Microcavity-Modified Emission from Rare-Earth Ion-Based Molecular Complexes

Abstract

Despite the remarkable optical properties of rare-earth ion materials, their applications as light sources and in quantum technologies are often hindered by their long lifetimes and weak emission.Leveraging the natural compatibility of rare-earth ion molecular complexes with photonic structures, here we modify their photoluminescence properties by coupling them to a flexible open Fabry-Pérot cavity. The full in situ tunability of the Fabry-Pérot cavity allows fine control over its cavity modes and the achievement of resonant coupling between the rare-earth ion emission and the cavity modes. This configuration allows us to achieve a maximum photoluminescence enhancement factor of 30 and accelerate the decay rate up to two orders of magnitude. Our pumppower dependent spectroscopic studies of the emitter-cavity system suggests that the cavitymodified emission is primarily caused by amplified spontaneous emission. These results suggest that integrating rare-earth ion molecular complexes with photonic structures could be a viable approach for the effective tuning of their optical properties. This natural compatibility, together with their versatile molecular structures and the resultant electronic states, renders rare-earth ion molecular complexes a potential alternative material platform for lighting and quantum applications.

2D Ionic Liquid‐Like State of Charged Rare‐Earth Clusters on a Metal Surface

“…[10,11] Such rare-earth coordination complexes are also uniquely advantageous in developing rational blueprints for the design and synthesis of new structures with improved functions for potential applications. [12,13] However, the role of counterions and the formation of rare-earth complex clusters have yet to be explored at the single complex level. Recently, it has been demonstrated that by efficient protection of the surrounding ligands, the rare-earth ions in the complexes together with counterions can remain charged even on a metallic surface.…”

Exploring Superradiance Effects of Molecular Emitters Coupled with Cavity Photons and Plasmon Polaritons: A Perspective from Macroscopic Quantum Electrodynamics

“…During the past few years, cavity (polariton) chemistry has become an active field due to its potential applications in the alteration of chemical kinetics, − the modification of electron transfer, − the realization of polariton-mediated intermolecular energy transfer, − and the enhancement of spontaneous emission rates. − In this research area, the collective effect of a group of molecules interacting with confined electromagnetic fields has received extensive attention because this effect is viewed as the origin of polariton formations. − Superradiance is a kind of collective effect and has been widely studied − since the pioneering work done by Dicke . Recently, several experimental studies pertinent to superradiance in cavities have been realized, and some of the results can be explained by the Tavis–Cummings (TC) model, , which provides an exact solution for N molecules coupled to a single photonic mode .…”

X-ray Spectroscopy of a Rare-Earth Molecular System Measured at the Single Atom Limit at Room Temperature

“…Here, we demonstrate that X-ray spectroscopy at atomic limits can be performed at room temperature. This work also provides a fundamental understanding of rare-earth ions coordinated with the molecules and will be useful for designing novel rare-earth molecular systems. , …”