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Optoelectronics Instrumentation and Data Processing

Local electric fields in ensembles of composite nanoparticles

Alexander A. Zabolotskii

Published Jul 1, 2016• 3 citations
Publisher

Abstract

Specific features of the formation of local fields in spherical composite nanoparticles containing metal cores surrounded by a silica shell with implanted dye molecules are studied. A system consisting of two closely located nanoparticles (dimers) is analyzed. It is shown that the field configuration in the dimer corresponds to a much more effective feedback than that in the case of individual spherical nanoparticles. The dynamics of the fluorescence field near a flat package of composite nanoparticles is studied numerically with due allowance for the enhancement of the dye fluorescence field, saturation of the energetic transition, and diffraction. It is found that close arrangement of nanoparticles leads under pumping conditions to the formation of high-intensity fields localized with time in the space of the nanoparticle package neighborhood.

DOI
10.3103/s8756699016040117

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Specific features of the formation of local fields in spherical composite nanoparticles containing metal cores surrounded by a silica shell with implanted dye molecules are studied. A system consisting of two closely located nanoparticles (dimers) is analyzed. It is shown that the field configuration in the dimer corresponds to a much more effective feedback than that in the case of individual spherical nanoparticles. The dynamics of the fluorescence field near a flat package of composite nanoparticles is studied numerically with due allowance for the enhancement of the dye fluorescence field, saturation of the energetic transition, and diffraction. It is found that close arrangement of nanoparticles leads under pumping conditions to the formation of high-intensity fields localized with time in the space of the nanoparticle package neighborhood.
This paper considers a thin plane nanosystem consisting of molecular chains of dye J-aggregates forming bundles elongated in one direction and spherical gold nanoparticles located near them. Expressions are derived for the polarization of the exciton transition in the external field under the mutual influence of the dipole fields of the monomers constituting the dye J-aggregates and for the induced dipole of the nanoparticle. It is shown that in this system, mirrorless optical bistability of the fluorescence spectral density of the dye J-aggregates is possible, depending on the pump field intensity. The parameters of this dependence are critically determined by the distance between the molecular bundles and nanoparticles and by the angle between the field polarization direction and the axis of the bundle of J-aggregates. The use of the nanosystem as a sensor is discussed.
This paper describes the nonradiation (Forster) energy transfer between a dye J-aggregate and closely located nanoparticles possessing the properties of two-level systems. Nanoparticles can be quantum dots (QDs) or a spherical symmetric package of atoms. The dynamics of the process is described by deriving the equations that characterize the density matrix dynamics in a two-level medium and the evolution of exciton pulses in an extended quasi-one-dimensional dye J-aggregate. It is shown that effective controlled resonant transfer of the energy stored in QDs is implemented in the system and manifested in the amplification of the exciton pulses. In turn, there is a possibility of the reverse process of exciton energy transfer in partial inversion of two-level transitions of QDs. The results of this paper are confirmed by the experimental data from the literature.
The near-field interaction of two spherical nanoparticles containing dense ensembles of two-or multilevel atoms in an external field of optical low-intensity radiation is shown to result in the formation of resonances whose frequencies differ considerably from the transition frequencies in the spectrum of the interacting atoms. Optical near-field resonances are shown to play an important role in metastructural systems composed of activated nanospheres. The reflectance of a metastructural system of activated nanospheres oriented along a certain direction depends strongly on the polarization and the frequency of external radiation, as well as on the concentration of impurity atoms inside the nanospheres and on their sizes.
Abstract It is demonstrated that the interaction of a two-level quantum emitter (atom, molecule, etc) with a plasmonic nanoparticle (prolate nanospheroid) in an external laser field features either an essential increase (up to a few orders of magnitude) or reduction (up to a few times) of the total decay rate of the emitter in specific areas around the nanoparticle in contrast to its decay rate in a vacuum. It is also shown that the resonance fluorescence spectrum of the emitter in close proximity to a plasmonic nanoparticle is very sensitive to both the location of the emitter around the nanoparticle and to polarization of the near-field, which depends in turn on the polarization of the incident laser field. This can be used in engineering potential quantum optics experiments with quantum emitters in the near-field, as well as for 3D nanoscopy of the near-field by registering the resonance fluorescence spectra of quantum emitters scattered in the vicinity of a plasmonic nanoparticle.
In the framework of classical electrodynamics we have obtained and investigated analytical expressions for the radiation linewidth of forbidden E2 transitions in an atom located near a dimer of spherical particles. It is shown that the material of particles, their location and size have a significant effect on the linewidth of the E2 transition in the atom. It is found that in the gap between metal spherical nanoparticles, the linewidth of E2 transitions in the atom can take on substantially larger values than in the case of an atom near a single metal nanoparticle.
Modification of the resonance fluorescence spectrum of a two-level atom driven by a monochromatic field in the close proximity of a plasmonic nanostructure (metal sphere) is studied in detail. It is shown that one can control this spectrum by varying several key parameters: (i) the radius of the nanosphere, (ii) polarization of the incident radiation, and (iii) the atom's location around the nanosphere (its radial coordinate and polar angle in the spherical coordinate system). These parameters affect the local field enhancement and the modification of the radiative decay rate of the atom interacting with the nanosphere, which leads to modification of the resonance fluorescence spectrum of the atom (e.g., frequency shift of the satellite lines in the Mollow-type triplet, widths of the lines, and the spectrum intensity) by contrast with that in free space. The permittivity of the metal the nanosphere is made of is also an additional parameter, which defines the nonradiative decay. The latter in combination with other parameters allows continuous control of the transition from resonance fluorescence enhancement to its quenching.