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Physical review. B, Solid state

Probabilistic Treatment of Stepwise Energy Transfer and Infrared-to-Visible Conversion

H. J. Richter, R. KENT WATTS

Published Jan 15, 1972• 4 citations
Publisher

Abstract

A probabilistic model for the two-photon process of infrared-to-visible light conversion by ${\mathrm{Yb}}^{3+}$-${\mathrm{Tm}}^{3+}$ or similar rare-earth ion systems in solids is considere. The model demonstrates the basic influence of the infrared pump power and the lifetime of the intermediate excited state on the conversion efficiency.

DOI
10.1103/physrevb.5.320

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A probabilistic model for the two-photon process of infrared-to-visible light conversion by Yb3+{\mathrm{Yb}}^{3+}Yb3+-Tm3+{\mathrm{Tm}}^{3+}Tm3+ or similar rare-earth ion systems in solids is considere. The model demonstrates the basic influence of the infrared pump power and the lifetime of the intermediate excited state on the conversion efficiency.
New efficient mechanisms of long-wavelength excitation of short-wavelength luminescence in a system of rare-earth impurity ions are proposed. The model studied involves a multilevel system of electronic states of a rare-earth ion interacting with the long-wavelength emission that is in resonance with one or several transitions between the excited levels. The concentration of impurity ions is assumed to be sufficiently high, so that the interionic cross-relaxation and the up-conversion play a significant role. Moreover, the model includes processes similar to photon avalanche, in which the photoinduced excitation of a single ion is converted into lower-level excitations of several ions, each of them reentering the process after photon absorption. Numerical solutions of the system of balance equations for a multilevel system are obtained with calculated and semiempirical parameters of self-quenching and up-conversion. It is shown that, in a system of Tm 3+ impurity ions, short-wavelength luminescence at λ≥0.29 μm can be efficiently excited by radiation at λ≅1.11 or 0.649 μm with a moderate intensity.
We have made an unexpected discovery of highly nonlinear optical behavior in certain praseodymium-doped lanthanum halides. When a LaCl3 or LaBr3 crystal containing Pr3+ ions is exposed to green laser radiation slightly in excess of a certain critical intensity, Pr fluorescence increases by orders of magnitude. Infrared output near 4.5-μm wavelength is associated with the large visible output, and pump power is strongly absorbed. We call this new phenomenon a photon avalanche. Critical pump power density is in the 1–15 W/cm2 range. At higher pump rates, a population inversion and lasing action take place between the lowest infrared levels of the Pr ion. Experimental results are presented and compared to predictions of a photon avalanche model based on resonant energy transfer.
We report on experimental verification of the proposed energy transfer mechanism responsible for photoluminescence of rare earth ions in semiconductors. Using two-color optical spectroscopy in the visible and the mid-infrared region, we demonstrate reversal of the most important step in the excitation process. This “back-transfer ” effect was supported experimentally only in an indirect manner by measurements on thermal quenching of PL intensity and lifetime. In the current study on InP:Yb, formation of the intermediate state bridging atomic states of the RE ion and extended orbitals of a semiconducting host is explicitly confirmed and its characteristic energy spectroscopically determined. This finding will allow optimization of the efficiency of semiconductor:RE systems for applications.