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Optics Express

Strong coupling in a microcavity containing β-carotene

Richard T. Grant, Rahul Jayaprakash, David M. Coles, Andrew J. Musser, Simone De Liberato, Ifor D. W. Samuel, Graham A. Turnbull, Jenny Clark, David George Lidzey

Published Jan 31, 2018• 13 citations
Publisher

Abstract

We have fabricated an open-cavity microcavity structure containing a thin film of the biologically-derived molecule β-carotene. We show that the β-carotene absorption can be described in terms of a series of Lorentzian functions that approximate the 0-0, 0-1, 0-2, 0-3 and 0-4 electronic and vibronic transitions. On placing this molecular material into a microcavity, we obtain anti-crossing between the cavity mode and the 0-1 vibronic transition, however other electronic and vibronic transitions remain in the intermediate or weak-coupling regime due to their lower oscillator strength and broader linewidth. We discuss the consequences of strong-coupling for the possible modification of photosynthetic processes, or a re-ordering of allowed and optically-forbidden states.

DOI
10.1364/oe.26.003320

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We have fabricated an open-cavity microcavity structure containing a thin film of the biologically-derived molecule β-carotene. We show that the β-carotene absorption can be described in terms of a series of Lorentzian functions that approximate the 0-0, 0-1, 0-2, 0-3 and 0-4 electronic and vibronic transitions. On placing this molecular material into a microcavity, we obtain anti-crossing between the cavity mode and the 0-1 vibronic transition, however other electronic and vibronic transitions remain in the intermediate or weak-coupling regime due to their lower oscillator strength and broader linewidth. We discuss the consequences of strong-coupling for the possible modification of photosynthetic processes, or a re-ordering of allowed and optically-forbidden states.
Summary form only given. The interaction between light and matter can be significantly altered by placing the material in an optical microcavity. Under appropriate conditions strong coupling may occur, a process in which the confined electromagnetic field of the microcavity dramatically modifies the optical transitions of the material, resulting in an anti-crossing (Rabi splitting) of the coupled modes of the microcavity. Recently strong coupling has been observed in organic materials including J-aggregates of cyanine dyes. They have the desired properties of large oscillator strength and narrow linewidth, and have shown large Rabi splitting at room temperature. We report here significant strong coupling in a new structure, a metal clad organic microcavity.
Optical cavity/molecule strong coupling offers attractive opportunities to modulate photochemical or photophysical processes. When atoms or molecules are placed in an optical cavity, they can coherently exchange photonic energy with optical cavity vacuum fields, entering the strong coupling interaction regime. Recent work suggests that the thermodynamic and kinetic properties of molecules can be significantly changed by strong coupling, resulting in the emergence of intriguing photochemical and photophysical phenomena. As more and more physico-chemical systems are studied under strong coupling conditions, optical cavities have also advanced in their sophistication, responsiveness, and (multi)functionality. In this review, we highlight some of these recent developments, particularly focusing on Fabry-Perot microcavities.
Molecular complexes are held together via a variety of bonds, but they all share the common feature that their individual entities are in contact. In this work, we introduce and demonstrate the concept of a \textit{molecular optical bond}, resulting from the far-field electromagnetic coupling of several molecules via a shared mode of an optical microcavity. We discuss a collective enhancement of the vacuum Rabi splitting and study super- and sub-radiant states that arise from the cavity-mediated coupling both in the resonant and dispersive regimes. Moreover, we demonstrate a two-photon transition that emerges between the ground and excited states of the new optical compound. Our experimental data are in excellent agreement with the predictions of the Tavis-Cummings Hamiltonian and open the door to the realization of hybrid light-matter materials.
Abstract Light–matter interaction leads to excitation of molecules, which, in turn, can exchange energy with a localized electromagnetic field. This can be used for engineering of the electronic and vibrational energy levels of the molecules. This study considers the conditions for the emergence of the strong light–matter coupling regime for organic dye molecules in a tunable Fabry–Perot microcavity formed by a convex mirror and a flat reflecting surface. The sample studied was made of hexagonal boron nitride (hBN), polyvinylpyrrolidone polymer (PVP, 55 kDa), and rhodamine 6G fluorophore (R6G). Strong light–matter coupling was obtained in a sample with a low concentration of PVP. Adjustment of the optical path length in the microcavity by varying the thickness of the hBN–R6G–PVP film made it possible to obtain a high density of modes in the cavity (several tens of (λ/n)3) and, hence, to study the weak and strong light–matter coupling regimes. The results offer the possibility of studying the basic mechanisms of resonant light–matter interaction at room temperature, as well as developing new practical applications of the strong coupling effect.
Optical microcavities and metallic nanostructures have been shown to significantly modulate the dynamics and spectroscopic response of molecular systems. We present a study of the nonlinear optics of a model consisting of NNN anharmonic multilevel systems (e.g., Morse oscillators) undergoing collective strong coupling with a resonant infrared microcavity. We find that, under experimentally accessible conditions, molecular systems in microcavities may have nonlinear phenomena significantly intensified due to the high quality of polariton resonances and the enhanced microcavity electromagnetic energy density relative to free space. Particularly large enhancement of multiphoton absorption happens when multipolariton states are resonant with bare molecule multiphoton transitions. In particular, our model predicts two-photon absorption cross-section enhancements by several orders of magnitude relative to free space when the Rabi splitting ${\mathrm{\ensuremath{\Omega}}}_{R}$ is approximately equal to the molecular anharmonic shift $2\mathrm{\ensuremath{\Delta}}$. Our results provide rough upper bounds to resonant nonlinear-response enhancement factors as relaxation to dark states is treated phenomenologically. Notably, ensembles of two-level systems undergoing strong coupling with a cavity (described by the Tavis-Cummings model) show no such optical nonlinearity enhancements, highlighting the rich phenomenology afforded by multilevel anharmonic systems. Similar conclusions are expected to hold for excitonic systems that share features with our model (e.g., molecular dyes with accessible ${S}_{0}\ensuremath{\rightarrow}{S}_{1}\ensuremath{\rightarrow}{S}_{2}$ transitions) and strongly interact with a UV-visible cavity.
We investigate the interaction between light and molecular systems modeled as quantum emitters coupled to a multitude of vibrational modes via a Holstein-type interaction. We follow a quantum Langevin equations approach that allows for analytical derivations of absorption and fluorescence profiles of molecules driven by classical fields or coupled to quantized optical modes. We retrieve analytical expressions for the modification of the radiative emission branching ratio in the Purcell regime and for the asymmetric cavity transmission associated with dissipative cross-talk between upper and lower polaritons in the strong coupling regime. We also characterize the Forster resonance energy transfer process between donor-acceptor molecules mediated by the vacuum or by a cavity mode.