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      Quantum dynamics of two quantum dots coupled through localized plasmons: An intuitive and accurate quantum optics approach using quasinormal modes

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          Abstract

          We study the quantum dynamics of two quantum dots (QDs) or artificial atoms coupled through the fundamental localized plasmon of a gold nanorod resonator. We derive an intuitive and efficient time-local master equation, in which the effect of the metal nanorod is taken into consideration self-consistently using a quasinormal mode (QNM) expansion technique of the photon Green function. Our efficient QNM technique offers an alternative and more powerful approach over the standard Jaynes-Cummings model, where the radiative decay, nonradiative decay, and spectral reshaping effect of the electromagnetic environment is rigorously included in a clear and transparent way. We also show how one can use our approach to compliment the approximate Jaynes-Cummings model in certain spatial regimes where it is deemed to be valid. We then present a study of the quantum dynamics and photoluminescence spectra of the two plasmon-coupled QDs. We first explore the non-Markovian regime, which is found to be important only on the ultrashort time scale of the plasmon mode which is about 40\(\,\)fs. For the field free evolution case of excited QDs near the nanorod, we demonstrate how spatially separated QDs can be effectively coupled through the plasmon resonance and we show how frequencies away from the plasmon resonance can be more effective for coherently coupling the QDs. Despite the strong inherent dissipation of gold nanoresonators, we show that qubit entanglements as large as 0.7 can be achieved from an initially separate state, which has been limited to less than 0.5 in previous work for weakly coupled reservoirs. We also study the superradiance and subradiance decay dynamics of the QD pair. Finally, we investigate the rich quantum dynamics of QDs that are incoherently pumped, ...

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          Chemical mapping of a single molecule by plasmon-enhanced Raman scattering.

          Visualizing individual molecules with chemical recognition is a longstanding target in catalysis, molecular nanotechnology and biotechnology. Molecular vibrations provide a valuable 'fingerprint' for such identification. Vibrational spectroscopy based on tip-enhanced Raman scattering allows us to access the spectral signals of molecular species very efficiently via the strong localized plasmonic fields produced at the tip apex. However, the best spatial resolution of the tip-enhanced Raman scattering imaging is still limited to 3-15 nanometres, which is not adequate for resolving a single molecule chemically. Here we demonstrate Raman spectral imaging with spatial resolution below one nanometre, resolving the inner structure and surface configuration of a single molecule. This is achieved by spectrally matching the resonance of the nanocavity plasmon to the molecular vibronic transitions, particularly the downward transition responsible for the emission of Raman photons. This matching is made possible by the extremely precise tuning capability provided by scanning tunnelling microscopy. Experimental evidence suggests that the highly confined and broadband nature of the nanocavity plasmon field in the tunnelling gap is essential for ultrahigh-resolution imaging through the generation of an efficient double-resonance enhancement for both Raman excitation and Raman emission. Our technique not only allows for chemical imaging at the single-molecule level, but also offers a new way to study the optical processes and photochemistry of a single molecule.
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            Modes and Mode Volumes of Leaky Optical Cavities and Plasmonic Nanoresonators

            Electromagnetic cavity modes in photonic and plasmonic resonators offer rich and attractive regimes for tailoring the properties of light-matter interactions. Yet there is a disturbing lack of a precise definition for what constitutes a cavity mode, and as a result their mathematical properties remain largely unspecified. The lack of a definition is evidenced in part by the diverse nomenclature at use - "resonance", "leaky mode", "quasimode", to name but a few - suggesting that the dissipative nature of cavity modes somehow makes them different from other modes, but an explicit distinction is rarely made. This perspective article aims to introduce the reader to some of the subtleties and working definitions that can be rigorously applied when describing the modal properties of leaky optical cavities and plasmonic nanoresonators. We describe some recent development in the field, including {calculation methods for quasinormal modes of both photonic and plasmonic resonators and the concept of a generalized effective mode volume, and we} illustrate the theory with several representative cavity structures from the fields of photonic crystals and nanoplasmonics.
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              Nonlinear photoluminescence spectra from a quantum dot-cavity system: Direct evidence of pump-induced stimulated emission and anharmonic cavity-QED

              We investigate the power-dependent photoluminescence spectra from a strongly coupled quantum dot-cavity system using a quantum master equation technique that accounts for incoherent pumping, pure dephasing, and fermion or boson statistics. Analytical spectra at the one-photon correlation level and the numerically exact multi-photon spectra for fermions are presented. We compare to recent experiments on a quantum dot-micropiller cavity system and show that an excellent fit to the data can be obtained by varying only the incoherent pump rates in direct correspondence with the experiments. Our theory and experiments together show a clear and systematic way of studying stimulated-emission induced broadening and anharmonic cavity-QED.
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                Author and article information

                Journal
                2015-05-08
                2015-11-17
                Article
                10.1103/PhysRevB.92.205420
                1505.02175
                5005ec2b-7a1c-4dde-9a10-be11805dfbac

                http://arxiv.org/licenses/nonexclusive-distrib/1.0/

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                Custom metadata
                Phys. Rev. B 92, 205420 (2015)
                cond-mat.mes-hall quant-ph

                Quantum physics & Field theory,Nanophysics
                Quantum physics & Field theory, Nanophysics

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