Excitation of surface plasmons at a SiO2/Ag interface by silicon quantum dots: Experiment and theory

The excitation of surface plasmons (SPs) by optically excited silicon quantum dots (QDs) located near a Ag interface is studied both experimentally and theoretically for different QD-interface separations. The Si QDs are formed in the near-surface region of an SiO2 substrate by Si ion implantation and thermal annealing. Photoluminescence decay-rate distributions, as derived from an inverse Laplace transform of the measured decay trace, are determined for samples with and without a Ag cover layer. For the smallest, investigated Si-QDs-to-interface distance of 44 nm the average decay rate at lambda=750 nm is enhanced by 80% due to the proximity of the Ag-glass interface, with respect to an air-glass interface. Calculations based on a classical dipole oscillator model show that the observed decay rate enhancement is mainly due to the excitation of surface plasmons that are on the SiO2/Ag interface. By comparing the model calculations to the experimental data, it is determined that Si QDs have a very high internal emission quantum efficiency of (77±17)%. At this distance they can excite surface plasmons at a rate of (1.1±0.2)×104 s¿1. From the model it is also predicted that by using thin metal films the excitation of surface plasmons by Si QDs can be further enhanced. Si QDs are found to preferentially excite symmetric thin-film surface plasmons

Planar metal plasmon waveguides: frequency-dependent dispersion, propagation, localization, and loss beyond the free electron model

A numerical analysis of surface plasmon dispersion, propagation, and localization on smooth lossy films is presented. Particular attention is given to determining wavelength-dependent behavior of thin Ag slab waveguides embedded in a symmetric SiO2 environment. Rather than considering Ag as a damped free electron gas, the metal is defined by the experimentally determined optical constants of Johnson and Christy and Palik. As in free electron gas models, analytic dispersion results indicate a splitting of plasmon modes—corresponding to symmetric and antisymmetric field distributions—as film thickness is decreased below 50 nm. However, unlike free electron gas models, the surface plasmon wave vector remains finite at resonance with the antisymmetric-field plasmon converging to a pure photon mode for very thin films. In addition, allowed excitation modes are found to exist between the bound and radiative branches of the dispersion curve. The propagation characteristics of all modes are determined, and for thin films (depending upon electric field symmetry), propagation distances range from microns to centimeters in the near infrared. Propagation distances are correlated with both the field decay (skin depth) and energy density distribution in the metal and surrounding dielectric. While the energy density of most long-range surface plasmons exhibits a broad spatial extent with limited confinement in the waveguide, it is found that high-field confinement does not necessarily limit propagation. In fact, enhanced propagation is observed for silver films at ultraviolet wavelengths despite strong field localization in the metal. The surface plasmon characteristics described in this paper provide a numerical springboard for engineering nanoscale metal plasmon waveguides, and the results may provide a new avenue for integrated optoelectronic applications

Size-dependent oxygen-related electronic states in silicon nanocrystals

Silicon nanocrystals embedded in SiO2 were isolated with a selective etching procedure, and the isolated nanocrystals' excitonic emission energy was studied during controlled oxidation. Nanocrystals having initial diameters, d(0), of similar to 2.9-3.4 nm showed a photoluminescence (PL) blueshift upon oxidatively induced size reduction, as expected from models of quantum confinement. Oxidation of smaller Si nanocrystals (d(0)similar to 2.5-2.8 nm) also initially resulted in a PL blueshift, but a redshift in the PL was then observed after growth of similar to 0.3 monolayers of native oxide. This decrease in excitonic emission energy during oxidation is consistent with the theoretically predicted formation of an oxygen-related excitonic recombination state

Highly confined electromagnetic fields in arrays of strongly coupled Ag nanoparticles

Linear arrays of very small Ag nanoparticles (diameter ~10 nm, spacing 0–4 nm) were fabricated in sodalime glass using an ion irradiation technique. Optical extinction spectroscopy of the arrays reveals a large polarization-dependent splitting of the collective plasmon extinction band. Depending on the preparation condition, a redshift of the longitudinal resonance as large as 1.5 eV is observed. Simulations of the three-dimensional electromagnetic field evolution are used to determine the resonance energy of idealized nanoparticle arrays with different interparticle spacings and array lengths. Using these data, the experimentally observed redshift is attributed to collective plasmon coupling in touching particles and/or in long arrays of strongly coupled particles. The simulations also indicate that for closely coupled nanoparticles (1–2 nm spacing) the electromagnetic field is concentrated in nanoscale regions (10 dB radius: 3 nm) between the particles, with a 5000-fold local field intensity enhancement. In arrays of 1-nm-spaced particles the dipolar particle interaction extends to over 10 particles, while for larger spacing the interaction length decreases. Spatial images of the local field distribution in 12-particle arrays of touching particles reveal a particlelike coupled mode with a resonance at 1.8 eV and a wirelike mode at 0.4 eV

Loss mechanisms of surface plasmon polaritons on gold probed by cathodoluminescence imaging spectroscopy

We use cathodoluminescence imaging spectroscopy to excite surface plasmon polaritons and measure their decay length on single crystal and polycrystalline gold surfaces. The surface plasmon polaritons are excited on the gold surface by a nanoscale focused electron beam and are coupled into free space radiation by gratings fabricated into the surface. By scanning the electron beam on a line perpendicular to the gratings, the propagation length is determined. Data for single-crystal gold are in agreement with calculations based on dielectric constants. For polycrystalline films, grain boundary scattering is identified as additional loss mechanism, with a scattering coefficient SG=0.2%

Photoluminescence quantum efficiency of dense silicon nanocrystal ensembles in SiO2

The photoluminescence decay characteristics of silicon nanocrystals in dense ensembles fabricated by ion implantation into silicon dioxide are observed to vary in proportion to the calculated local density of optical states. A comparison of the experimental 1/e photoluminescence decay rates to the expected spontaneous emission rate modification yields values for the internal quantum efficiency and the intrinsic radiative decay rate of silicon nanocrystals. A photoluminescence quantum efficiency as high as 59%±9% is found for nanocrystals emitting at 750 nm at low excitation power. A power dependent nonradiative decay mechanism reduces the quantum efficiency at high pump intensity

Tuning the emission wavelength of Si nanocrystals in SiO2 by oxidation

Si nanocrystals (diameter 2–5 nm) were formed by 35 keV Si + implantation at a fluence of 6 × 1016 Si/cm2 into a 100 nm thick thermally grown SiO2 film on Si (100), followed by thermal annealing at 1100 °C for 10 min. The nanocrystals show a broad photoluminescence spectrum, peaking at 880 nm, attributed to the recombination of quantum confined excitons. Rutherford backscattering spectrometry and transmission electron microscopy show that annealing these samples in flowing O2 at 1000 °C for times up to 30 min results in oxidation of the Si nanocrystals, first close to the SiO2 film surface and later at greater depths. Upon oxidation for 30 min the photoluminescence peak wavelength blueshifts by more than 200 nm. This blueshift is attributed to a quantum size effect in which a reduction of the average nanocrystal size leads to emission at shorter wavelengths. The room temperature luminescence lifetime measured at 700 nm increases from 12 µs for the unoxidized film to 43 µs for the film that was oxidized for 29 min

Local density of states, spectrum, and far-field interference of surface plasmon polaritons probed by cathodoluminescence

The surface plasmon polariton (SPP) field intensity in the vicinity of gratings patterned in an otherwise planar gold surface is spatially resolved using cathodoluminescence (CL). A detailed theoretical analysis is presented that successfully explains the measured CL signal based upon interference of transition radiation directly generated by electron impact and SPPs launched by the electron and outcoupled by the grating. The measured spectral dependence of the SPP yield per incoming electron is in excellent agreement with rigorous electromagnetic calculations. The CL emission is shown to be similar to that of a dipole oriented perpendicular to the surface and situated at the point of electron impact, which allows us to establish a solid connection between the CL signal and the photonic local density of states associated to the SPPs