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Physical Review B

Resonance fluorescence of single molecules assisted by a plasmonic structure

Ying Gu, Lina Huang, Olivier J. F. Martin, Qihuang Gong

Published May 19, 2010• 62 citations
Publisher

Abstract

The resonance fluorescence of a two-level single molecular system interacting with a plasmonic nanostructure is investigated. Specific regions of space are identified, where a balance exists between the near-field enhancement and the modification of the decay rate, such that the fluorescence spectrum of the molecule exhibits the Mollow triplet and the emission photons are antibunched. The utilization of such quantum phenomena at the vicinity of custom-designed plasmonic nanostructures paves the way for applications in nanoscale quantum devices and quantum information processing.

DOI
10.1103/physrevb.81.193103

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The resonance fluorescence of a two-level single molecular system interacting with a plasmonic nanostructure is investigated. Specific regions of space are identified, where a balance exists between the near-field enhancement and the modification of the decay rate, such that the fluorescence spectrum of the molecule exhibits the Mollow triplet and the emission photons are antibunched. The utilization of such quantum phenomena at the vicinity of custom-designed plasmonic nanostructures paves the way for applications in nanoscale quantum devices and quantum information processing.
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.
We present a theoretical study of the resonance fluorescence of a four-level double-V\mathsf{V}V-type quantum emitter near a plasmonic nanostructure. The quantum system interacts with two orthogonal circularly polarized laser fields with the same frequency and intensity, but with different phases. For the plasmonic nanostructure we consider a two-dimensional array of metal-coated dielectric nanospheres. We show that the presence of the plasmonic nanostructure leads to strong modification of both the resonance fluorescence spectrum and the transition from antibunching to bunching for the fluorescent photons. In addition, we show that both the resonance fluorescence spectrum and the second-order correlation function are strongly phase-dependent so that the relative phase of laser fields can be used for the efficient control of the resonance fluorescence characteristics. The results are explained by using a dressed-state picture.
This review is devoted to the study of effects of quantum optics in nanostructures. The mechanisms by which the rates of radiative and nonradiative decay are modified are considered in the model of a two-level quantum emitter (QE) near a plasmonic nanoparticle (NP). The distributions of the intensity and polarization of the near field around an NP are analyzed, which substantially depend on the polarization of the external field and parameters of plasmon resonances of the NP. The effects of quantum optics in the system NP + QE plus external laser field are analyzed-modification of the resonance fluorescence spectrum of a QE in the near field, bunching/antibunching phenomena, quantum statistics of photons in the spectrum, formation of squeezed states of light, and quantum entangled states in these systems.
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.
The resonance fluorescence spectrum of an atom located in the near field of a plasmonic nanoparticle is considered. It is shown that, as the atom gets close to the nanoparticle, the high-frequency peak of the Mollow triplet disappears and the spectrum has a Fano resonance shape. The low-frequency peak also disappears as the distance between the atom and the nanoparticle decreases further. For small distances, when the atom interacts with the nanoparticle much more strongly than with the external field, the spectrum represents a Lorentzian line whose width is proportional to the square of the atom-nanoparticle coupling constant.