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IEEE Journal of Quantum Electronics

Multiphonon relaxation in laser materials and applications to the design of quantum electronic devices

L. A. Riseberg, Henry W. Moos, William D. Partlow

Published Oct 1, 1968• 18 citations
Publisher

Abstract

An account is given of the results of a recent investigation of multiphonon orbit-lattice relaxation of excited states of rare-earth ions in crystals. The use of these results in the design of quantum electronic devices is discussed, using as examples the Nd3+laser transition and a 10.6-μ infrared quantum counter. A discussion is presented of the infrared limit of quantum electronic devices using these materials. Extension of these concepts to transition-metal ions in crystals is considered and a measurement of1Eto3Emultiphonon decay in Al2O3: V3+is presented.

DOI
10.1109/jqe.1968.1074938

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Journal of Applied Physics•Sep 15, 1997•17 citations
An account is given of the results of a recent investigation of multiphonon orbit-lattice relaxation of excited states of rare-earth ions in crystals. The use of these results in the design of quantum electronic devices is discussed, using as examples the Nd3+laser transition and a 10.6-μ infrared quantum counter. A discussion is presented of the infrared limit of quantum electronic devices using these materials. Extension of these concepts to transition-metal ions in crystals is considered and a measurement of1Eto3Emultiphonon decay in Al2O3: V3+is presented.
Noise arising from strong laser pumping and 77-K internal phonon noise upconversion in the proposed supposedly noiseless 10-μ quantum counters using rare-earth-doped crystals is described. The discussions are specialized to the crystals states of the Eu3+ ion. It is shown that at the pump power (∼50 kW cm−2) necessary for background-limited 10-μ quantum counter upconversion detection at 77 K, all the three major processes of noise generation discussed are insignificant compared to the background thermal (300 K) radiation considered previously in arriving at realistic theoretical quantum efficiencies of the proposed 10-μ quantum counters.
An analysis made in a recent publication indicates that two-photon, Raman, and thermal excitation noise contributions in a 10-μm infrared quantum counter (IRQC) are insignificant compared to that due to the background (300 K) radiation. This conclusion is found to be unwarranted because of several errors in the analysis, foremost of which is an overestimation by 9 orders of magnitude of the transition rate Wα′αbir induced by background radiation. The revised calculation presented here demonstrates that the background radiation, far from being the dominant noise source, is at most comparable in magnitude with the other noise mechanisms.
An analysis of an ideal five-level ir quantum counter (IRQC) is presented. The importance of the two additional levels is discussed and analyzed. The parameters for achieving optimum performance as an ir detector and/or an image converter are presented. In theory, the IRQC is the only quantum amplifier with photon gain that can approach a noise temperature of absolute zero. In practice, with the constriction of available materials and technology, the most feasible use for the IRQC in the near term would be in an active system. An ir laser would be used to scan the target while another laser would pump the excited state transition. The IRQC action has been observed in this laboratory in the tripositive rare earths of Pr, Nd, Eu, Tb, Dy, Er, and Tm. These ions were incorporated in single crystal lattices of CaF(2), BaF(2), SrF(2), CdF(2), LaF(3), CaWO(4), A1(2)O(3), YAG, LaCl(3), and in solutions of the various trichlorides (dissolved in D(2)O). A total of 165 schemes are reported. The rare earth impurity concentration varied from 0.05% to 20%. In our laboratory, the primary range of interest for detection and/or image conversion is between 1 micro and 2 micro. Therefore, almost all the systems studied involved the detection of an ir photon in this region.
Quantum information uses special properties of quantum systems to manipulate or transmit data. This results in new processes, which are impossible to obtain with classical devices. For example, quantum computing and quantum storage, which are two important fields in quantum information research, aim respectively at performing very fast calculations and at storing quantum states of photons. These two applications could be obtained in solid-state systems using rare earth doped crystals. In this context, the most important property of these materials is the long coherence lifetimes of rare earth ion optical and hyperfine transitions. This allows one to create long-lived superposition states, which is a fundamental requirement for efficient quantum computing and storage. Promising results have already been demonstrated in rare earth doped crystals but it will be difficult to improve them with current materials. In this paper, we discuss the general and specific requirements for rare earth ions and crystals in order to perform quantum computing with a large number of quantum bits as well as all solid-state quantum storage. We also present the properties of a few recently studied crystals: Ho3+:YVO4, Ho3+:LuVO4 (quantum computing) and Tm3+:Y3Al5O12 (quantum storage).
Rare-earth ions play an important role in modern technology as optically active elements in solid-state luminescent materials. In many of these materials, interactions between the electronic band states of the host crystal and the rare-earth ion's localized 4f N and 4f N−1 5d states influence the material's optical properties. The importance of these interactions is discussed for material applications in photon-gated hole burning, quantum information and phosphors. Material dependent trends in the relative binding energies of the 4f N states and the host bands have been observed and are summarized. An empirical model for the ion dependence of the 4f electron binding energies is formulated in terms of atomic number and compared with previous models. These models are extended to describe the 4f N−1 5d states with one additional parameter. Improved estimates for the free-ion ionization potentials used in the model are also presented and discussed.
Short pulse laser-induced fluorescence experiments on the lowest-energy electronic states (υ<10−4 cm−1) of trivalent praseodymium ions are reported. Crystals of lanthanum trichloride with a range of Pr3+ concentrations were examined. We compute cross relaxation and upconversion coefficients for the metastable energy levels using a standard rate equation analysis. The limitations of the rate equation approach are examined with a focus on the underlying dynamics of this rare-earth system. The implications of these results for laser emission in the 1.3–7.2 μm spectral range are discussed.