arXiv subjects

Yi-Ting Chuang

Publications and source records attributed to Yi-Ting Chuang.

5 recordsLinked to original sources

arXiv2026

Polaron-Polariton Assisted Thermally Activated Superradiance

We predict an anomalous thermally activated superradiance in molecular aggregates within polaritonic environments. In contrast to free space, the collective emission is enhanced when either the exciton-phonon coupling or the temperature increases. This counterintuitive phenomenon is captured by a microscopic theory that combines macroscopic quantum electrodynamics with a modified polaron quantum master equation approach, revealing a nontrivial interplay among excitons, phonons, and polaritons.

physics.chem-ph↗

arXiv2024

Anomalous Giant Superradiance in Molecular Aggregates Coupled to Polaritons

In this study, we unveil an eccentric superradiance phenomenon in molecular aggregates coupled to surface plasmon polaritons. Through the quantization of electromagnetic fields in media, we demonstrate that superradiance can be significantly enhanced by polaritons and its behavior distinguishably surpasses the Dick's $N$ scaling law. To understand the mechanism of this anomalous phenomenon, we derive an analytical expression of the superradiance rate, which is general for molecular aggregates in arbitrary dispersive and absorbing media. Furthermore, we show the importance of intermolecular distance for this extraordinary superradiance.

physics.chem-ph↗

arXiv2023

Microscopic theory of exciton-polariton model involving multiple molecules: Macroscopic quantum electrodynamics formulation and essence of direct intermolecular interactions

Cavity quantum electrodynamics (CQED) and its extensions are widely used for the description of exciton-polariton systems. However, the exciton-polariton models based on CQED vary greatly within different contexts. One of the most significant discrepancies among these CQED models is whether one should include direct intermolecular interactions in the CQED Hamiltonian. To answer this question, in this article, we derive an effective dissipative CQED model including free-space dipole-dipole interactions (CQED-DDI) from a microscopic Hamiltonian based on macroscopic quantum electrodynamics. Dissipative CQED-DDI successfully captures the nature of vacuum fluctuations in dielectric media and separates it into the free-space effects and the dielectric-induced effects. The former include spontaneous emissions, dephasings and dipole-dipole interactions in free space; the latter include exciton-polariton interactions and photonic losses due to dielectric media. We apply dissipative CQED-DDI to investigate the exciton-polariton dynamics (the population dynamics of molecules above a plasmonic surface) and compare the results with those based on the methods proposed by several previous studies. We find that direct intermolecular interactions are a crucial element when employing CQED-like models to study exciton-polariton systems involving multiple molecules.

quant-ph↗

arXiv2023

Quantum dynamics of molecular ensembles coupled with quantum light: Counter-rotating interactions as an essential component

The rotating-wave approximation to light-matter interactions is widely used in the quantum electrodynamics Hamiltonian; however, its validity has long been a matter of debate. In this article, we explore the impact of the rotating-wave approximation on the quantum dynamics of multiple molecules in complex dielectric environments within the framework of macroscopic quantum electrodynamics. In general, we find that the energy shifts of the molecules and the inter-molecule dipole-dipole interaction obtained in the weak coupling regime are correct only when the counter-rotating interactions are considered. Moreover, under the rotating-wave approximation, the energy shifts of the ground-state molecules and a portion of the inter-molecule interaction are discarded. Notably, in the near-field zone (short inter-molecular distance), the reduction of inter-molecule interaction can reach up to 50 percent. We also conduct a case study on the population dynamics of a pair of identical molecules above a plasmonic surface. Through analytical and numerical analysis, it is revealed that the rotating-wave approximation can profoundly affect the dynamics of the molecules in both strong and weak coupling regimes, emphasizing the need for careful consideration when making the rotating-wave approximation in a multiple-molecule system coupled with quantum light.

quant-ph↗

arXiv2021

Simple but accurate estimation of light-matter coupling strength and optical loss for a molecular emitter coupled with photonic modes

Light-matter coupling strength and optical loss are two key physical quantities in cavity quantum electrodynamics (cQED), and their interplay determines whether light-matter hybrid states can be formed or not in chemical systems. In this study, by using macroscopic quantum electrodynamics (mQED) combined with a pseudomode approach, we present a simple but accurate method which allows us to quickly estimate the light-matter coupling strength and optical loss without free parameters. Moreover, for a molecular emitter coupled with photonic modes (including cavity modes and plasmon polartion modes), we analytically and numerically prove that the dynamics derived from the mQED-based wavefunction approach is mathematically equivalent to the dynamics governed by the cQED-based Lindblad master equation when the Purcell factor behaves like Lorentzians.

physics.chem-ph↗