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Applied Physics Letters

Observation of spontaneous emission lifetime change of dye-containing Langmuir–Blodgett films in optical microcavities

M. Suzuki, H. Yokoyama, Stuart D. Brorson, Erich P. Ippen

Published Mar 11, 1991• 81 citations
Publisher

Abstract

We have studied the spontaneous emission properties of Langmuir–Blodgett films containing dye molecules confined in Fabry–Perot microcavity structures having wavelength thickness. The presence of the cavity causes great modifications in the emission spectrum and emission intensity in the direction of the cavity axis. A clear change in spontaneous emission lifetime occurs, which is also attributed to the microcavity effect.

DOI
10.1063/1.104388

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We have studied the spontaneous emission properties of Langmuir–Blodgett films containing dye molecules confined in Fabry–Perot microcavity structures having wavelength thickness. The presence of the cavity causes great modifications in the emission spectrum and emission intensity in the direction of the cavity axis. A clear change in spontaneous emission lifetime occurs, which is also attributed to the microcavity effect.
Optical microcavities are structures which confine light to a small region in the range of one wavelength. The radiation of a quantum emitter is coupled to cavity resonances which leads to an optical confinement of the broadband fluorescence. A practical design for this single-mode microcavity is formed by two silver mirrors enclosing a transparent dielectric medium with single quantum emitters. Steiner et al. have shown that the fluorescence spectra and decay lifetimes of single molecules in this Fabry-Perot type microcavity are strongly dependent on the resonator length.
We used cavity quantum electrodynamic effects to determine the orientation of a species of organic dye molecule located in a microcavity environment. We used the Langmuir-Blodgett technique to fabricate well-controlled multilayer structures into which we incorporated dye molecules with well-defined layer positions. Comparing the results of fluorescence lifetime measurements and radiation patterns with theoretical calculations allowed us to determine both the orientation and the quantum efficiency of the dye molecules.
We present for the first time cavity-controlled fluorescence spectra and decay curves of single dipole emitters interacting at room temperature with the first longitudinal mode of a Fabry-Perot microcavity offering a lambda/2-spacing between its silver mirrors. The spontaneous emission rate of individual dye molecules was found to be enhanced by the Purcell effect by up to three times compared to the rate in free space, in agreement with theoretical predictions. Moreover, our new microcavity design was found to provide long-term stability and single-molecule sensitivity under ambient conditions for several months without noticeable reduction of the cavity-Q value. We consider this as a significant advance for single-photon sources operating at room temperature.
We discuss the frequency dependence of the spontaneous-emission rate (power) in a Fabry-Perot microcavity containing a Lorentz dielectric, with emphasis on modifications of the spectrum under the circumstances of the strong medium-cavity coupling. With the standard-cavity tuning, the total spontaneous-emission power spectrum consists of a multiwave version of the familiar low-frequency vacuum Rabi split peak and a broad structure on the high-frequency side coming from the enhanced spontaneous emission into the continuum of the obliquely propagating waves. This form of the spectrum derives from the properties of the (single-wave) radiation-intensity spectrum of the molecule. Depending on the observation direction, the radiation-intensity spectrum exhibits either a double-peak structure characteristic of the vacuum Rabi splitting, as observed in light transmisssion and reflection experiments, or a single-peak structure describing the enhanced spontaneous emission at the corresponding cavity resonant frequency.
We calculate the spontaneous-emission characteristics of a quantum-well exciton embedded in the center of a planar microcavity and compare them with the emission characteristics in a single-mode cavity with lateral confinement of the electromagnetic field. The results indicate that because the modal structure of a planar microcavity consists of a spectrally dense continuum, the exciton decays into the cavity continuum with a time constant close to the free-space spontaneous-emission lifetime, even under conditions in which its spectrum displays the vacuum Rabi splitting. This behavior contrasts with the case of cavities with lateral in-plane confinement of the field, in which the vacuum Rabi splitting is the signature of a dramatic modification of the spontaneous-emission lifetime. The technological implications of this difference are discussed.
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.