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Selective control of reconfigurable chiral plasmonic metamolecules

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 Added by Na Liu
 Publication date 2021
  fields Physics
and research's language is English




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Selective configuration control of plasmonic nanostructures using either top-down or bottom-up approaches has remained challenging in the field of active plasmonics. We demonstrate the realization of DNA-assembled reconfigurable plasmonic metamolecules, which can respond to a wide range of pH changes in a programmable manner. This programmability allows for selective reconfiguration of different plasmonic metamolecule species coexisting in solution through simple pH tuning. This approach enables discrimination of chiral plasmonic quasi-enantiomers and arbitrary tuning of chiroptical effects with unprecedented degrees of freedom. Our work outlines a new blueprint for implementation of advanced active plasmonic systems, in which individual structural species can be programmed to perform multiple tasks and functions in response to independent external stimuli.



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Molecular chirality is a geometric property that is of great importance in chemistry, biology, and medicine. Recently, plasmonic nanostructures that exhibit distinct chiroptical responses have attracted tremendous interest, given their ability to emulate the properties of chiral molecules with tailored and pronounced optical characteristics. However, the optical chirality of such human-made structures is in general static and cannot be manipulated postfabrication. Herein, different concepts to reconfigure the chiroptical responses of plasmonic nano- and micro-objects are outlined. Depending on the utilized strategies and stimuli, the chiroptical signature, the 3D structural conformation, or both can be reconfigured. Optical devices based on plasmonic nanostructures with reconfigurable chirality possess great potential in practical applications, ranging from polarization conversion elements to enantioselective analysis, chiral sensing, and catalysis.
Motivated by the recent growing demand in dynamically-controlled flat optics, we take advantage of a hybrid phase-change plasmonic metasurface (MS) to effectively tailor the amplitude, phase, and polarization responses of the incident beam within a unique structure. Such a periodic architecture exhibits two fundamental modes; pronounced counter-propagating short-range surface plasmon polariton (SR-SPP) coupled to the Ge2Sb2Te5 (GST) alloy as the feed gap, and the propagative surface plasmon polariton (PR-SPP) resonant modes tunneling to the GST nanostripes. By leveraging the multistate phase transition of alloy from amorphous to the crystalline, which induces significant complex permittivity change, the interplay between such enhanced modes can be drastically modified. Accordingly, in the intermediate phases, the proposed system experiences a coupled condition of operational over-coupling and under-coupling regimes leading to an inherently broadband response. We wisely addressing each gate-tunable meta-atom to achieve robust control over the reflection characteristics, wide phase agility up to 315? or considerable reflectance modulation up to 60%, which facilitate a myriad of on-demand optical functionalities in the telecommunication band. Based on the revealed underlying physics and electro-thermal effects in the GST alloy, a simple systematic approach for realization of an electro-optically tunable multifunctional metadevice governing anomalous reflection angle control (e.g., phased array antenna), near-perfect absorption (e.g., modulator), and polarization conversion (e.g., wave plate) is presented. As a promising alternative to their passive counterparts, such high-speed, non-volatile MSs offer an smart paradigm for reversible, energy-efficient, and programmable optoelectronic devices such as holograms, switches, and polarimeters.
Guided-wave plasmonic circuits are promising platforms for sensing, interconnection, and quantum applications in the sub-diffraction regime. Nonetheless, the loss-confinement trade-off remains a collective bottleneck for plasmonic-enhanced optical processes. Here, we report a unique plasmonic waveguide that can alleviate such trade-off and improve the efficiencies of plasmonic-based emission, light-matter-interaction, and detection simultaneously. Through different bias configurations, record experimental attributes such as normalized Purcell factor approaching 10^4, 10-dB amplitude modulation with <1 dB insertion loss and fJ-level switching energy, and photodetection sensitivity and internal quantum efficiency of -54 dBm and 6.4 % respectively can be realized within the same amorphous-based plasmonic structure. The ability to support multiple optoelectronic phenomena while providing performance gains over existing plasmonic and dielectric counterparts offers a clear path towards reconfigurable, monolithic plasmonic circuits.
We present a comprehensive review of recent developments in the field of chiral plasmonics. Significant advances have been made recently in understanding the working principles of chiral plasmonic structures. With advances in micro- and nanofabrication techniques, a variety of chiral plasmonic nanostructures have been experimentally realized; these tailored chiroptical properties vastly outperform those of their molecular counterparts. We focus on chiral plasmonic nanostructures created using bottom-up approaches, which not only allow for rational design and fabrication but most intriguingly in many cases also enable dynamic manipulation and tuning of chiroptical responses. We first discuss plasmon-induced chirality, resulting from the interaction of chiral molecules with plasmonic excitations. Subsequently, we discuss intrinsically chiral colloids, which give rise to optical chirality owing to their chiral shapes. Finally, we discuss plasmonic chirality, achieved by arranging achiral plasmonic particles into handed configurations on static or active templates. Chiral plasmonic nanostructures are very promising candidates for real-life applications owing to their significantly larger optical chirality than natural molecules. In addition, chiral plasmonic nanostructures offer engineerable and dynamic chiroptical responses, which are formidable to achieve in molecular systems. We thus anticipate that the field of chiral plasmonics will attract further widespread attention in applications ranging from enantioselective analysis to chiral sensing, structural determination, and in situ ultrasensitive detection of multiple disease biomarkers, as well as optical monitoring of transmembrane transport and intracellular metabolism.
With the rise of artificial magnetism and metamaterials, the toroidal family recently attracts more attention for its unique properties. Here we propose an all-dielectric pentamer metamolecule consisting of nano-cylinders with two toroidal dipolar resonances, whose frequencies, EM distributions and Q factor can be efficiently tuned due to the additional electric dipole mode offered by a central cylinder. To further reveal the underlying coupling effects and formation mechanism of toroidal responses, the multiple scattering theory is adopted. It is found that the first toroidal dipole mode, which can be tuned from 2.21 to 3.55 $mu$m, is mainly induced by a collective electric dipolar resonance, while the second one, which can be tuned from 1.53 to 1.84 $mu$m, relies on the cross coupling of both electric and magnetic dipolar responses. The proposed low-loss metamolecule and modes coupling analyses may pave the way for active design of toroidal responses in advanced optical devices.
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