极化子双量子相干的普遍尺度与多体复活
Universal Scaling and Many-Body Resurrection of Polaritonic Double-Quantum Coherences
AI总结：
研究通过非微扰Maxwell-Liouville框架揭示强光物质耦合下多体相互作用如何复活极化子双量子相干，提出通用双光子匹配规则保护宏观相干性。
摘要：
分子集体腔局域化驱动宏观非线性信号向严重谐波抵消（称为“频谱饥饿”）发展，但内在多体分子相互作用稳健地复活真实极化子双量子相干（DQCs）。这种多体复活由通用双光子匹配规则Δ_B + 4J = Ω_R控制，连接分子非谐性（Δ_B）到宏观Rabi分裂（Ω_R）和激子耦合（J）。关键在于利用宏观极化子与局域双激子对的空间不匹配打破谐波抵消。对于J-聚集体（J < 0），此条件独特地隔离共振多体态在密集局域暗态之下，保护宏观相干免受空间碎裂。该预测框架建立直接相图以在不同强耦合平台中设计和保护光学非线性性。
英文摘要：
The ultrafast nonlinear optical response of molecular ensembles is fundamentally altered under strong light-matter coupling. To rigorously isolate the genuine many-body contributions, an exact time-domain field-subtraction protocol is developed within a fully non-perturbative Maxwell-Liouville framework explicitly incorporating the two-exciton manifold in real space and time. This approach reveals that while collective cavity delocalization drives the macroscopic nonlinear signal toward a severe harmonic cancellation (an effect termed "spectral starvation"), intrinsic many-body molecular interactions robustly resurrect genuine polaritonic double-quantum coherences (DQCs). This many-body resurrection is governed by a universal two-photon matching rule, $Δ_B + 4J = Ω_R$, linking molecular anharmonicity ($Δ_B$) to the macroscopic Rabi splitting ($Ω_R$) and excitonic coupling ($J$). Crucially, this resonance exploits the spatial mismatch between macroscopic polaritons and localized two-exciton pairs to break harmonic cancellation. For J-aggregates ($J < 0$), this condition uniquely isolates the resonant many-body state below the dense manifold of localized dark states, protecting the macroscopic coherence from spatial fragmentation. This predictive framework establishes a direct phase diagram to engineer and protect optical nonlinearities across diverse strongly coupled platforms.
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