We introduce a second quantization scheme based on quasinormal modes, which are the dissipative modes of leaky optical cavities and plasmonic resonators with complex eigenfrequencies. The theory enables the construction of multi-plasmon/photon Fock states for arbitrary three-dimensional dissipative resonators and gives a solid understanding to the limits of phenomenological dissipative Jaynes-Cummings models. In the general case, we show how different quasinormal modes interfere through an off-diagonal mode coupling and demonstrate how these results affect cavity-modified spontaneous emission. To illustrate the practical application of the theory, we show examples using a gold nanorod dimer and a hybrid dielectric-metal cavity structure. arXiv:1808.06392v3 [cond-mat.mes-hall]
Nanophotonics finds ever broadening applications requiring complex components with many parameters to be simultaneously designed. Recent methodologies employing optimization algorithms commonly focus on a single performance objective, provide isolated designs, and do not describe how the design parameters influence the device behaviour. Here we propose and demonstrate a machine-learning-based approach to map and characterize the multi-parameter design space of nanophotonic components. Pattern recognition is used to reveal the relationship between an initial sparse set of optimized designs through a significant reduction in the number of characterizing parameters. This defines a design sub-space of lower dimensionality that can be mapped faster by orders of magnitude than the original design space. The behavior for multiple performance criteria is visualized, revealing the interplay of the design parameters, highlighting performance and structural limitations, and inspiring new design ideas. This global perspective on high-dimensional design problems represents a major shift in modern nanophotonic design and provides a powerful tool to explore complexity in next-generation devices.
Using carefully designed hybrid metal-dielectric resonators, we study molecular optomechanics in the strong coupling regime (g 2 /ωm>κ), which manifests in anharmonic emission lines in the sideband-resolved region of the cavity-emitted spectrum (κ<ωm). This optomechanical strong coupling regime is enabled through a metal-dielectric cavity system that yields not only deep subwavelength plasmonic confinement, but also dielectric-like confinement rates that are more than two orders of magnitude smaller than those from typical plasmonic modes. The classical mode parameters are quantified using quasinormal mode theory, and the quantum dynamics are computed using both standard and generalized quantum master equations. These hybrid metal-dielectic cavity modes enables one to study new avenues of multi-photon quantum plasmonics through surface enhanced Raman spectroscopy, and is also well into the ultrastrong coupling regime (g/ωm>0.1). arXiv:1805.10153v2 [cond-mat.mes-hall]
Quantum emitters coupled to plasmonic resonators are known to allow enhanced broadband Purcell factors, and such systems have been recently suggested as possible candidates for on-demand single photon sources, with fast operation speeds. However, a true single photon source has strict requirements of high efficiency (brightness) and quantum indistinguishability of the emitted photons, which can be quantified through two-photon interference experiments. To help address this problem, we employ and extend a recently developed quantized quasinormal mode approach, which rigorously quantizes arbitrarily lossy open system modes, to compute the key parameters that accurately quantify the figures of merit for plasmon-based single photon sources. We also present a quantized input-output theory to quantify the radiative and nonradiative quantum efficiencies. We exemplify the theory using a nanoplasmonic dimer resonator made up of two gold nanorods, which yields large Purcell factors and good radiative output beta factors. Considering an optically pulsed excitation scheme, we explore the key roles of pulse duration and pure dephasing on the single photon properties, and show that ultrashort pulses (sub-ps) are generally required for such structures, even for low temperature operation. We also quantify the role of the nonradiative beta factor both for single photon and two-photon emission processes. Our general approach can be applied to a wide variety of plasmon systems, including metal-dielectrics, and cavity-waveguide systems, without recourse to phenomenological quantization schemes.
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