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Journal of Experimental and Theoretical Physics Letters

Modification of the resonance fluorescence spectrum of a two-level atom in the near field of a plasmonic nanoparticle

Evgenii S. Andrianov, Александр Александрович Пухов, Alexey P. Vinogradov, A. V. Dorofeenko, Alexander A. Lisyansky

Published Jun 1, 2013• 22 citations
Publisher

Abstract

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.

DOI
10.1134/s0021364013080043

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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.
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.
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.
We theoretically study the resonance fluorescence spectrum of a three-level quantum emitter coupled to a spherical metallic nanoparticle. We consider the case in which the quantum emitter is driven by a single laser field along one of the optical transitions. We show that the development of the spectrum depends on the relative orientation of the dipole moments of the optical transitions in relation to the metal nanoparticle. In addition, we demonstrate that the location and width of the peaks in the spectrum are strongly modified by the exciton-plasmon coupling and the laser detuning, allowing one to achieve a controlled strongly subnatural spectral line. A strong antibunching of the fluorescent photons along the undriven transition is also obtained. Our results may be used for creating a tunable source of photons which could be used for a probabilistic entanglement scheme in the field of quantum information processing.
Modification of the resonance fluorescence spec-trum of a two-level atom driving by a lasermonochromatic field in the close proximity of aplasmonic nanostructure (metal sphere) is studiedin detail. It is shown that one can control thisspectrum varying four key parameters: distancebetween the atom and the nanosphere, atom’s lo-cation around the nanosphere, the radius of thenanosphere, and polarization of the incident ra-diation. These parameters affect the local fieldenchancement, transition frequency shift and themodification of the radiative decay rate of the atominteracting with the nanosphere, which lead tomodification of the resonance fluorescence spec-trum of the atom (frequency shift of the satellitelines in the Mollow-type triplet, widths of the lines,the spectrum intensity) by contrast with that onein free space. The permittivity of the metal thenanosphere is made of is also an additional param-eter, which defines the nonradiative decay. The lat-ter in combination with other parameters allows tocontinuously control the transition from resonancefluorescence enhancement to its quenching. Thecalculation results are generalized to the case ofN two-level atoms, distributed around the nanopar-ticle in the close proximity of its surface. Thecalculations were performed for different positionsof the detector relative to the system nanoparticle-atom(s).
The photon-number statistics from resonance fluorescence of a two-level atom near a metal nanosphere driven by a laser field with finite bandwidth is studied theoretically. Our analysis shows that all interesting physics here takes place in a small area around the nanosphere where the near field and the atom-nanosphere coupling essentially affect the radiative properties of the atom. Computer modeling estimates this area roughly as $r\ensuremath{\le}2a$ (r(r(r is the distance from the center of the nanosphere to the atom), with aaa being the radius of the nanosphere. At the larger distances, the influence of the nanoparticle vanishes and the atom tends to behave similarly to that in free space. It is shown that the distribution function p(n,T)p(n,T)p(n,T) of the emission probability of nnn photons in a given time interval TTT in steady-state resonance fluorescence drastically depends on the atom location around the nanosphere for $r\ensuremath{\le}2a$, featuring a characteristic twist in the ridgelike dependence and a convergence time of up to $9\ensuremath{\mu}\text{s}$, two orders of magnitude slower than for the atom in free space. At large distances, the distribution converges to a Gaussian one, as for the atom in free space. The typical convergence time scale at large distances r>2ar>2ar>2a tends to the convergence time of the atom in free space. There are also two areas symmetrical around the nanosphere in which $\ensuremath{\Omega}\ensuremath{\sim}\ensuremath{\gamma}$ and the convergence time goes to zero. This behavior is determined by the interplay of the radiative and nonradiative decay rates of the atom due to the coupling with the metal nanosphere and by the near-field intensity. Additional parameters are the normalized laser frequency detuning from the atomic resonance and the bandwidth of the incoming laser field.
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.