Unlocking Delocalization: How Much Coupling Strength can Overcome Energy Disorder in Molecular Polaritons?

Опубликована: Май 21, 2024

We investigated the criteria to ensure delocalization exists in molecular polaritons – quasiparticles formed from collective strong coupling of light and matter that have shown capabilities modify chemical reactions. Importantly, delocalization, i.e., possess delocalized wavefunctions, is one hallmarks which enables energy transport dynamics. Delocalization polariton systems has been long assumed be robust against disorder ubiquitous real systems. However, this study reveals destroys polaritons. In order mitigate impact disorder, a strength exceeding 3 times inhomogeneous linewidth necessary. When smaller, properties are significantly compromised both static picture dynamic point view. This observation indicates more stringent criterion for preserving unique characteristics compared conventionally adopted standard (collective strengths larger than photonic spectral linewidths). work sheds lights on previous works explain why onset modified dynamics criteria, also serves as an important consideration existing future studies involving high levels disorder.

Язык: Английский

Ultra-fast photochemistry in the strong light-matter coupling regime

Опубликована: Июнь 5, 2024

Strong coupling between molecules and confined light modes of optical cavities to form polaritons can alter photochemistry, but the origin this effect remains largely unknown. While theoretical models suggest a suppression photochemistry due formation new polaritonic potential energy surfaces, many these do not account for energetic disorder among molecules, which is unavoidable at ambient conditions. Here, we combine simulations experiments show that an ultra-fast photochemical reaction such thermal prevents modification surface radiative decay lossy cavity modes. We also excitation spectrum under strong product “bare” absorption molecule-cavity system, suggesting act as gateways channeling into molecule, then reacts “normally”. Our results therefore imply provides means tune action rather than change reaction.

Язык: Английский

Enhanced Energy Transfer in Cavity QED Based Phototransistors

The Journal of Physical Chemistry Letters, Год журнала: 2024, Номер 15(32), С. 8211 - 8217

Опубликована: Авг. 5, 2024

We leveraged strong light–matter coupling, a quantum process generating hybridized states, to prepare phototransistors using donor–acceptor pairs that transfer energy via Rabi oscillations. In prototype experiment, we used cyanine J-aggregate (TDBC; donor) and MoS2 monolayer (acceptor) in field effect transistor cavity study photoresponsivity. Energy migrates through the newly formed polaritonic ladder, with enhanced device efficiency when is resonant donors. A theoretical model based on time-dependent Schrödinger equation helped interpret results, states acting as funnel monolayer. These findings suggest novel applications of coupling materials.

Язык: Английский