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Journal of Luminescence

Intrinsic thermo-optical feedback as a fundamental nonlinear interaction in rare-earth-doped systems

Rodrigo F. Silva, José dos Santos, Emanuel Pinheiro Santos, Daniel F. Luz, Célio V. T. Maciel, Gabriela Soares, Carlos Jacinto, André L. Moura

Published Aug 29, 2026• 0 citations
Publisher

Abstract

Intrinsic heating is generally regarded as a secondary consequence of optical excitation in rare-earth (RE$^{3+}$)-doped materials. Here, we demonstrate that intrinsic thermo-optical feedback can drive the transient dynamics of optically excited RE$^{3+}$ systems. To isolate this mechanism, we develop a minimal coupled population-temperature model that describes the interplay among optical excitation, temperature-dependent non-radiative relaxation, heat generation, and thermal dissipation. The model predicts the emergence of a threshold excitation power associated with intrinsic thermo-optical feedback, giving rise to pronounced slowing down of the transient dynamics, non-monotonic evolution of the characteristic transient time, population overshoot, and accelerated relaxation above threshold. These phenomena originate from the progressive establishment of a positive feedback loop linking temperature, non-radiative relaxation, quantum efficiency, and heat generation. Our results demonstrate that temperature should no longer be regarded merely as a passive external parameter, but rather as an active dynamical variable capable of continuously reshaping the relaxation pathways of the system. More broadly, this work establishes intrinsic thermo-optical feedback as a general framework for understanding nonlinear transient phenomena in optically excited RE$^{3+}$ materials and provides a complementary perspective for interpreting threshold-like optical responses beyond conventional photon-avalanche mechanisms.

DOI
10.1016/j.jlumin.2026.122137

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Intrinsic heating is generally regarded as a secondary consequence of optical excitation in rare-earth (RE3+^{3+}3+)-doped materials. Here, we demonstrate that intrinsic thermo-optical feedback can drive the transient dynamics of optically excited RE3+^{3+}3+ systems. To isolate this mechanism, we develop a minimal coupled population-temperature model that describes the interplay among optical excitation, temperature-dependent non-radiative relaxation, heat generation, and thermal dissipation. The model predicts the emergence of a threshold excitation power associated with intrinsic thermo-optical feedback, giving rise to pronounced slowing down of the transient dynamics, non-monotonic evolution of the characteristic transient time, population overshoot, and accelerated relaxation above threshold. These phenomena originate from the progressive establishment of a positive feedback loop linking temperature, non-radiative relaxation, quantum efficiency, and heat generation. Our results demonstrate that temperature should no longer be regarded merely as a passive external parameter, but rather as an active dynamical variable capable of continuously reshaping the relaxation pathways of the system. More broadly, this work establishes intrinsic thermo-optical feedback as a general framework for understanding nonlinear transient phenomena in optically excited RE3+^{3+}3+ materials and provides a complementary perspective for interpreting threshold-like optical responses beyond conventional photon-avalanche mechanisms.
Optically bistable materials promise technological advances in optical information processing, memristive devices, and multiparametric sensing. However, optical bistability is predominantly observed under cryogenic conditions or is governed by subtle thermo-optical nonlinearities. Here, we report on Ho3+-activated nanocrystals that exhibit cavity-free intrinsic optical bistability (IOB) at ambient conditions. Non-thermal IOB stems from a cross-coupled photon avalanche (XPA) mechanism enabled by a low-phonon-energy double-perovskite host, which reduces nonradiative losses and facilitates excited-state population via XPA, even when the pump intensity is below threshold. Time-resolved luminescence measurements support the proposed XPA, as evidenced by a double-rise profile consistent with two reservoir states interlocked in energy looping. IOB with high-contrast photoswitching (up to 46 dB) is observed at room temperature across multiple visible emission lines, enabling wavelength-division multiplexing and compatibility with common detectors. IOB is preserved across nano- to microscale crystals and different double-perovskite compositions, broadly enabling information photonics and advanced sensing.
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.
This paper presents theoretical investigations on the dynamics of intrinsic optical bistability (IOB) in Tm3+/Yb3+ codoped systems with an upconversion avalanche mechanism. Numerical simulations based on the rate equation model demonstrate distinct IOB hysteresis and critical slowing dynamics around the avalanche thresholds. Moreover, the unusual IOB characteristics are well interpreted by developing a simplified analytic model which gives the formulations of two critical thresholds and the necessary condition for IOB to occur. The simplified model shows that such IOB phenomena may occur only if the total quantum yields of the dipole–dipole energy transfer processes are much higher than that of the inherent decay losses involved in an upconversion avalanche. The analytic model developed in the paper may be useful for the prediction of new rare-earth-doped materials giving rise to IOB.
Intrinsic optical bistability and dynamic hysteresis phenomenon, induced by nonlinear excitation and energy level coupling, are predicted theoretically in single Tm-doped laser crystal pumped at 648nm avalanche wavelength. Taking into account the dominant energy transfer processes including excited state absorption, cross relaxation, energy transfer up-conversion and decay of the metastable level Tm3+ 3F4, the analytical formula of avalanche threshold condition are deduced in the steady-state approximation. Based on the theory of microscopic coupled rate equations, intrinsic optical bistability and influence of system parameters on hysteresis loop are studied numerically in detail by using a four-order Runge-Kutta technique. The numerical results predict that intrinsic optical bistability of near 2 micrometer fluorescence emission relevant to Tm 3F4→3H6 transition is achievable experimentally in single Tm-doped laser crystal. For realization of low threshold optical bistability and notable bistable hysteresis loop, it is beneficial to properly increase Tm3+-doped concentration and suppress energy transfer up-conversion. Furthermore, the interesting results obtained numerically show that laser-induced thermal effect is not the indispensable factor for occurrences of intrinsic optical bistability in rear-earth-doped crystal. Cooperation of nonliear excitation and energy level coupling can essentially lead to intrinsic optical bistability in rear-earth-doped system.
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.