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When do molecular polaritons behave like optical filters?

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arxiv 2408.05036 v2 pith:J4ZERUPP submitted 2024-08-09 physics.chem-ph physics.opticsquant-ph

classification physics.chem-phphysics.opticsquant-ph
keywords opticalmolecularcavitycouplingeffectspolaritonslaserlight-matter
verification ladder T0 review T1 audit T2 compute T3 formal

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This review outlines several linear optical effects featured by molecular polaritons arising in the collective strong light-matter coupling regime. Under weak laser irradiation and when the single-molecule light-matter coupling can be neglected (often in the limit when the number of molecules per photon mode is large), we show that the excited-state molecular dynamics under collective strong coupling can be exactly replicated without the cavity using a shaped (or ``filtered'') laser, whose field amplitude is enhanced by the cavity quality factor, shining on the bare molecules. As a consequence, the absorption within a cavity can be understood as the overlap between the polariton transmission and the bare molecular absorption, suggesting that polaritons act in part as optical filters. This framework demystifies and provides a straightforward explanation for a large class of experiments and theoretical models in molecular polaritonics, highlighting that the same effects can be achieved without the cavity with shaped laser pulses. With a few modifications, this simple conceptual picture can also be adapted to understand the incoherent nonlinear response of polaritonic systems. This review establishes a clear distinction between polaritonic phenomena that can be fully explained through classical linear optics and those that require a quantum electrodynamics approach. It also highlights the need to differentiate between effects that necessitate polaritons (i.e., hybrid light-matter states) and those that can occur in the weak coupling regime. We further discuss that certain quantum optical effects like fluorescence can be partially described as optical filtering, whereas some others like cavity-induced Raman scattering go beyond this. Further exploration in these areas is needed to uncover novel polaritonic phenomena beyond optical filtering.

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Cited by 5 Pith papers

Reviewed papers in the Pith corpus that reference this work. Sorted by Pith novelty score. Full citation record

  1. Quantization of Polaritons Confined in Dielectric Structures

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    A method to construct polariton quantum master equations from classical Maxwell-mode solutions, applied to design structures with boosted polariton interactions and nonlocal correlations.

  2. Light-Matter Entanglement in Real-Time Nuclear-Electronic Orbital Polariton Dynamics

    physics.chem-ph 2025-06 conditional novelty 6.0 of 10

    A new full-quantum RT-NEO method propagates a joint molecule-cavity density matrix, yielding an entanglement Rabi splitting roughly twice the dipole Rabi splitting for H2 under electronic strong coupling and HCN under...

  3. Mapping molecular polariton transport via pump-probe microscopy

    quant-ph 2025-04 unverdicted novelty 6.0 of 10

    A modeling framework for pump-probe microscopy in cavities shows molecular dephasing and dark excitons drive sub-group-velocity transport of polaritons, with velocity tied to excitonic weight.

  4. Selective Excitation of IR-Inactive Modes via Vibrational Polaritons: Insights from Atomistic Simulations

    physics.chem-ph 2025-01 conditional novelty 6.0 of 10

    Pumping the upper polariton of liquid methane can transiently excite the IR-inactive symmetric bending mode, and the effect is strongest when the polariton is two-thirds photonic in character.

  5. Hidden nonlinear optical susceptibilities in linear polaritonic spectra

    quant-ph 2024-11 conditional novelty 6.0 of 10

    Linear polaritonic spectra contain finite-size (1/N) vacuum-induced Raman sidebands, observable when the cavity decay rate is comparable to the single-molecule coupling.

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