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Strong coupling in light-matter interaction with THz metamaterials and microcavity

초록/요약

We demonstrated a phonon-polariton in the terahertz (THz) frequency range, generated in a crystallized lead halide perovskite film coated on metamaterials. When the metamaterial resonance was in tune with the phonon resonance of the perovskite film, Rabi splitting occurred due to the strong coupling between the resonances. The Rabi splitting energy was about 1.1 meV, which is larger than the metamaterial and phonon resonance line widths; the interaction potential estimation confirmed that the strong coupling regime was reached successfully. We were able to tune the polaritonic branches by varying the metamaterial resonance, thereby obtaining the dispersion curve with a clear anticrossing behavior. Additionally, we performed in situ THz spectroscopy as we annealed the perovskite film and studied the Rabi splitting as a function of the films’ crystallization coverage. The Rabi splitting versus crystallization volume fraction exhibited a unique power-law scaling, depending on the crystal growth dimensions. We generated and controlled quantum states in perovskite phonon polaritons within a flexible Fabry–Perot cavity. Flexible perovskites were fabricated on a microporous substrate coated with graphene oxide, which enabled us to incorporate them within microcavities. Rabi splitting was observed when the cavity resonance coincided with the phonon resonance. A Rabi splitting energy of 1.9 meV was obtained for 1.67 μm film thickness, which is 2.4 times greater than the criterion for strong coupling. For various perovskite film thicknesses, we obtained dispersion curves exhibiting two polaritonic branches by varying the cavity length. A clear quantum beat was observed in the time domain between the two polaritonic branches, which resulted from the large Rabi splitting of the thick perovskite film. The manipulation of quantum devices can be enhanced by using flexible cavity devices with perovskite phonons, which provide an additional degree of freedom in manipulating quantum energy states at the macroscopic level. In this thesis, we investigate the phonon polariton in lead halide perovskites as an optoelectronic component and as a quantum state manipulator. Further exploration of perovskite-based devices with tunable properties and flexible properties opens the door to the development of advanced quantum devices with tunable energy states.

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목차

I. Introduction 1
1. Strong coupling in light-matter interaction 1
2. Organization of the thesis 9
3. Reference 12
II. Background 14
1. THz time-domain spectroscopy and imaging technology 14
2. Lead halide perovskite (MAPbI3) 19
3. Metamaterials 24
4. Fabry-Perot cavity 39
5. References 44
III. Phonon-Polaritons in Lead Halide Perovskite Film Hybridized with THz Metamaterials 62
1. Introduction 62
2. Observation of Phonon polariton using THz metamaterials 64
3. Dispersion curve 69
4. Calculation of strong coupling 74
5. In situ phonon-polariton formation 77
6. Methods 83
7. Conclusion 84
8. References 86
IV. Mechanical control of quantum states in lead halide perovskite phonons strongly coupled in THz microcavity 95
1. Introduction 95
2. Observation of Phonon polariton using THz Fabry-Perot Cavity 97
3. Dispersion curve 104
4. Calculation of strong coupling 108
5. Flexible phonon-polariton device 112
6. Methods 117
7. Conclusion 118
8. References 119
V. Conclusion 203

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