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Physical Review A

Photon-number statistics from resonance fluorescence of a two-level atom near a plasmonic nanoparticle

Vladimir Pastukhov, Yu. V. Vladimirova, Victor N. Zadkov

Published Dec 22, 2014• 19 citations
Publisher

Abstract

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 $r\ensuremath{\le}2a$ $(r$ is the distance from the center of the nanosphere to the atom), with $a$ 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 $p(n,T)$ of the emission probability of $n$ photons in a given time interval $T$ 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 $r>2a$ 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.

DOI
10.1103/physreva.90.063831

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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≤2ar\ensuremath{\le}2ar\ensuremath≤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≤2ar\ensuremath{\le}2ar\ensuremath≤2a, featuring a characteristic twist in the ridgelike dependence and a convergence time of up to 9\ensuremathμs9\ensuremath{\mu}\text{s}9\ensuremathμs, 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 \ensuremathΩ\ensuremath∼\ensuremathγ\ensuremath{\Omega}\ensuremath{\sim}\ensuremath{\gamma}\ensuremathΩ\ensuremath∼\ensuremathγ 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.
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.
We study the resonant fluorescence emission spectrum and the intensity-intensity correlations of the emitted fluorescent field by a V-type quantum emitter (QE) which is located near a metal nanosphere. For the description of the studied phenomena, we use the density matrix equations methodology combined with electromagnetic calculations and obtain results for the profile of the resonant fluorescence spectrum and the second-order correlation functions associated with the fluorescent photons. The decay rates and the coupling term exhibit a strong dependence on the distance that separates the QE from the metal nanoparticle. This distance also influences the resonance fluorescence of the V-type QE. We find that, in the general case, the resonant fluorescence spectrum is composed of five Lorentzian-type peaks, for high interparticle distances, while, when the QE is located very close to the surface of the nanosphere, the central resonance becomes dominant, and a single-peaked spectral profile appears. The two-time correlation functions of the fluorescent photons evolve in an oscillatory manner around unity, for non-zero time delay, with a period that decreases with the increase of the field intensity. In the strong driving field regime, the antibunching to bunching crossing time does not depend on the interparticle distance, contrary to the results found in the weak driving field regime. We also find that, for a weak laser field and under specific conditions, the second-order correlation functions constantly remain in the antibunching region.
The theory of photon-number statistics in resonance fluorescence is treated, starting with the general formula for the emission probability of nnn photons during a given time interval TTT. The results fully confirm formerly obtained results by Cook that were based on the theory of atomic motion in a traveling wave. General expressions for the factorial moments are derived and explicit results for the mean and the variance are given. It is explicitly shown that the distribution function tends to a Gaussian when TTT becomes much larger than the natural lifetime of the excited atom. The speed of convergence towards the Gaussian is found to be typically slow, that is, the third normalized central moment (or the skewness) is proportional to ${T}^{\ensuremath{-}\frac{1}{2}}$. However, numerical results illustrate that the overall features of the distribution function are already well represented by a Gaussian when TTT is larger than a few natural lifetimes only, at least if the intensity of the exciting field is not too small and its detuning is not too large.
A derivation of surface-dressed optical Bloch equations, involving a treatment of surface-reflected photons and a surface plasmon resonance, is presented for a collision-damped two-level atom near or adsorbed on a metal surface. Effects of the laser bandwidth are included by means of a phase-diffusion model for the driving field. In the weak-field or large detuning limit, the population inversion and resonance fluorescence spectrum are obtained analytically. These quantities along with the surface-induced phase-decay constant of the adatom show strong oscillatory behavior as a function of the adatom-surface distance.