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Optics Express

Introduction

Charles M. Bowden, Mark J. Bloemer

Published Sep 15, 1997• 1 citation
Publisher

Abstract

Local field effects that occur due to dipole-dipole interactions have been vigorously investigated since the initial works of Lorentz[1] and Lorenz[2]. Linear interactions of light in condensed matter and dense gases are manifest in the Clausius-Mossotti relations[3], and nonlinear effects have been known for some time[4]. Generalized Maxwell-Bloch formulation incorporating local field effects[5, 6] has stimulated considerable theoretical development and predictions, but to date few experiments have been performed. Several experiments, however, have addressed key issues stemming from various theoretical developments. Boyd and coworkers have observed local field induced spectral red shifts in rubidium vapor[7], and Rand and coworkers have observed intrinsic bistability due to local field effects in a crystal lattice highly doped with rare earth ions[8]. Most recently, Eliel and coworkers have studied local field effects in very high density metal vapors[9], and find novel cooperative effects and excitation dependent line narrowing. The papers presented in this Focus Issue are indicative of the currently increasing interest and activity in this field.

DOI
10.1364/oe.1.000133

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Local field effects that occur due to dipole-dipole interactions have been vigorously investigated since the initial works of Lorentz[1] and Lorenz[2]. Linear interactions of light in condensed matter and dense gases are manifest in the Clausius-Mossotti relations[3], and nonlinear effects have been known for some time[4]. Generalized Maxwell-Bloch formulation incorporating local field effects[5, 6] has stimulated considerable theoretical development and predictions, but to date few experiments have been performed. Several experiments, however, have addressed key issues stemming from various theoretical developments. Boyd and coworkers have observed local field induced spectral red shifts in rubidium vapor[7], and Rand and coworkers have observed intrinsic bistability due to local field effects in a crystal lattice highly doped with rare earth ions[8]. Most recently, Eliel and coworkers have studied local field effects in very high density metal vapors[9], and find novel cooperative effects and excitation dependent line narrowing. The papers presented in this Focus Issue are indicative of the currently increasing interest and activity in this field.
It is well known that dense materials with local-field effects can show "intrinsic" optical bistability when they are directly irradiated by a light beam. This has been shown theoretically in a number of works and also experimentally in several cases, in gas media and also in doped solid-state materials where nonlinearities based on standard local-field effects can be reinforced with other ion interaction effects. Although from the point of view of applications nonlinearities stronger than those found so far would be desirable, the fact that no optical resonator is needed to achieve bistability makes these materials potentially interesting for applications in optical information storage and processing.
This thesis reports experiments and theory on intrinsic mirrorless bistability in the luminescence of ytterbium-doped crystals and glasses. The main results are the observation of intrinsically bistable luminescence at room temperature and chromatic switching at low temperature, reported here for the first time. The nonlinear dynamics responsible for these optical phenomena are shown to arise from ion-ion interactions controlled by the application of resonant electromagnetic fields. On the theoretical side, the classical Lorentz local field correction is shown to be the lowest order term of radiation-driven correlation contributions to local polarization which arise from inter-ion coherences and cooperative relaxation and frequency shifts beyond the dynamic shift are predicted. The nonlinear Maxwell-Bloch equations are extended to describe energy transfer between different species of ions predicting bistability in excited state populations which then emit bistable luminescence as a consequence, and an intensity dependent transfer rate is predicted. Diffusive excitation migration in space is also explored as a possible mechanism for generating multiple instabilities, but is not predicted to give rise to hysteresis loops by itself. On the experimental side, original observations of intrinsic optical switching and hysteresis are reported in the luminescence of Yb:CsCdBr 3 and Yb, Tm:glass. Evidence of cross-coupling between different impurities is also presented, together with spectroscopic details of intrinsic chromatic switching between different luminescent transitions of the acceptor species in Yb, Er:CsCdBr3 excited at the infrared Yb resonance wavelength. Conclusive spectroscopic evidence that excludes thermal effects as responsible for low temperature intrinsic switching is also presented. Room temperature intrinsic optical switching and hysteresis are reported for the first time in bulk Yb,Tm:glass samples. Switching, hysteresis, and clamping of laser output from waveguide channels fabricated in the glass material are also reported and indicate fundamental design limitations for compact optical amplifiers and oscillators.
Solids containing rare earth (RE) ions have attracted spectroscopists' attention since the beginning of this century.In the last 30 years, their extremely narrow spectral features in combination with the use of non linear spectroscopy have served to sensitively measure ion-solid interactions and to progressively observe narrower homogeneous linewidths.The potential for using RE ion doped crystals as optical storage materials and processors has lately been a driving force in their investigations, Here, the ratio of inhomogeneous to homogeneous linewidth is regarded as an adequate measure of storage density and can become as big as 10 7 at cryogenic temperatures.Therefore, the analysis of line broadening is of fundamental as well as applied interest.This work is concerned with the investigation of interactions of RE ions with their environment.By means of a laser with a kilohertz resolution and non-linear spectroscopy, spectral dynamics as a function of intrinsic, external electric field, or light-pulse induced perturbations are analyzed on different time scales.In the first part, the theoretical background for the spectroscopy of RE ion doped crystals is outlined.The energy levels are presented and it is shown that due to their electronic properties RE ions have spectrally narrow electronic transitions, sometimes in the sub-kHz regime.The investigations of these narrow spectral features on the seconds to minutes time scale require very stable tunable laser sources.At present, such devices are not commercially available.In the second part, the performance of ahorne built laser system is characterized using persistent spectral holes, The results show that frequency selective materials can be used as powerful tools for the high resolution Vlll Abstract spectral analysis of laser sources.Complementary to that, they give a measure for the long term evolution of the spectral holes for the particular hole burning substance.In the third part, the effect of an external electric field on RE ion doped crystals is investigated.It is shown that for these systems the electric field induced frequency shifts are fully reversible.A general theory of Stark splittings of RE doped crystals is introduced and two methods are presented which allow for the determination of the magnitude and orientation of the electric dipole moment differences with sub-degree accuracy.Finally in the last part, spectral line broadening mechanisms of RE ion doped crystals are discussed and investigated by means of two-pulse photon echoes.Through variation of the experimental parameters, a discrimination between the different contributions is partly achieved and characteristic properties for different dephasing mechanisms are presented.In combination with the measurements from the third part, quantitative predictions of the electric dipole-dipole induced broadening are carried out, which are compared to the experimental results,