Quantum Interference and Entanglement of Surface Plasmons

Surface plasma waves arise from the collective oscillations of billions of electrons at the surface of a metal in unison. The simplest way to quantize these waves is by direct analogy to electromagnetic fields in free space, with the surface plasmon, the quantum of the surface plasma wave, playing the same role as the photon. It follows that surface plasmons should exhibit all of the same quantum phenomena that photons do, including quantum interference and entanglement.

Unlike photons, however, surface plasmons suffer strong losses that arise from the scattering of free electrons from other electrons, phonons, and surfaces. Under some circumstances, these interactions might also cause “pure dephasing,” which entails a loss of coherence without absorption. Quantum descriptions of plasmons usually do not account for these effects explicitly, and sometimes ignore them altogether. In light of this extra microscopic complexity, it is necessary for experiments to test quantum models of surface plasmons.

In this thesis, I describe two such tests that my collaborators and I performed. The first was a plasmonic version of the Hong-Ou-Mandel experiment, in which we observed two-particle quantum interference between plasmons with a visibility of 93 ± 1%. This measurement confirms that surface plasmons faithfully reproduce this effect with the same visibility and mutual coherence time, to within measurement error, as in the photonic case.

The second experiment demonstrated path entanglement between surface plasmons with a visibility of 95 ± 2%, confirming that a path-entangled state can indeed survive without measurable decoherence. This measurement suggests that elastic scattering mechanisms of the type that might cause pure dephasing must have been weak enough not to significantly perturb the state of the metal under the experimental conditions we investigated.

These two experiments add quantum interference and path entanglement to a growing list of quantum phenomena that surface plasmons appear to exhibit just as clearly as photons, confirming the predictions of the simplest quantum models.

Classical and Quantum Effects in Plasmonic Metals

The field of plasmonics exploits the unique optical properties of metallic nanostructures to concentrate and manipulate light at subwavelength length scales. Metallic nanostructures get their unique properties from their ability to support surface plasmons– coherent wave-like oscillations of the free electrons at the interface between a conductive and dielectric medium. Recent advancements in the ability to fabricate metallic nanostructures with subwavelength length scales have created new possibilities in technology and research in a broad range of applications.

In the first part of this thesis, we present two investigations of the relationship between the charge state and optical state of plasmonic metal nanoparticles. Using experimental bias-dependent extinction measurements, we derive a potential- dependent dielectric function for Au nanoparticles that accounts for changes in the physical properties due to an applied bias that contribute to the optical extinction. We also present theory and experiment for the reverse effect– the manipulation of the carrier density of Au nanoparticles via controlled optical excitation. This plasmoelectric effect takes advantage of the strong resonant properties of plasmonic materials and the relationship between charge state and optical properties to eluci- date a new avenue for conversion of optical power to electrical potential.

The second topic of this thesis is the non-radiative decay of plasmons to a hot-carrier distribution, and the distribution’s subsequent relaxation. We present first-principles calculations that capture all of the significant microscopic mechanisms underlying surface plasmon decay and predict the initial excited carrier distributions so generated. We also preform ab initio calculations of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We extend these first-principle methods to calculate the electron-temperature dependent dielectric response of hot electrons in plasmonic metals, including direct interband and phonon-assisted intraband transitions. Finally, we combine these first-principles calculations of carrier dynamics and optical response to produce a complete theoretical description of ultrafast pump-probe measurements, free of any fitting parameters that are typical in previous analyses.

Optical waveguides and switches based on periodic arrays of carbon nanotubes

This document presents the modeling and characterization of novel optical devices based on periodic arrays of multiwalled carbon nanotubes. Vertically aligned carbon nanotubes can be grown in the arrangement of two-dimensional arrays of precisely determined dimensions. Having their dimensions comparable to the wavelength of light makes carbon nanotubes good candidates for utilization in nano-scale optical devices. We report that highly dense periodic arrays of multiwalled carbon nanotubes can be utilized as sub-wavelength structures for establishing advanced optical materials, such as metamaterials and photonic crystals. We demonstrate that when carbon nanotubes are grown close together at spacing of the order of few hundred nanometers, they display artificial optical properties towards the incident light, acting as metamaterials. By utilizing these properties we have established micro-scaled plasmonic high pass filter which operates in the optical domain. Highly dense arrays of multiwalled also offer a periodic dielectric constant to the incident light and display interesting photonic band gaps, which are frequency domains within which on wave propagation can take place. We have utilized these band gaps displayed by a periodic nanotube array, having 400 nm spacing, to construct photonic crystals based optical waveguides and switches. © 2011 IEEE.

Plasmonic nanofocusing of light in an integrated silicon photonics platform.

The capability to focus electromagnetic energy at the nanoscale plays an important role in nanoscinece and nanotechnology. It allows enhancing light matter interactions at the nanoscale with applications related to nonlinear optics, light emission and light detection. It may also be used for enhancing resolution in microscopy, lithography and optical storage systems. Hereby we propose and experimentally demonstrate the nanoscale focusing of surface plasmons by constructing an integrated plasmonic/photonic on chip nanofocusing device in silicon platform. The device was tested directly by measuring the optical intensity along it using a near-field microscope. We found an order of magnitude enhancement of the intensity at the tip's apex. The spot size is estimated to be 50 nm. The demonstrated device may be used as a building block for "lab on a chip" systems and for enhancing light matter interactions at the apex of the tip.

Plasmonic nanotips for on-chip nanoscale confinement of light

We demonstrate the on-chip nanoscale focusing of surface plasmons in metallic nanotip coupled to the silicon waveguide. Strong field enhancement is observed at the apex of the tip. Enhancing light matter interactions is discussed. © 2012 OSA.

Plasmonic nanotips for on-chip nanoscale confinement of light

We demonstrate the on-chip nanoscale focusing of surface plasmons in metallic nanotip coupled to the silicon waveguide. Strong field enhancement is observed at the apex of the tip. Enhancing light matter interactions is discussed. © 2011 Optical Society of America.

Numerical study of sub-wavelength plasmonic waveguide

The authors present an analysis of a plasmonic waveguide, simulated using a two-dimensional finite-difference time-domain technique. With the surface structures located on the surface of the metal, the device is able to confine and guide light waves in a sub-wavelength scale. And two waveguides can be placed within 150 nm (similar to 6% of the incident wavelength) that will helpful for the optoelectronic integration. Within the 20 mu m simulation region, it is found that the intensity of the guided light at the interface is roughly two to four times the peak intensity of the incident light, and the propagation length can reach approximately 40 Pm at the wavelength of 2.44 mu m. (c) 2007 Elsevier B.V. All rights reserved.

Resonant Enhanced Wave Filter and Waveguide via Surface Plasmons

The authors present an analysis of plasmonic wave filter and curved waveguide, simulated using a 2-D finite-difference time-domain technique. With different dielectric materials or surface structures located on the interface of the metal/dielectric, the resonant enhanced wave filter can divide light waves of different wavelengths and guide them with low losses. And the straight or curved waveguide can confine and guide light waves in a subwavelength scale. Within the 20 mu m simulation region, it is found that the intensity of the guided light at the interface is roughly four times the peak intensity of the incident light.

High efficiency fiber to waveguide optical coupler in silicon-on-insulator-based slot waveguides - art. no. 68310R

We propose a novel optical fiber-to-waveguide coupler for integrated optical circuits. The proper materials and structural parameters of the coupler, which is based on a slot waveguide, are carefully analyzed using a full-vectorial three dimensional mode solver. Because the effective refractive index of the mode in a silicon-on-insulator-based slot waveguide can be extremely close to that of the fiber, a highly efficient fiber-to-waveguide coupling application can be realized. For a TE-like mode, the calculated minimum mismatch loss is about 1.8dB at 1550nm, and the mode conversion loss can be less than 0.5dB. The discussion of the present state-of-the-art is also involved. The proposed coupler can be used in chip-to-chip communication.

Growth mechanism of InGaAlAs waveguides by narrow stripe selective MOVPE

Growth mechanism of InGaAlAs waveguides by narrow stripe selective MOVPE has been studied. Both the InGaAlAs bulk waveguides and the InGaAlAs MQW waveguides were successful grown on the patterned substrates at optimized growth conditions. The mask stripe width varied from 0 to 40 mu m, while the window region width between a pair of mask stripes was fixed 2.5 mu m. These selectively grown waveguides were covered by specific InP layers, which can keep the InGaAlAs waveguides from being oxidized during the fabrication of devices. In particular, there exhibit strong dependences of the photoluminescence (PL) spectrum on the mask stripe width for the samples. The results were explained in considering both the migration effect from a masked region (MMR) and the lateral vapor diffusion effect (LVD).

Probing the ultimate limits of plasmonic enhancement.

Metals support surface plasmons at optical wavelengths and have the ability to localize light to subwavelength regions. The field enhancements that occur in these regions set the ultimate limitations on a wide range of nonlinear and quantum optical phenomena. We found that the dominant limiting factor is not the resistive loss of the metal, but rather the intrinsic nonlocality of its dielectric response. A semiclassical model of the electronic response of a metal places strict bounds on the ultimate field enhancement. To demonstrate the accuracy of this model, we studied optical scattering from gold nanoparticles spaced a few angstroms from a gold film. The bounds derived from the models and experiments impose limitations on all nanophotonic systems.

Plasmonic nanorod metamaterials for biosensing.

Label-free plasmonic biosensors rely either on surface plasmon polaritons or on localized surface plasmons on continuous or nanostructured noble-metal surfaces to detect molecular-binding events(1-4). Despite undisputed advantages, including spectral tunability(3), strong enhancement of the local electric field(5,6) and much better adaptability to modern nanobiotechnology architectures(7), localized plasmons demonstrate orders of magnitude lower sensitivity compared with their guided counterparts(3). Here, we demonstrate an improvement in biosensing technology using a plasmonic metamaterial that is capable of supporting a guided mode in a porous nanorod layer. Benefiting from a substantial overlap between the probing field and the active biological substance incorporated between the nanorods and a strong plasmon-mediated energy confinement inside the layer, this metamaterial provides an enhanced sensitivity to refractive-index variations of the medium between the rods (more than 30,000nm per refractive-index unit). We demonstrate the feasibility of our approach using a standard streptavidin-biotin affinity model and record considerable improvement in the detection limit of small analytes compared with conventional label-free plasmonic devices.

Dressing Plasmons in Particle-in-Cavity Architectures

Placing metallic nanoparticles inside cavities, rather than in dimers, greatly improves their plasmonic response. Such particle-in-cavity (PIC) hybrid architectures are shown to produce extremely strong field enhancement at the particle cavity junctions, arising from the cascaded focusing of large optical cross sections into small gaps. These simply constructed PIC structures produce the strongest field enhancement for coupled nanoparticles, up to 90% stronger than for a dimer. The coupling is found to follow a universal power law with particle surface separation, both for field enhancements and resonant wavelength shifts. Significantly enhanced Raman signals are experimentally observed for molecules adsorbed in such PIC structures, in quantitive agreement with theoretical calculations. PIC architectures may have important implications in many applications, such as reliable single molecule sensing and light harvesting in plasmonic photovoltaic devices.

Actively Tuned Plasmons on Elastomerically Driven Au Nanoparticle Dimers

We demonstrate a novel way to actively tune surface plasmons by fabricating plasmonic nanostructures on stretchable elastomeric films. This allows reversible modification of the metal geometry on the nanometer scale. Using 100 nm scale Au nanoparticle dimers whose spacing is stretch-tuned reveals radically different spectral tuning than previously reported for sub-10-nm nanoparticles, but which can be explained by a revised interpretation of existing models. Tuning plasmons in this way offers a much more robust way than lithography to interrogate the physics of localized plasmons and has applications in optimized surface-enhanced luminescence and Raman scattering.