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Journal of Experimental and Theoretical Physics

Efficient transfer of light energy to a nanoparticle by means of a resonance atomic lens

G. N. Nikolaev

Published Mar 1, 2006• 1 citation
Publisher

Abstract

A cascade transfer of light energy to a resonance atom situated near a spherical nanoparticle and then, by a nonradiative mechanism, to the nanoparticle itself is considered. It is established that the efficiency of the cascade transfer essentially depends on the frequency and polarization of light, on the distance between the atom and the particle, on the optical properties of the particle, and on the time conditions of radiation. The rate of light absorption by a metal nanoparticle via cascade energy transfer may be 10 4 –10 5 times higher than the direct absorption of light by a nanoparticle. For a fixed frequency of light, the cascade transfer of energy is a sharply selective function of the distance between the atom and the particle (the resonance width is about 10 −2 of the particle radius). Atomic fluorescence exhibits similar behavior. This feature can form the basis for a new method of optical scanning microscopy and location and localization of atoms near the surface of a particle.

DOI
10.1134/s1063776106030034

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A cascade transfer of light energy to a resonance atom situated near a spherical nanoparticle and then, by a nonradiative mechanism, to the nanoparticle itself is considered. It is established that the efficiency of the cascade transfer essentially depends on the frequency and polarization of light, on the distance between the atom and the particle, on the optical properties of the particle, and on the time conditions of radiation. The rate of light absorption by a metal nanoparticle via cascade energy transfer may be 10 4 –10 5 times higher than the direct absorption of light by a nanoparticle. For a fixed frequency of light, the cascade transfer of energy is a sharply selective function of the distance between the atom and the particle (the resonance width is about 10 −2 of the particle radius). Atomic fluorescence exhibits similar behavior. This feature can form the basis for a new method of optical scanning microscopy and location and localization of atoms near the surface of a particle.
Absorption of light by nanoparticle in the presence of resonant atom is theoretically investigated. Both the direct absorption of light by the nanoparticle and the absorption due to cascade energy transfer from light to the atom and then to the nanoparticle are taken into account. It is shown, that the cascade energy transfer is proportional to the imaginary part of the Green's photon function in this conditions. The Green's function is calculated in the quasi static approximation because of smallness both the size of the nanoparticle and the distance between it and the atom. The resonant atom is described in the generalized two-level model taking into account the direction of the atomic dipole moment. It is shown, that the light absorption by the nanoparticle can be increased by several orders because of presence of the atom. In the case when the nanoparticle is surrounded by collection of atoms it is found that the optical bistability is possible in this system. The range of parameters leading to the bistable behavior is found.
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.
We report the results of numerical modelling of emission of a two-level atom near a metal nanoparticle under resonant interaction of light with plasmon modes of the particle. Calculations have been performed for different polarisations of light by a dipole approximation method and a complex multipole method. Depending on the distance between a particle and an atom, the contribution of the nonradiative process of electron tunnelling from a two-level atom into a particle, which is calculated using the quasi-classical approximation, has been taken into account and assessed. We have studied spherical gold and silver particles of different diameters . The rates of electron tunnelling and of spontaneous decay of the excited atomic state are found. The results can be used to develop nanoscale plasmonic emitters, lasers and photodetectors.
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.
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).
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.