Unveiling the mixed nature of polaritonic transport: From enhanced diffusion to ballistic motion approaching the speed of light
- Tuning the coherent propagation of organic exciton-polaritons through dark state delocalization
- Microscopic modelling of exciton-polariton diffusion coefficients in atomically thin semiconductors
Cited by in corpus (37)
- Roadmap for Photonics with 2D Materials
- Enhanced Excitation Energy Transfer under Strong Light-Matter Coupling: Insights from Multi-Scale Molecular Dynamics Simulations
- When do molecular polaritons behave like optical filters?
- Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factor
- Investigating the Collective Nature of Cavity Modified Chemical Kinetics under Vibrational Strong Coupling
- Non-Hermitian molecular dynamics simulations of exciton-polaritons in lossy cavities
- Collective Polaritonic Effects on Chemical Dynamics Suppressed by Disorder
- Extracting accurate light-matter couplings from disordered polaritons
- Theoretical Analysis of Exciton Wave Packet Dynamics in Polaritonic Wires
- Coherent transient exciton transport in disordered polaritonic wires
- Detecting, distinguishing, and spatiotemporally tracking photogenerated charge and heat at the nanoscale
- Polaritonic Quantum Matter
- Photochemical Initiation of Polariton Propagation
- Spatiotemporal imaging of nonlinear optics in van der Waals waveguides
- Nonlinear semiclassical spectroscopy of ultrafast molecular polariton dynamics
- Mean-field Mixed Quantum-Classical Approach for Many-Body Quantum Dynamics of Exciton-Polaritons
- Unraveling Abnormal Collective Effects via the Non-Monotonic Number Dependence of Electron Transfer in Confined Electromagnetic Fields
- Exciton Delocalization Suppresses Polariton Scattering
- Disentangling enhanced diffusion and ballistic motion of excitons coupled to Bloch surface waves with molecular dynamics simulations
- Two dimensional semiconductors: optical and electronic properties
- Dissecting Exciton-Polariton Transport in Organic Molecular Crystals: Emerging Conductivity Assisted by Intermolecular Vibrational Coupling
- Microscopic Theory of Polaron-Polariton Dispersion and Propagation
- Robust Surface-Induced Enhancement of Exciton Transport in Magic-Angle-Oriented Molecular Aggregates
- Resolving exciton and polariton multi-particle correlations in an optical microcavity in the strong coupling regime
- Tilted Material in an Optical Cavity: Light-Matter Moiré Effect and Coherent Frequency Conversion
- Directional Flow of Confined Polaritons in CrSBr
- Optically trapped exciton-polariton condensates in a perovskite microcavity
- Disorder-Induced Spectral Splitting versus Rabi Splitting under Strong Light-Matter Coupling
- Direct readout of excited state lifetimes in chlorin chromophores under electronic strong coupling
- Polariton transport in 2D semiconductors: Phonon-mediated transitions between ballistic, superdiffusive and exciton-limited regimes
- Discovery of energy landscapes towards optimized quantum transport: Environmental effects and long-range tunneling
- Mechanistic principles of exciton-polariton relaxation
- MQED-QD: An Open-Source Package for Quantum Dynamics Simulation in Complex Dielectric Environments
- Elucidating the Synergetic Interplay between Average Intermolecular Coupling and Coupling Disorder in Short-Time Exciton Transfer
- Molecular Electron Transfer in Optical Cavities: From Excitonic to Vibronic Polaritons
- Scalable Quantum Monte Carlo Method for Polariton Chemistry via Mixed Block Sparsity and Tensor Hypercontraction Method
- Beyond mean-field dynamics of the Dicke model with non-Markovian dephasing