Tamm‐Plasmon Exciton‐Polaritons in Single‐Monolayered CsPbBr₃ Quantum Dots at Room Temperature

Abstract

Constructing polaritonic devices in monolithic, ultra‐compact photonic architectures with monolayer‐featured exciton‐emitters is decisive to exploit the coherent superposition between entangled photonic and excitonic eigenstates for potential realizations of optical nonlinearities, macroscopic condensations, and superfluidity. Here, a feasible strategy for exciton‐polariton formations is demonstrated by implementing a Tamm‐plasmon (TP) polaritonic device with the active material composed of single‐monolayered perovskite (CsPbBr3) quantum dots (QDs). The metallic character of the TP configuration is able to concentrate its resonance mode into a confined region beyond the diffraction limit, which highly overlaps, both spatially and spectrally, with the single‐monolayered CsPbBr3 QDs embedded inside. The mode volume of the device is hence reduced dramatically, leading to an enhanced light–matter coupling strength for the polaritonic emission at room temperature. In particular, it is found that the dispersion relation of the TP polaritonic device is tunable by detuning the excitonic and photonic eigenmodes and that the polariton–polariton interaction energy is strongly dependent on the polariton's spin state. The presented strategy is a determinant step toward the realization of strong light–matter coupling and polariton spintronics in the CsPbBr3 QDs with a single‐monolayered feature.

Control of Lateral Assembly and Vertical Stacking in Spin-Coated Lead Halide Perovskite Nanocrystal Films for Enhanced Photoluminescence Efficiency

“…The details of the model calculation are explained in the SI (section 2.6). Furthermore, recent studies of plasmonic and photonic structures ,, and their mutual couplings with CsPbBr 3 NCs − stress the importance of our findings, whereby LHP NC assemblies are manipulatable to induce novel interactions with the external medium, for exploring future technology and applications.…”

Strong Light–Matter Coupling in Lead Halide Perovskite Quantum Dot Solids

“…Exciton-polaritons arise as a result of the strong coupling between confined photons and bound electron–hole pairs, and are thus characterized by their hybrid light–matter nature. − This hybridization takes place within designed optical environments, such as optical cavities, in which the electromagnetic field intensity is magnified for specific photon energies selected to match those of the targeted electronic transitions. , The exploration of this interaction in the field of lead halide perovskite materials has given rise to polaritonic controlled optical absorption and emission in film-shaped, , microcrystalline, , nanosized , (namely, nanowires, nanoplatelets, , and nanocubes) and low-dimensional (such as Ruddlesden–Popper phases) perovskites, which has been put into practice to develop optical switches, lasers, ,, solar cells, light emitting diodes, sensors, and photodetectors with enhanced performance. Reciprocally, the integration of these emerging materials in the field of polariton physics has provided the opportunity to observe fundamental phenomena. − However, the observation of strong light–matter coupling in PQD solids has remained elusive, in spite of being some of the most appealing materials for both fundamental analysis and applications in optoelectronics. − Furthermore, this interaction has been scarcely investigated in QD solids in general, regardless of their composition, with only a few examples employing extremely thin CdSe and CdZnS/ZnS QD films. , The reason for this is 3-fold.…”

“… 2 − 4 This hybridization takes place within designed optical environments, such as optical cavities, in which the electromagnetic field intensity is magnified for specific photon energies selected to match those of the targeted electronic transitions. 5 , 6 The exploration of this interaction in the field of lead halide perovskite materials has given rise to polaritonic controlled optical absorption and emission in film-shaped, 7 , 8 microcrystalline, 9 , 10 nanosized 11 , 12 (namely, nanowires, 13 nanoplatelets, 14 , 15 and nanocubes 16 ) and low-dimensional (such as Ruddlesden–Popper phases 17 ) perovskites, which has been put into practice to develop optical switches, 18 lasers, 13 , 15 , 19 solar cells, 8 light emitting diodes, 10 sensors, 20 and photodetectors 21 with enhanced performance. Reciprocally, the integration of these emerging materials in the field of polariton physics has provided the opportunity to observe fundamental phenomena.…”

Observation of transition from superfluorescence to polariton condensation in CsPbBr3 quantum dots film

“…In fact, extensive research has been dedicated to investigating the interactions between perovskite single crystals and DBRs 13 – 16 over the years. There have also been concerted efforts to develop low-threshold lasers through the integration of quantum dots with DBRs 17 – 21 . However, here we focus on elucidating the formalism of a novel class of quasiparticles known as cooperative exciton-polaritons (CEPs), which emerge due to the strong coupling between cooperative excitons and optical modes.…”