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Physica status solidi. C, Conferences and critical reviews/Physica status solidi. C, Current topics in solid state physics

Luminescent activity of two‐level molecule with population inversion

Ryosuke Hata, Hiroshi Ajiki, Nobuhiko Yokoshi, Hajime Ishihara

Published Dec 9, 2015• 1 citation
Publisher

Abstract

Abstract A novel technique for up‐converted luminescence generation from a two‐level molecule via population inversion is studied using the quantum toy model; this model is used to represent a coupled‐molecule and metallic nano‐antenna system sustaining a localized surface plasmon polariton (LSPP). The metallic nano‐antenna is assumed to have anharmonicity, reflecting experimentally observed results. The system is driven by a strong, offresonant, and Gaussian pulse laser so that the LSPP exhibits a Mollow triplet spectrum. When the two‐level molecular resonance is tuned to the upper Mollow triplet sideband, the molecular‐level population is inverted. We discuss the population dynamics, the Purcell effect, and the up‐converted luminescence activity of the two‐level molecule. These results indicate the potential applications of the present system in novel coherent light sources. (© 2016 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

DOI
10.1002/pssc.201510157

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Abstract A novel technique for up‐converted luminescence generation from a two‐level molecule via population inversion is studied using the quantum toy model; this model is used to represent a coupled‐molecule and metallic nano‐antenna system sustaining a localized surface plasmon polariton (LSPP). The metallic nano‐antenna is assumed to have anharmonicity, reflecting experimentally observed results. The system is driven by a strong, offresonant, and Gaussian pulse laser so that the LSPP exhibits a Mollow triplet spectrum. When the two‐level molecular resonance is tuned to the upper Mollow triplet sideband, the molecular‐level population is inverted. We discuss the population dynamics, the Purcell effect, and the up‐converted luminescence activity of the two‐level molecule. These results indicate the potential applications of the present system in novel coherent light sources. (© 2016 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
We theoretically study a novel up-converted luminescence from a two-level molecule coupled with an auxiliary system such as an anharmonic LC resonator and a metallic nano-antenna. The auxiliary system is assumed to be strongly driven by a continuous wave laser so that a Mollow triplet appears in the luminescent spectrum. When the peak energy of the upper Mollow triplet sideband is tuned to the molecular excited level, the intensity of the up-converted luminescence is considerably enhanced. At the same time, the population of the two-level molecule is inverted. We also discuss the conditions for high photoemission efficiency in the up-converted luminescence under a highly inverted population. This result indicates the potential applications in future single-molecule lasers.
Coherent light sources pumped by external fields require multi-level systems to achieve a population inversion and they always convert an input frequency into lower one. In their paper on pp. 105–108, Hata and coworkers, however, theoretically proposed a frequency up-conversion luminescence from a two-level system with inverted population. The two-level system interacts with a metallic nano-antenna sustaining a localized surface plasmon-polariton. The obtained result shows that a strong and off-resonant Gaussian pulse laser with optimum peak intensity realizes the population inversion of the two-level system, which generates the up-converted luminescence. This demonstration indicates the potential applications of the present system in novel coherent light sources.
We theoretically propose a new method for generating up-converted coherent light from two-level systems (TLSs) coupled with a plasmonic nanocavity. The emission spectrum of a TLS excited by a strong laser exhibits a triplet structure called the Mollow triplet. If the lower Mollow sideband is tuned to the cavity mode energy, population inversion of a TLS occurs. When the driving laser is abruptly truncated under this condition, an up-converted photon is emitted from the TLSs. We also predict the up-converted superfluorescence from an ensemble of TLSs as a correlation effect among the excited states of the TLSs.
Surface plasmon polaritons (SPPs) lasing requires population inversion, it is inefficient and possesses poor spectral properties. We develop an inversion-less concept for a quantum plasmonic waveguide that exploits unidirectional superradiant SPP (SSPP) emission of radiation to produce intense coherent surface plasmon beams. Our scheme includes a resonantly driven cold atomic medium in a lossless dielectric situated above an ultra-low loss negative index metamaterial (NIMM) layer. We propose generating unidirectional superradiant radiation of the plasmonic field within an atomic medium and a NIMM layer interface and achieve amplified SPPs by introducing phase-match between the superradiant SPP wave and coupled laser fields. We also establish a parametric resonance between the weak modulated plasmonic field and the collective oscillations of the atomic ensemble, thereby suppressing decoherence of the stably amplified directional polaritonic mode. Our method incorporates the quantum gain of the atomic medium to obtain sufficient conditions for coherent amplification of superradiant SPP waves, and we explore this method to quantum dynamics of the atomic medium being coupled with the weak polaritonic waves. Our waveguide configuration acts as a surface plasmon laser and quantum plasmonic transistor and opens prospects for designing controllable nano-scale lasers for quantum and nano-photonic applications.
We investigate properties of a two-level atom coupled to a single cavity mode, and driven by a strong, in general off-resonance, external field. The cavity field is tuned to resonance with a Mollow sideband. We show that the steady-state atomic population may be highly (nearly totally) inverted, a phenomenon forbidden in semiclassical theory, and that a strong enhancement of the resonance fluorescence results. This system is suggested as an alternative approach to create the atomic inversion necessary for laser or maser generation without using additional atomic levels. We also investigate properties of the cavity field, derive an analytical expression for the photon number distribution in the good cavity or strong-coupling limit, and discuss the conditions under which this system acts as a single-atom dressed-state laser.
We have investigated the coherent transfer of excitonic populations in a semiconductor quantum dot (SQD) modulated by the surface plasmon of a metallic nanoparticle (MNP). The SQD is considered as a three-level V-type atomic system. We applied a transform-limited laser pulse field resonant with the upper atomic levels of the SQD. When the SQD is close enough to the MNP, the otherwise equally populated atomic levels can be selectively excited. Selectivity population can be achieved by two physical mechanisms: an enhancement of the Rabi frequencies that drive the optical transitions, which depends on the polarization arrangement, and a frequency shift of the optical transitions that leads to a dynamical detuning.