Long-lived polaritonic coherence and polaron decoupling effects

• 成果类型: Article
• 署名作者: Mondal, M. Elious; Park, Seongje; Son, Minjung; Vamivakas, A. Nickolas; Cundif, Steven T.; Krauss, Todd D.; Huo, Pengfei
• 署名单位: University of Rochester; Boston University; Boston University; University of Rochester; University of Rochester; University of Rochester; University of Michigan System; University of Michigan
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-8424; 1091-6490
• DOI: 10.1073/pnas.2530454123
• 发表日期: 2026-04-21
• 页码: e2530454123
• 关键词: exciton polariton; 2D electronic spectroscopy; coherence enhancement; polaron decoupling; DYNAMICS

摘要

Molecular polaritons, formed by coupling molecular excitons with cavity photons, offer a promising platform for exploring quantum phenomena. A key challenge is understanding how these hybrid states maintain coherence in the presence of environmental vibrations. Here, we show theoretically that collective coupling of many molecular excitons in a cavity can protect polariton coherence from phonon-induced decoherence. Under realistic conditions, the coherence time can extend up to 200 fs at room temperature, compared with 15 fs for typical molecular systems. Simulations of two-dimensional electronic spectra reveal prolonged oscillations between upper and lower polariton states, and reduced vibrational coupling as indicated by changes in the nodal line slope of the lower polariton peak. These findings provide guidance for experimental efforts to realize long-lived polaritons, such as coupling CdSe nanoplatelets to optical cavities.