Cavity Polaritons Research Articles

Excitation Ladder of Cavity Polaritons.

Multidimensional coherent spectroscopy directly unravels multiply excited states that overlap in a linear spectrum. We report multidimensional coherent optical photocurrent spectroscopy in a semiconductor polariton diode and explore the excitation ladder of cavity polaritons. We measure doubly and triply avoided crossings for pairs and triplets of exciton polaritons, demonstrating the strong coupling between light and dressed doublet and triplet semiconductor excitations. These results demonstrate that multiply excited excitonic states strongly coupled to a microcavity can be described as two coupled quantum-anharmonic ladders.

The Role of Long-Lived Excitons in the Dynamics of Strongly Coupled Molecular Polaritons

The concept of modifying molecular dynamics in strongly coupled exciton-polariton systems is an emerging topic in photonics due to its potential to produce customized chemical systems with tailored photophysical properties. However, before such systems can be realized, it is essential to address the open questions concerning the nature and strength of electronic interactions between exciton-polaritons and localized excited states in chemical system as well as the proper way to measure such interactions. Here, we use transient optical spectroscopy to investigate dynamical interactions between exciton-polaritons, singlet excitons, and triplet excitons in a molecular singlet fission system that is strongly coupled to an optical microcavity. We identify some of the major limitations to modify molecular dynamics in the strong coupling regime. Simultaneous excitation of cavity polaritons and 'reservoir' states, defined as dark polaritons and dark excitons (e.g. triplets) from coupled molecules and excitons from uncoupled molecules, always occurs. In addition, slow conversion from reservoir states to cavity polaritons results in minimal changes to the overall population dynamics. Furthermore, we demonstrate how in addition to the usual population dynamics, transient optical measurements on microcavities reveal information pertaining to modification of the exciton-polariton transition energies due to changes in the population of molecular excited states and the exciton-photon coupling conditions. As a consequence of weak interactions between reservoir states and cavity polaritons, judicious design considerations are required to achieve modified chemical dynamics, necessitating the use of molecular systems with long excited-state lifetimes or strong coupling approaches that require a small number of molecules.

Collective Rayleigh Scattering from Molecular Ensembles under Strong Coupling.

Rayleigh scattering is usually considered to be the elastic scattering of photons from subwavelength physical objects, such as small particles or molecules. Here, we present a quantitative spectroscopic study of the scattering properties of molecules embedded in an optical cavity under strong coupling conditions, where the collective interaction between the molecules and the cavity gives rise to composite light-matter excitations known as cavity polaritons. We show that the polaritonic states exhibit strong resonant Rayleigh scattering, which depends on both the coupling strength and detuning and reaching ∼25% efficiency. Since the polaritonic wave functions in such systems are delocalized, our observations correspond to the collective scattering of each photon from a large ensemble of molecules.

Polariton Transitions in Femtosecond Transient Absorption Studies of Ultrastrong Light-Molecule Coupling.

Strong light–matter coupling is emerging as a fascinating way to tune optical properties and modify the photophysics of molecular systems. In this work, we studied a molecular chromophore under strong coupling with the optical mode of a Fabry–Perot cavity resonant to the first electronic absorption band. Using femtosecond pump–probe spectroscopy, we investigated the transient response of the cavity-coupled molecules upon photoexcitation resonant to the upper and lower polaritons. We identified an excited state absorption from upper and lower polaritons to a state at the energy of the second cavity mode. Quantum mechanical calculations of the many-molecule energy structure of cavity polaritons suggest assignment of this state as a two-particle polaritonic state with optically allowed transitions from the upper and lower polaritons. We provide new physical insight into the role of two-particle polaritonic states in explaining transient signatures in hybrid light–matter coupling systems consistent with analogous many-body systems.

Ultrafast acoustic switching of an optically pumped cavity polariton system in the bistable regime

Nonequilibrium transitions are investigated in a plane exciton-polariton system with complex acousto-optical excitation: stationary resonant optical excitation of polaritons along the normal to the surface of the resonator and picosecond strain pulses causing reversible exciton energy perturbations. It is shown that acoustic pulses can be used for ultrafast switching of the optical response of a bistable polariton system. Switching is experimentally implemented in a high-Q GaAs microcavity.

All-optical control of exciton flow in a colloidal quantum well complex

Excitonics, an alternative to romising for processing information since semiconductor electronics is rapidly approaching the end of Moore’s law. Currently, the development of excitonic devices, where exciton flow is controlled, is mainly focused on electric-field modulation or exciton polaritons in high-Q cavities. Here, we show an all-optical strategy to manipulate the exciton flow in a binary colloidal quantum well complex through mediation of the Förster resonance energy transfer (FRET) by stimulated emission. In the spontaneous emission regime, FRET naturally occurs between a donor and an acceptor. In contrast, upon stronger excitation, the ultrafast consumption of excitons by stimulated emission effectively engineers the excitonic flow from the donors to the acceptors. Specifically, the acceptors’ stimulated emission significantly accelerates the exciton flow, while the donors’ stimulated emission almost stops this process. On this basis, a FRET-coupled rate equation model is derived to understand the controllable exciton flow using the density of the excited donors and the unexcited acceptors. The results will provide an effective all-optical route for realizing excitonic devices under room temperature operation.

Cooper pair polaritons in cold fermionic atoms within a cavity

We formulate a Bardeen-Cooper-Schriffer (BCS) theory of quasiparticles in a degenerate Fermi gas strongly coupled to photons in a optical cavity. The elementary photonic excitations of the system are cavity polaritons, which consist of a cavity photon and an excitation of an atom within the Fermi sea. The excitation of the atom out of the Fermi sea leaves behind a hole, which together results in a loosely bound Cooper pair, allowing for the system to be written by a BCS wavefunction. As the density of the excitations is increased, the excited atom and hole become more strongly bound, crossing over into the molecular regime. This thus realizes an alternative BCS to BEC crossover scenario, where the participating species are quasiparticle excitations in a Fermi sea consisting of excited atoms and holes.

Quantum Control of Ultrafast Internal Conversion Using Nanoconfined Virtual Photons.

The rational control of nonradiative relaxation remains an unfulfilled goal of synthetic chemistry. In this study, we show how strongly coupling an ensemble of molecules to the virtual photons of an electromagnetic cavity provides a rational handle over ultrafast, nonradiative dynamics. Specifically, we control the concentration of zinc tetraphenyl porphyrin molecules within nanoscale Fabry-Perot cavity structures to show a variable collective vacuum Rabi splitting between cavity polaritons coincides with systematic changes in internal conversion rates. We find these changes deviate from the predictions of so-called gap laws. We also show that simple theories of structural changes caused by polariton formation cannot explain discrepancies between our results and established theoretical predictions. In light of these deficiencies, we explore other ways to explain the dependence of the internal conversion rate on polariton parameters. Our results demonstrate cavity polariton formation controls the photophysics of light harvesting and photocatalytic molecular moieties and the gap remaining in our fundamental understanding of mechanisms enabling this control.

Strain-engineered room temperature cavity polariton in ZnO whispering gallery microcavity

Cavity polaritons, originating from the strong coupling effect between cavity modes and excitons, have been tremendously investigated because of their high potential in new or quantum optoelectronic devices. Among them, realization of their dynamic controllability is highly desirable for real applications. In this work, we present a dynamic modulation of cavity polaritons via strain-engineering in the ZnO whispering gallery microcavity. By using a home-made strain apparatus, a nearly uniaxial stress is precisely applied to ZnO microwires, thus inducing an internal strain along its c-axis. Dynamic tuning of cavity polariton modes is clearly characterized by angle-resolved microphotoluminescence spectroscopy. The coupled oscillator's model with fitting parameters of strain-dependent excitons' energies can well describe the modes' redshift. Moreover, we show that the modes' redshift can also be understood by the strain-induced refractive index increase, described by the Lorentz model, of which the underlying mechanism is also related to light-exciton strong coupling. Finally, the strain-engineered dynamic tuning of polariton lasing modes is demonstrated as well, and this actually provides convincing evidence for the polariton states surviving above the threshold. This work indicates that strain-engineered cavity polaritons would pave an alternative way for developing polariton-based integrated or flexible optoelectronic devices.

Exciton-Polariton Properties in Planar Microcavity of Millimeter-Sized Two-Dimensional Perovskite Sheet.

In this work, the self-organized two-dimensional (2D) perovskite crystal sheet was synthesized for exciton-polariton studies. The layered 2D perovskite sheets naturally form Fabry-Pérot (F-P) optical cavities and exhibit evident cavity polariton modes. In the region of F-P cavity polariton modes, an exciton-polariton is formed by the superposition of strongly coupled exciton and photon states and the decreased spacing between two adjacent oscillation modes can be well explained by the formation of exciton polarities. Rabi splitting energy (Ω) evaluated from the energy-wavevector (E-k) dispersion relation of exciton-polariton coupling was about 259 ± 10 meV. For edge emissions of the laminated structure, the thickness-dependent quantum well exerts great influence on the band-gap absorption and emission. This work studies exciton-polariton properties in layered 2D perovskite sheets, making it possible application for polariton devices in the strong light-matter interaction region.

Modulated phases of graphene quantum Hall polariton fluids

This work is placed in the context of solid-state systems in the regime of ultra-strong light-matter coupling. To date, the highest light-matter coupling strengths have been measured in experiments with polaritons in semiconductor systems under the conditions of the Integer Quantum Hall effect. Polaritons are excitations resulting from strong coupling of light with a dipole-carrying matter excitation. In Pellegrino et al. (2016), we studied the impact of electron-electron interaction on polaritons in cavities in the case of graphene under the conditions of the Integer Quantum Hall effect. By using a mean-field (Hartree-Fock) approach we have shown the possibility of formation of spatially modulated light-matter phases characterized by a wavelength that is dependent on the value of the applied static magnetic field and the concentration of carriers, which is tunable by varying the gate voltage.

Interrogating the Structure of Molecular Cavity Polaritons with Resonance Raman Scattering: An Experimentally Motivated Theoretical Description

The formation of exciton polaritons by strongly coupling molecular electronic transitions to spatially confined photons may change photochemical processes. However, the fundamental physical drivers of these proposed changes remain unclear. To understand the role of changes to molecular structure caused by polariton formation in these photochemical processes we develop an experimentally motivated theoretical description of resonance Raman scattering from exciton polaritons. By modeling the structural parameters of light absorption in zinc tetraphenyl porphyrin and exciton polaritons formed from this molecule in nano-structured Fabry-Perot cavities, we simulate resonance Raman scattering excitation spectra from exciton polaritons and assess how these spectra depend on the polariton characteristics. We find the detuning of the cavity mode energy from that of the molecular transition can affect the structure of the resulting polaritonic states, as inferred from our simulated spectra. We also find previously u...

Propagating Hybrid Tamm Exciton Polaritons in Organic Microcavity

Strong coupling between Tamm plasmons and organic cavity polaritons is observed at room temperature. Angle-resolved reflectometry experiments unambiguously indicate the anticrossing in the dispersion relations, which is characteristic of the strong coupling regime, and the Tamm plasmon–cavity polariton hybrid states can be energetically manipulated by tuning the Tamm plasmons. The experimental data are in good agreement with calculations based on the transfer matrix method. Emission from the lower energy Tamm plasmon–cavity polariton hybrid states is observed, and the propagation property of the hybrid Tamm plasmon polariton is also studied. The real-space imaging experiments reveal that the propagation distance is larger when the Tamm plasmon and cavity polariton are strongly coupled in comparison to both the exciton of the uncoupled organic neat film and the cavity polaritons. Moreover, the propagation length of the hybrid polaritons increases as the fraction of Tamm plasmon component in the hybrid states increases.

Strong exciton-photon coupling in organic microcavity electroluminescence devices with thiophene/phenylene co-oligomer derivatives

Organic electroluminescence (EL) devices with surface-emitting microcavity structure were fabricated using vapor-deposited films of thiophene/phenylene co-oligomer derivatives, aiming at polariton formation under electrical excitation. Owing to strong coupling between excitons and photons in the device, we demonstrated the formation of cavity polaritons with a large Rabi-splitting energy (2ħΩ = 250 meV). Furthermore, efficient relaxation into the bottom of lower polariton branch was confirmed from angle-resolved EL spectra. In excitation-density dependence, the luminance of microcavity EL devices showed a superlinear increase with an elevation of current density indicating a contribution of triplet excitons.

Exciton polaritons based on planar dielectric Si asymmetric nanogratings coupled with J-aggregated dyes film.

Optical cavity polaritons, originated from strong coupling between the excitons in materials and photons in the confined cavities field, have recently emerged as their applications in the high-speed lowpower polaritons devices, low-threshold lasing and so on. However, the traditional exciton polaritons based on metal plasmonic structures or Fabry-Perot cavities suffer from the disadvantages of large intrinsic losses or hard to integrate and nanofabricate. This greatly limits the applications of exciton poalritons. Thus, here we implement a compact low-loss dielectric photonic - organic nanostructure by placing a 2-nm-thick PVA doped with TDBC film on top of a planar Si asymmetric nanogratings to reveal the exciton polaritons modes. We find a distinct anti-crossing dispersion behavior appears with a 117.16 meV Rabi splitting when varying the period of Si nanogratings. Polaritons dispersion and mode anti-crossing behaviors are also observed when considering the independence of the height of Si, width of Si nanowire B, and distance between the two Si nanowires in one period. This work offers an opportunity to realize low-loss novel polaritons applications.

Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity

The condensation of half-light half-matter exciton polaritons in semiconductor optical cavities is a striking example of macroscopic quantum coherence in a solid-state platform. Quantum coherence is possible only when there are strong interactions between the exciton polaritons provided by their excitonic constituents. Rydberg excitons with high principal value exhibit strong dipole-dipole interactions in cold atoms. However, polaritons with the excitonic constituent that is an excited state, namely Rydberg exciton polaritons (REPs), have not yet been experimentally observed. Here, we observe the formation of REPs in a single crystal CsPbBr3 perovskite cavity without any external fields. These polaritons exhibit strong nonlinear behavior that leads to a coherent polariton condensate with a prominent blue shift. Furthermore, the REPs in CsPbBr3 are highly anisotropic and have a large extinction ratio, arising from the perovskite's orthorhombic crystal structure. Our observation not only sheds light on the importance of many-body physics in coherent polariton systems involving higher-order excited states, but also paves the way for exploring these coherent interactions for solid-state quantum optical information processing.

Nonlinear Polariton Fluids in a Flatband Reveal Discrete Gap Solitons.

Phase frustration in periodic lattices is responsible for the formation of dispersionless flatbands. The absence of any kinetic energy scale makes flatband physics critically sensitive to perturbations and interactions. We report on the experimental investigation of the nonlinear response of cavity polaritons in the gapped flatband of a one-dimensional Lieb lattice. We observe the formation of gap solitons with quantized size and abrupt edges, a signature of the frozen propagation of switching fronts. This type of gap soliton belongs to the class of truncated Bloch waves, and has only been observed in closed systems up to now. Here, the driven-dissipative character of the system gives rise to a complex multistability of the flatband nonlinear domains. These results open up an interesting perspective regarding more complex 2D lattices and the generation of correlated photon phases.

Manipulating optical nonlinearities of molecular polaritons by delocalization.

Optical nonlinearities are key resources in the contemporary photonics toolbox, relevant to quantum gate operations and all-optical switches. Chemical modification is often used to control the nonlinear response of materials at the microscopic level, but on-the-fly manipulation of such response is challenging. Tunability of optical nonlinearities in the mid-infrared (IR) is even less developed, hindering its applications in chemical sensing or IR photonic circuitry. Here, we report control of vibrational polariton coherent nonlinearities by manipulation of macroscopic parameters such as cavity longitudinal length or molecular concentration. Further two-dimensional IR investigations reveal that nonlinear dephasing provides the dominant source of the observed ultrafast polariton nonlinearities. The reported phenomena originate from the nonlinear macroscopic polarization stemming from strong coupling between microscopic molecular excitations and a macroscopic photonic cavity mode.

Observation of cavity polaritons in a metal-mirror Fabry-Pérot microcavity containing liquid-crystalline semiconductor based on perylene bisimide units.

We investigate the optical properties of a metal-mirror microcavity containing a liquid-crystalline (LC) perylene tetracarboxylic bisimide (PTCBI) derivative. Measurements of the transmission's incidence angle dependence show that the peaks are split in a complex way and shift as the angle changes. Further, measurements of the photoluminescence spectrum's emission angle dependence show that the peak also shifts with the angle, as in the transmission experiment. We also carry out a theoretical analysis; the theoretical and experimental results are in very good agreement, and we estimate the vacuum Rabi splitting energies to be about 212, 180, and 240 meV. In addition, the peak photoluminescence energy coincides with the lower polariton branch obtained by transmission experiment. Finally, in a time-resolved photoluminescence experiment, we observe a fast relaxation component that is not seen in the bare LC PTCBI film. We believe this is due to cavity effects increasing the spontaneous emission transition rate, indicating that the emissions are due to cavity polaritons.

Nonlocal collective ultrastrong interaction of plasmonic metamaterials and photons in a terahertz photonic crystal cavity.

Light-matter interaction in the strong coupling regime is of profound interest for fundamental quantum optics, information processing and the realization of ultrahigh-resolution sensors. Here, we report a new way to realize strong light-matter interaction, by coupling metamaterial plasmonic "quasi-particles" with photons in a photonic cavity, in the terahertz frequency range. The resultant cavity polaritons exhibit a splitting which can reach the ultra-strong coupling regime, even with the comparatively low density of quasi-particles, and inherit the high Q-factor of the cavity despite the relatively broad resonances of the Swiss-cross and split-ring-resonator metamaterials used. We also demonstrate nonlocal collective interaction of spatially separated metamaterial layers mediated by the cavity photons. By applying the quantum electrodynamic formalism to the density dependence of the polariton splitting, we can deduce the intrinsic transition dipole moment for single-quantum excitation of the metamaterial quasi-particles, which is orders of magnitude larger than those of natural atoms. These findings are of interest for the investigation of fundamental strong-coupling phenomena, but also for applications such as ultra-low-threshold terahertz polariton lasing, voltage-controlled modulators and frequency filters, and ultra-sensitive chemical and biological sensing.