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Physical Review A

Quantum particle interacting with a metallic particle: Spectra from quantum Langevin theory

W. M. Edmund Loh, C. H. Raymond Ooi

Published Jan 23, 2017• 3 citations
Publisher

Abstract

The effect of a nearby metallic particle on the quantum optical properties of a quantum particle in the four-level double Raman configuration is studied using the quantum Langevin approach. We obtain analytical expressions for the correlated quantum fields of Stokes and anti-Stokes photons emitted from the system and perform analysis on how the interparticle distance, the direction of observation or detection, the strengths of controllable laser fields, the presence of surface plasmon resonance, and the number density of the quantum particle affect the quantum spectra of the Stokes and anti-Stokes fields. We explore the physics behind the quantum-particle--metallic-nanoparticle interaction within the dipole approximation, that is, when the interparticle distance is much larger than the sizes of the particles. Our results show the dependence of the spectra on the interparticle distance in the form of oscillatory behavior with damping as the interparticle distance increases. At weaker laser fields the enhancement of quantum fields which manifests itself in the form of a Fano dip in the central peak of the spectra becomes significant. Also, the quantum-particle--metallic-nanoparticle coupling, which is affected by the size of the metallic nanoparticle and the number density of the quantum particle, changes the angular dependence of the spectra by breaking the angular rotational symmetry. In the presence of surface plasmon resonance the oscillatory dependence of the spectra on the interparticle distance and angles of observation becomes even stronger due to the plasmonic enhancement effect.

DOI
10.1103/physreva.95.013836

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The effect of a nearby metallic particle on the quantum optical properties of a quantum particle in the four-level double Raman configuration is studied using the quantum Langevin approach. We obtain analytical expressions for the correlated quantum fields of Stokes and anti-Stokes photons emitted from the system and perform analysis on how the interparticle distance, the direction of observation or detection, the strengths of controllable laser fields, the presence of surface plasmon resonance, and the number density of the quantum particle affect the quantum spectra of the Stokes and anti-Stokes fields. We explore the physics behind the quantum-particle--metallic-nanoparticle interaction within the dipole approximation, that is, when the interparticle distance is much larger than the sizes of the particles. Our results show the dependence of the spectra on the interparticle distance in the form of oscillatory behavior with damping as the interparticle distance increases. At weaker laser fields the enhancement of quantum fields which manifests itself in the form of a Fano dip in the central peak of the spectra becomes significant. Also, the quantum-particle--metallic-nanoparticle coupling, which is affected by the size of the metallic nanoparticle and the number density of the quantum particle, changes the angular dependence of the spectra by breaking the angular rotational symmetry. In the presence of surface plasmon resonance the oscillatory dependence of the spectra on the interparticle distance and angles of observation becomes even stronger due to the plasmonic enhancement effect.
We have developed a semianalytical theory to study a quantum plasmonic system composed of a quantum particle and a metallic particle with finite size. The quantum particle is composed of molecules driven by three laser fields and produces a coherent anti-Stokes Raman scattering (CARS) signal which is enhanced by plasmonic resonance of the metallic particle. The enhanced CARS field and the control laser form a $\mathrm{\ensuremath{\Lambda}}$ scheme that gives highly nonlinear and spatially nonlocal effects. We obtain absorption spectra that show periodic oscillations with radius of the spherical quantum particle, the whispering gallery effect. Plasmonic resonance gives very large and narrow absorption peaks as well as vanishing absorption or Fano dip at specific values of frequency and interparticle distance. The space between the two particles provides a resonant cavity effect which explains the oscillations of absorption power spectra with interparticle distance.
Quantum Langevin formalism with noise operators is used to provide quantum descriptions of photon pairs (the Stokes and anti-Stokes fields) emitted by a mesoscopic spherical particle composed of quantum particles in a double Raman configuration. The spectra of the fields obtained are sensitive to the dimension of the microsphere and can be controlled by pump and control laser fields. Spectral peaks due to quantum coherence are Stark shifted by the laser fields experiencing autofocusing inside the spherical particle, causing broadening of peaks as the size of the microsphere increases. The antinormal-order spectrum is found to be identical to the normal-order spectrum. The anti-Stokes spectrum is identical to the Stokes spectrum when the linear dispersion is neglected. Frequency-dependent dielectric functions of the Stokes and anti-Stokes spectra corresponding to the linear dispersions of the particle yield narrow morphology-dependent resonance gain peaks at certain frequencies of the Stokes and anti-Stokes spectra that depend not only on the particle size but also on the angle of observation.
We present a semi-analytical theory to describe the nonlinear scattering of Raman photon pairs from a cylindrical microparticle comprising of quantum particles in double Raman configuration. The normally ordered Stokes and anti-Stokes spectra are computed to gain insights into the quantum optical properties of the system and the variation of the spectra with microparticle’s size, orientation as well as observation angles are also analyzed and compared with the results obtained in our previous work involving mesoscopic spherical particle. Our results show several features in the spectra that are unique to the case of cylindrical microparticle and not found in the spherical particle case, such as the shifting of the side peaks originally formed due to ac Stark shifts towards the center at certain range of particle radius values, occurrence of side peaks with magnitudes comparable to that of the central peak, formation of additional peaks at certain observation angles and strong dependence of the spectra on the microparticle’s cylinder axis orientation. Most of these effects are either caused by the inhomogeneity of the incident pump and control laser fields within the volume of the cylindrical microparticle or simply due to the lack of three-dimensional symmetry of cylindrical geometry.
The mesoscopic effects on quantum correlations of photon pairs emitted by a microspherical particle composed of many quantum particles in a double Raman scheme are studied. Quantum Langevin formalism with noise operators is used to compute the nonclassical correlations between the Stokes and anti-Stokes photons, particularly the Glauber’s second-order cross- and self-correlation functions. The theory includes realistic situations of inhomogeneous field distributions of the pump and control laser fields as the result of the focusing effect of the microsphere as well as its linear dispersion. The results show that the photon correlations are affected by the size and density of the microsphere, the detection direction, and the detuning and strength of the laser fields. The self-correlation times of the quantum fields are significantly enhanced by the focusing effect of the microsphere with certain sizes.
This thesis is an attempt at studying quantum coherence effects coupled via plasmons. After introducing the quantum coherence in atomic systems in Chapter 1, we utilize it in Chapter 2 to demonstrate a new technique of detection of motion of single atoms or irons inside an optical cavity. By taking into account the interaction of coherences with surface plasmonic waves excited in metal nanoparticles, we provide a theoretical model along with experimental data in Chapter 3 to describe the modification of Raman spectra near metal nanoparticles. We show in chapter 4 that starting from two emitters, coupled via a plasmonic field, the symmetry breaking occurs, making detectable the simultaneous existence of the fast super-radiance and the slow sub-radiance emission of dye fluorescence near a plasmonic surface. In Chapter 5, we study the photon statistics of a group of emitters coupled via plasmons and by the use of quantum regression theorem, we provide a theoretical model to fully investigate the dependence of photon bunching and anti-bunching effects to the interaction between atoms, fields and surrounding mediums.
In this research, we consider the interaction between an atomic or molecular quantum system (QS) and a metallic nanoparticle (MP). We modelled QS by a three-level lambda system. Under the probe field and control field, the QS become transparent to incident light within a narrow spectrum of frequency, a phenomena known as electro- magnetically induced transparency (EIT). The quantum coherence of the QS under EIT and the strong exciton-plasmon coupling between the QS and MP are dependant on each other. The analytical expressions for the interaction of QS and MP are derived using two methods. First, the QS-MP system is considered as a one-dimensional problem. The ex- pressions derived using this method is not general, however, they provide a simple and more intuitive understanding of the interaction. The second method employed to derive the analytical expressions is by using a vectorial description. Using this model, the exact and general expressions describing the QS-MP system are derived. The density matrix of the QS-MP system was used to obtain numerical results for the dielectric function of QS and MP. The effect of field detuning, distance between the QS and MP, laser field direction and polarization on the dielectric functions are investigated.