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Physical Review B

Förster transfer and the local optical density of states in erbium-doped silica

M. J. A. de Dood, Jasper Knoester, A. Tip, Albert Polman

Published Mar 4, 2005• 109 citations
Publisher

Abstract

Optically excited erbium ions incorporated near the surface of a silica glass decay by spontaneous emission and---at high Er concentration---via F\"orster energy transfer to quenching sites. By externally modifying the photonic microstructure we vary the local optical density of states (LDOS) in samples with different degrees of F\"orster transfer. Changes in spontaneous emission rate are consistent with calculated variations in LDOS at $1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$, while F\"orster energy transfer is not affected by the LDOS. The latter is attributed to the fact that F\"orster transfer involves virtual photons with a broad energy spectrum, excluding a special role for the LDOS at the atom's transition frequency.

DOI
10.1103/physrevb.71.115102

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Optically excited erbium ions incorporated near the surface of a silica glass decay by spontaneous emission and---at high Er concentration---via F"orster energy transfer to quenching sites. By externally modifying the photonic microstructure we vary the local optical density of states (LDOS) in samples with different degrees of F"orster transfer. Changes in spontaneous emission rate are consistent with calculated variations in LDOS at 1.5\ensuremathμm1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}1.5\ensuremathμm, while F"orster energy transfer is not affected by the LDOS. The latter is attributed to the fact that F"orster transfer involves virtual photons with a broad energy spectrum, excluding a special role for the LDOS at the atom's transition frequency.
Spherical SiO2 colloids with two different diameters (175 nm, 340 nm) were doped with erbium at different concentrations. The spheres show sharply peaked photoluminescence centered at 1.535 μm, due to intra-4f transitions in Er3+. From measurements of the Er decay rate for different Er concentrations the decay rate of isolated Er ions (i.e., in absence of concentration quenching) was determined for the two colloid diameters. The data were compared to spontaneous emission rates derived from calculations of the local optical density of states in the colloids. The calculation predicts a large difference in the spontaneous emission rate for both colloid sizes (61 vs 40 s−1), in perfect agreement with the measured data.
Erbium is a rare-earth metal that, when incorporated in a solid, can emit light at a wavelength of 1.5 μm. It plays a key role in current day telecommunication technology as the principle ingredient of optical fiber amplifiers. In this thesis the control of the Er spontaneous emission in three different types of microphotonic materials is described. Part I of this thesis focuses on the effect of a metallo-dielectric interface on the spontaneous emission of optical emitters in silica glass. It is shown that Er ions near a Ag interface can couple to surface plasmons (SPs) via a near-field interaction. By coupling SPs out into the far field, large changes in the Er photoluminescence emission distribution, spectra, and polarization can be observed. The excitation of SPs also results in an increase of the Er photoluminescence decay rate. The observed decay rates are in good agreement with calculations based on a classical dipole oscillator model. From the change in photoluminescence decay rate of Si nanocrystals near a Ag interface it is shown that Si nanocrystals can efficiently excite SPs and have an internal quantum efficiency of 77 %. Part II focuses on the effect of a microcavity on the spontaneous emission of Er and describes how ion implantation can be used to dope dielectric microresonators with optically active Er ions. The fabrication and characterization of an Er ion-implanted silica microsphere resonator is described that shows lasing at 1.5 μm when pumped above its lasing threshold. Ion implantation is also used to dope toroidal microcavities on a Si chip with Er. The microtoroids are doped by either pre-implantation into the SiO2 base material, or by post-implantation in a fully fabricated microtoroid. The optical activation of Er ions in the microtoroid is investigated and Er lasing at 1.5 μm is observed for both types of microcavities with the lowest threshold (4.5 μW) for the pre-implanted microtoroids. Part III describes the fabrication of an Er-doped Si-inverse opal photonic crystal. These photonic crystals can potentially have a photonic bandgap that can fully inhibit the spontaneous emission of on optical emitter. Fabrication criteria are derived for such a photonic crystal, based on the lattice parameter, filling fraction, and Si refractive index. In the opal photonic crystal composed of both Si and SiO2 we show that Er ions can be selectively excited in both the Si and SiO2 part of the photonic crystal by changing the excitation wavelength and/or the measurement temperature.
Local radiative density of optical states (LDOS) offers a tool to control the radiative rate of spontaneous emission from molecules, atoms, and quantum dots, which is proportional to LDOS. This paper presents that LDOS how to make the population of excited-state decay exponentially in time, and how these dynamics can be affected. By adopting the plane-wave expansion method, properties of an inverse-opal photonic crystal are studied with the help of photonic dispersion relations. Results in this paper show that the LDOS is radically modified in photonic crystal, and the rate of spontaneous emission can be described by the functions of position in the crystal and orientation of transition dipole moment.
Erbium implanted sodalime silicate glass was covered with a range of transparent liquids. The spontaneous emission rate of Er3+{\mathrm{Er}}^{3+}Er3+ around 1.54 $\ensuremath{\mu}$m shows clear changes depending on the liquid refractive index and Er depth. A rigorous quantum mechanical calculation shows that the effect of the interface on the spontaneous emission rate is fully described by the classical density of optical modes as a function of distance from the interface. The data provide the first direct determination of the radiative transition rate $(45{s}^{\ensuremath{-}1})$ at 1.54 $\ensuremath{\mu}$m of Er3+{\mathrm{Er}}^{3+}Er3+ which is widely used in optical amplifiers.
In order to discriminate between the two macroscopic models for the dependence of the spontaneous emission rates of emitters on the refractive indices of the surrounding optical dielectric media, i.e., the local-field effect, Eu3+ activated glass samples with a range of different refractive indices were prepared for the measurements of photoluminescence emission spectrum, luminescent decay rate and refractive index. Detail analyses indicate that the local-field effect on the spontaneous emission rates follows the virtual-cavity model derived by assuming the doped luminescent ions do not disturb the optical dielectric media.
Since the advent of vertical cavity surface-emitting lasers, a renewed interest has also emerged for the spontaneous emission from Fabry-Pérot microcavities. Changes in spontaneous emission characteristics in a 1D microcavity were predicted long ago,1 but have been demonstrated only recently in the optical domain for solid-state, e.g. semiconductor, structures where changes in spectral purity, lifetime, and emission intensity were observed.2 However, the interpretation of these effects is somewhat obscure, because these structures are highly absorbing and often involve band-to-band, rather than atomic, transitions. In the present study, we use optically transparent Si/SiO2 cavities, consisting of two coplanar Si/SiO2 distributed Bragg reflectors (DBR) around a (λ/2) SiO2 active region, which was doped with ~0.2 at.% Er3+ ions through MeV ion implantation. The Er3+ ions in SiO2 exhibit a sharp, atomic-like, intra-4f transition around λem=1.54 μm, which is effectively shielded by the outerlying filled 5s2 and 5p6 shells. Recently, we reported on the considerable enhancement of the spontaneous emission intensity out of such an Er-doped microcavity.3 In this paper, we present a more detailed study of the modified spontaneous emission, including fluorescence decay measurements to study the effect of the cavity on the spontaneous emission rate.