0000000000330694
AUTHOR
Ville Tiainen
Optimizing geometry of low-Q all-metal Fabry-Pérot microcavity for fluorescence spectroscopy
Abstract Fluorescence spectroscopy is commonly employed to study the excited-state photophysics of organic molecules. Planar Fabry-Pérot microcavities play an essential role in such studies and a strategic cavity design is necessary to attain an enhanced light-matter interaction. In this work, we computationally study different geometries for a planar metallic Fabry-Pérot microcavity tuned for the absorption of Sulforhodamine 101, a typical dye for fluorescence spectroscopy. The cavity consists of a polymer layer enclosed between two silver mirrors, where the thicknesses of all the three layers are varied to optimize the cavity. Our transfer-matrix and finite-difference time-domain simulati…
Effect of molecular Stokes shift on polariton dynamics
When the enhanced electromagnetic field of a confined light mode interacts with photoactive molecules, the system can be driven into the regime of strong coupling, where new hybrid light-matter states, polaritons, are formed. Polaritons, manifested by the Rabi split in the dispersion, have shown potential for controlling the chemistry of the coupled molecules. Here, we show by angle-resolved steady-state experiments accompanied by multi-scale molecular dynamics simulations that the molecular Stokes shift plays a significant role in the relaxation of polaritons formed by organic molecules embedded in a polymer matrix within metallic Fabry-Pérot cavities. Our results suggest that in the case …
Numerical study on the limit of quasi-static approximation for plasmonic nanosphere
Plasmonic nanospheres are often employed as resonant substrates in many nanophotonic applications, like in enhanced spectroscopy, near-field microscopy, photovoltaics, and sensing. Accurate calculation and tuning of optical responses of such nanospheres are essential to achieve optimal performance. Mie theory is widely used to calculate optical properties of spherical particles. Although, an approximated version of Mie approach, the quasi-static approximation (QSA) can also be used to determine the very same properties of those spheres with a lot simpler formulations. In this work, we report our numerical study on the limit and accuracy of QSA with respect to the rigorous Mie approach. We c…
Modeling optical constants from the absorption of organic thin films using a modified Lorentz oscillator model
Optical constants of organic thin films can be evaluated using the Lorentz oscillator model (LOM) which fails to fit inhomogeneously broadened absorption of highly concentrated molecular films. In modified LOM (MLOM), the inhomogeneous broadening is implemented through a frequency-dependent adjustable broadening function. In this work, we evaluate the optical constants of rhodamine 6G doped poly-vinyl alcohol thin films with varying doping concentration (including also extensively high concentrations) using MLOM, which outperforms LOM by showing a better agreement with the experimental results. Our proposed method provides a way to accurately determine optical constants of isotropic organic…
Effect of molecular Stokes shift on polariton dynamics
When the enhanced electromagnetic field of a confined light mode interacts with photoactive molecules, the system can be driven into the regime of strong coupling, where new hybrid light–matter states, polaritons, are formed. Polaritons, manifested by the Rabi split in the dispersion, have shown potential for controlling the chemistry of the coupled molecules. Here, we show by angle-resolved steady-state experiments accompanied by multi-scale molecular dynamics simulations that the molecular Stokes shift plays a significant role in the relaxation of polaritons formed by organic molecules embedded in a polymer matrix within metallic Fabry–Pérot cavities. Our results suggest that in the case …