Interplay between disorder, local relaxation, and collective behavior for an ensemble of emitters outside versus inside a cavity

Zeyu Zhou, Hsing Ta Chen, Joseph E. Subotnik, Abraham Nitzan

Research output: Contribution to journalArticlepeer-review

Abstract

The interplay between collective optical response and molecular static and dynamic disorder is studied using simple effective Hamiltonians for an ensemble of two-level emitters inside and outside a single-mode cavity. We model environmental disorder by randomly modulating the molecular transition frequencies and the coupling between the emitters and the electromagnetic field. We also consider the effects of intermolecular interactions and orientational disorder. We investigate how these effects lead to new features in the steady-state absorption (outside the cavity), transmission spectra (inside the cavity), and the yield of local molecular processes such as a unimolecular reaction. Outside the cavity, the collective behavior is manifested in the linewidth of the steady-state absorption, the emission spectrum, and the local chemical yield. Inside the cavity, however, the collective behavior primarily determines the Rabi splitting. The effects of intermolecular interactions under orientational disorder are also studied. For the most part, for all types of disorder, if we increase disorder, we find a reduction in the collective nature of the molecular response (smaller effective N) and therefore the Rabi splitting contraction occurs with orientational disorder. Moreover, we find that static disorder is more destructive to collective behavior than dynamic disorder.

Original languageEnglish
Article number023708
JournalPhysical Review A
Volume108
Issue number2
DOIs
StatePublished - Aug 2023

Funding

FundersFunder number
U.S. Department of Energy
National Science FoundationCHE1953701
Basic Energy SciencesDE-SC0019397
Office of Science

    Fingerprint

    Dive into the research topics of 'Interplay between disorder, local relaxation, and collective behavior for an ensemble of emitters outside versus inside a cavity'. Together they form a unique fingerprint.

    Cite this