Collective Polaritonic Effects on Chemical Dynamics Suppressed by Disorder

التفاصيل البيبلوغرافية
العنوان: Collective Polaritonic Effects on Chemical Dynamics Suppressed by Disorder
المؤلفون: Pérez-Sánchez, Juan B., Mellini, Federico, Giebink, Noel C., Yuen-Zhou, Joel
المصدر: Phys. Rev. Research 6, 013222, 2024
سنة النشر: 2023
المجموعة: Condensed Matter
Quantum Physics
مصطلحات موضوعية: Quantum Physics, Condensed Matter - Disordered Systems and Neural Networks
الوصف: We present a powerful formalism, disordered collective dynamics using truncated equations (d-CUT-E), to simulate the ultrafast quantum dynamics of molecular polaritons in the collective strong coupling regime, where a disordered ensemble of $N\gg10^{6}$ molecules couples to a cavity mode. Notably, we can capture this dynamics with a cavity hosting a single \textit{effective} molecule with $\sim N_{bins}$ electronic states, where $N_{bins}\ll N$ is the number of bins discretizing the disorder distribution. Using d-CUT-E we conclude that strong coupling, as evaluated from linear optical spectra, can be a poor proxy for polariton chemistry. For highly disordered ensembles, total reaction yield upon broadband excitation is identical to that outside of the cavity, while narrowband excitation produces distinct reaction yields solely due to differences in the initial states prepared prior to the reaction.
Comment: 16 pages, 12 figures
نوع الوثيقة: Working Paper
DOI: 10.1103/PhysRevResearch.6.013222
URL الوصول: http://arxiv.org/abs/2308.03954
رقم الانضمام: edsarx.2308.03954
قاعدة البيانات: arXiv
الوصف
DOI:10.1103/PhysRevResearch.6.013222