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arXiv:1303.3720 · Europhysics Letters (EPL)

Polariton condensation with saturable molecules dressed by vibrational modes

Justyna A. Ćwik, Sahinur Reja, P. B. Littlewood, Jonathan Keeling

Published Feb 1, 2014• 75 citations
arXivHTMLPDF

Abstract

Polaritons, mixed light-matter quasiparticles, undergo a transition to a condensed, macroscopically coherent state at low temperatures or high densities. Recent experiments show that coupling light to organic molecules inside a microcavity allows condensation at room temperature. The molecules act as saturable absorbers with transitions dressed by molecular vibrational modes. Motivated by this, we calculate the phase diagram and spectrum of a modified Tavis-Cummings model, describing vibrationally dressed two-level systems, coupled to a cavity mode. Coupling to vibrational modes can induce re-entrance, i.e. a normal-condensed-normal sequence with decreasing temperature and can drive the transition first-order.

DOI
10.1209/0295-5075/105/47009

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Polaritons, mixed light-matter quasiparticles, undergo a transition to a condensed, macroscopically coherent state at low temperatures or high densities. Recent experiments show that coupling light to organic molecules inside a microcavity allows condensation at room temperature. The molecules act as saturable absorbers with transitions dressed by molecular vibrational modes. Motivated by this, we calculate the phase diagram and spectrum of a modified Tavis-Cummings model, describing vibrationally dressed two-level systems, coupled to a cavity mode. Coupling to vibrational modes can induce re-entrance, i.e. a normal-condensed-normal sequence with decreasing temperature and can drive the transition first-order.
The field of Polaritonic Chemistry studies molecules strongly coupled to the light field of optical cavities. The resulting modification of the potential energy landscape has been demonstrated to enable control over the chemical and physical properties of materials and molecular ensembles. This thesis extends the Tavis–Cummings model to describe molecules under strong light–matter coupling, incorporating static dipole moments and dipole self-energy contributions derived from the Pauli–Fierz Hamiltonian. These additional terms are shown to be essential for reproducing cavity-modified molecular dynamics and spectra. Simulations on the nuclear wavefunction propagation of MgH+ molecules demonstrate the impact of these terms, while an effective two-level system model accurately captures the behavior of large ensembles. Beyond single excitations, the thesis also explores the higher excitation manifolds of the Tavis-Cummings model, which reveals that allowing for more than a single excitation makes the reaction of the involved polaritons entropically more favorable. Open-system simulations highlight how the coherence of the system's initial state governs decay pathways and enables long-lived energy storage. Finally, a multilevel vibrational model coupled to a two-mode cavity is introduced, where a Raman scheme enables selective mixing of vibrational states. The simulation results show that continuous pumping can drive molecules into specific vibrational states while suppressing electronic excitation, both for single molecules and small ensembles. Together, these results provide new theoretical insights into the mechanisms by which optical cavities reshape molecular energy landscapes. The results suggest approaches for controlling photonic, electronic, and vibrational dynamics in strongly coupled systems, contributing to the theoretical foundation of polariton chemistry.
In this work, we study the exciton-polariton condensate phase transition in a microcavity matter-light system in which electron-hole Coulomb interaction and matter-light coupling effects are treated on an equal footing. In the framework of the unrestricted Hartree-Fock approximation applying the two-dimensional exciton-polariton model, we derive the self-consistent equations determining simultaneously the excitonic and the photonic condenstate order parameters. In the thermal-equilibrium limit, we find a condensed state of the exciton-polariton systems and phase diagrams are then constructed. At a given low temperature, the condensate by its nature shows a crossover from an excitonic to a polaritonic and finally photonic condensed state as the excitation density increases at large detuning. Without the detuning, the excitonic condensed state disappears whereas the polaritonic or photonic phases dominate. The crossover is also found by lowering the Coulomb interaction at a finite matter-light coupling. Lowering the Coulomb interaction or increasing the temperature, the excitonic Mott transition occurs, at which the exciton-polariton condensates dissociate to free electron-hole/photon. Depending on temperature and excitation density, the phase transition of the exciton-polariton condensates is also addressed in signatures of photoluminescence mapping to the photonic momentum distribution.
The quantum dynamics of vibrational polaritonic states arising from the interaction of a bistable molecule with the quantized mode of a Fabry-Perot microcavity is investigated using a generic asymmetric double-well potential as a simplified one-dimensional model of a reactive molecule. After discussing the role of the light-matter coupling strength in the emergence of avoided crossings between polaritonic states, we investigate the possibility of using these crossings to trigger a dynamical switching of these states from one potential well to the other. Two schemes are proposed to achieve this coherent state switching, either by preparing the molecule in an appropriate vibrational excited state before inserting it into the cavity, or by applying a short laser pulse inside the cavity to obtain a coherent superposition of polaritonic states. The respective influences of dipole moment amplitude and potential asymmetry on the coherent switching process are also discussed.
Strong coupling of organic molecules to the vacuum field of a nanoscale cavity can be used to modify their chemical and physical properties. We extend the Tavis-Cummings model for molecular ensembles and show that the often neglected interaction terms arising from the static dipole moment and the dipole self-energy are essential for a correct description of the light-matter interaction in polaritonic chemistry. On the basis of a full quantum description, we simulate the excited-state dynamics and spectroscopy of MgH+ molecules resonantly coupled to an optical cavity. We show that the inclusion of static dipole moments and the dipole self-energy is necessary to obtain a consistent model. We construct an efficient two-level system approach that reproduces the main features of the real molecular system and may be used to simulate larger molecular ensembles.
The recent progress in nanotechnology [1,2] and single-molecule spectroscopy [3-5] paves the way for cost-effective organic quantum optical technologies emergent with a promise to real-life devices operating at ambient conditions. In this letter, we harness πππ-conjugated segments of an organic ladder-type polymer strongly coupled to a microcavity forming correlated collective dressed states of light, so-called of exciton-polariton condensates. We explore an efficient way for all-optical ultra-fast control over the macroscopic condensate wavefunction via a single photon. Obeying Bose statistics, exciton-polaritons exhibit an extreme nonlinearity undergoing bosonic stimulation [6] which we have managed to trigger at the single-photon level. Relying on the nature of organic matter to sustain stable excitons dressed with high energy molecular vibrations we have developed a principle that allows for single-photon nonlinearity operation at ambient conditions opening the door for practical implementations like sub-picosecond switching, amplification and all-optical logic at the fundamental limit of single light quanta.
Bose-Einstein condensates of exciton-polaritons in inorganic semiconductor microcavities are known to possess strong interparticle interactions attributed to their excitonic component. The interactions play a crucial role in the nonlinear dynamics of such systems and can be witnessed as the high energy shift of polariton states. However, the localised nature of Frenkel excitons in strongly coupled organic microcavities precludes interparticle Coulomb exchange-interactions that affect nonlinear dynamics and change mechanisms of polariton energy shifts accordingly. We have scrutinized the origins of energy shifts in connection with nonlinear dynamics in Frenkel exciton-polariton condensates and examined the possible contributions: intracavity optical Kerr-effect, gain-induced frequency pulling, polariton interactions and effects related to saturation of optical transitions for "dark"- and "bright" molecules [1]. Unlike the conventional strongly coupled semiconductor microcavities, we have shown that nonlinear interactions within the condensate do not rely on polariton interactions but instead originated from Pauli-blocking principle forbidding double excitation of the same molecular states. We have developed a theoretical model explaining the omnipresent energy shift of the condensate wavefunction together with its spectral and polarization features at the BEC transition in a consistent way. The crucial role of intermolecular energy transfer and “dark” exciton reservoir has been demonstrated for the first time. We believe the principles explored in this work are relevant to other systems exhibiting strong coupling of Frenkel excitons with a cavity mode, regardless of a cavity type, whether one dealing with Fabry-Perot cavities or plasmonic nanocavities etc and; therefore, provide general insight on nonlinear phenomena in composite light-matter condensates. [1] T. Yagafarov, D. Sannikov, A. Zasedatelev, K. Georgiou, A. Baranikov, O. Kyriienko, I. Shelykh, L. Gai, Z. Shen, D. G. Lidzey, P. Lagoudakis, Mechanisms of blueshifts in organic polariton condensates, Commun Phys 3, 18 (2020). https://doi.org/10.1038/s42005-019-0278-6