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Physical Review Letters

Site-Selective, Intrinsically Bistable Luminescence of Yb3+ Ion Pairs in CsCdBr3

Markus P. Hehlen, Amos Kuditcher, Stephen Colby Rand, Stefan R. Lüthi

Published Apr 12, 1999• 81 citations
Publisher

Abstract

We report the first observation of intrinsic optical bistability in ${\mathrm{CsCdBr}}_{3}:1%$ ${\mathrm{Yb}}^{3+}$ and show, using site-selective spectroscopy, that only the asymmetric, strongly coupled ${\mathrm{Yb}}^{3+}$ ion-pair minority site gives rise to hysteresis of near-infrared and cooperative up-conversion luminescence as a function of incident laser intensity below 15 K.

DOI
10.1103/physrevlett.82.3050

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We report the first observation of intrinsic optical bistability in CsCdBr3:1{\mathrm{CsCdBr}}_{3}:1%CsCdBr3​:1 Yb3+{\mathrm{Yb}}^{3+}Yb3+ and show, using site-selective spectroscopy, that only the asymmetric, strongly coupled Yb3+{\mathrm{Yb}}^{3+}Yb3+ ion-pair minority site gives rise to hysteresis of near-infrared and cooperative up-conversion luminescence as a function of incident laser intensity below 15 K.
In single crystals of the dimer compound Cs3Y2Br9:10% Yb3+ below 31 K, both visible (VIS) and near-infrared (NIR) luminescence intensities were found to exhibit hysteresis as a function of incident NIR intensity and temperature. The optical bistability is intrinsic to Cs3Y2Br9:10% Yb3+ and not a result of an external feedback. Lowering the temperature to 11 K strongly enhances the all-optical switching behavior. The switching on VIS cooperative upconversion and NIR luminescence transitions occurs simultaneously and with opposite polarity reflecting the competition of both emission processes. On/Off switching ratios of up to 4.8 and 1.7 were observed for VIS and NIR luminescence intensities. Using NIR luminescence spectroscopy, differences in the internal sample temperature of up to 7 K were found between the upper and lower branches of the hystereses. A two-level density-matrix model is developed which includes ground- and excited-state interactions and shows that the intrinsic bistability due to a local field different from the external field is strongly amplified by the nonlinear cooperative upconversion process. Alternatively, a rate-equation model is presented which takes the multilevel nature of the ions into account but is more phenomenological in nature. Formally, the two models are shown to be equivalent, and they qualitatively explain all major experimental observations. It is found both theoretically and experimentally that increasing the coupling within Yb3+ dimers and/or decreasing energy migration through the Yb3+ lattice enhances switching and renders it easier to observe intrinsic optical bistability.
Optical bistability is a well-known phenomenon in optical systems of many kinds. However observations of intrinsic bistability are rare and have not been reported previously in rare earth systems for nonlinear dynamics due to inter-atom coupling which arises at high impurity concentrations. Typically, nonlinear response by this mechanism is too weak to give rise to sizeable nonlinearities. Here we present observations of cooperative upconversion emission from crystals of Yb3+ Cs3Y2Br4 at low temperatures however, in which hysteresis without mirrors provides evidence of strong cooperative nonlinear response.
We present a mechanism able to show intrinsic bistable behaviour involving single Yb3+ ions embedded into bromide lattices, in which intrinsic optical bistability (IOB) has been observed. The mechanism is based on the experimentally found coupling between the Yb3+ ion and the totally symmetric local mode of vibration of the [YbBr6]3- coordination unit. The model reproduces the IOB observed in CsCdBr3:1% Yb3+ and allows to understand the experimentally found presence of the phenomenon in the other bromides, but its absence in Cs3Lu2Cl9:Yb3+.
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.
Materials displaying intrinsic optical bistability (IOB), i.e., allowing the coexistence of two stable steady-state excitation rates for a single given excitation power, are of interest for potential technological applications related to optical data switching and manipulation. The properties of the unusual IOB previously observed in Yb 3+ -doped Cs 3 Lu 2 Br 9 and CsCdBr 3 host materials are studied here using absorption and luminescence spectroscopies. The IOB phenomenon is concluded to derive ultimately from laser heating effects. When combined with a strongly increasing and nonlinear dependence of the material's absorbance on internal temperature, laser heating leads to a positive-feedback absorption amplification process showing a hysteresis in both power- and temperature-sweep experiments. A simple model describing this effect in terms of rates of sample heating and cooling in the irradiated volume reproduces the power, temperature, concentration, and excitation-energy dependence of the Yb 3+ IOB using only the experimental absorption data as input. The temperature dependence of the absorption cross section is correlated with thermal changes in the monomeric YbBr 6 3- geometry, which becomes more asymmetric as the temperature is elevated. The IOB observed in Yb 3+ -doped Cs 3 Lu 2 Br 9 and CsCdBr 3 host lattices is therefore a property of the monomeric Yb 3+ ion in these materials, and not a dimer property as was previously believed. These results also emphasize the more general conclusion that laser heating may contribute significantly to the shape or slope of an excitation power dependence curve, and may even be the dominant aspect of that curve when absorption cross sections are strongly dependent on temperature.