Intrinsically ultrastrong plasmon-exciton interactions in crystallized films of carbon nanotubes

Abstract

In cavity quantum electrodynamics, optical emitters that are strongly coupled to cavities give rise to polaritons with characteristics of both the emitters and the cavity excitations. We show that carbon nanotubes can be crystallized into chip-scale, two-dimensionally ordered films and that this new material enables intrinsically ultrastrong emitter-cavity interactions: rather than interacting with external cavities, nanotube excitons couple to the near-infrared plasmon resonances of the nanotubes themselves. Our polycrystalline nanotube films have a hexagonal crystal structure, ~25 nm domains, and a 1.74 nm lattice constant. With this extremely high nanotube density and nearly ideal plasmon-exciton spatial overlap, plasmon-exciton coupling strengths reach 0.5 eV, which is 75% of the bare exciton energy and a near record for room-temperature ultrastrong coupling. Crystallized nanotube films represent a milestone in nanomaterials assembly and provide a compelling foundation for high-ampacity conductors, low-power optical switches, and tunable optical antennas.

arXiv comment35 pages, including supplementary information

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• Groove-Assisted Global Spontaneous Alignment of Carbon Nanotubes in Vacuum Filtration
• Science and applications of wafer-scale crystalline carbon nanotube films prepared through controlled vacuum filtration
• Gauge freedom, quantum measurements, and time-dependent interactions in cavity and circuit QED
• Macroscopically Aligned Carbon Nanotubes as a Refractory Platform for Hyperbolic Thermal Emitters
• Self-Hybridized Polaritonic Emission from Layered Perovskites
• Global alignment of solution-based single-wall carbon nanotube films via machine-vision controlled filtration
• Multiple Tunable Hyperbolic Resonances in Broadband Infrared Carbon-Nanotube Metamaterials
• Strong-field-driven dynamics and high-harmonic generation in interacting 1D systems
• Collective Excitations and Optical Response of Ultrathin Carbon Nanotube Films
• Giant anisotropy and Casimir phenomena: the case of carbon nanotube metasurfaces
• Electrically Driven Hyperbolic Nanophotonic Resonators as High Speed, Spectrally Selective Thermal Radiators
• Controlled Exciton-Plasmon Coupling in a Mixture of Ultrathin Periodically Aligned Single-Wall Carbon Nanotube Arrays
• Confinement-Induced Nonlocality and Casimir Force in Transdimensional Systems
• Anisotropic Photon Emission Enhancement near Carbon Nanotube Metasurfaces
• Polaritonic Ultrastrong Coupling: Quantum Entanglement in Ground State
• Tunable Hyperbolic Metamaterials Based on Self-Assembled Carbon Nanotubes