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Journal of Applied Physics

Multiphonon, Raman, and Two-Photon Excitation of Rare-Earth Ions in Crystals: Photon and Phonon Noise in 10-μ Quantum Counters

Francis K. Fong, Marvin M. Miller

Published May 1, 1972• 4 citations
Publisher

Abstract

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.

DOI
10.1063/1.1661527

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Physical review. B, Condensed matter•Sep 1, 1998•58 citations
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 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.
In this paper, we report the first laser-excited optical double-resonance experiments in rare-earth-doped crystals. Infrared upconversion in LaCl3 : Pr3+ and LaF3 : Pr3+ has been achieved by means of a tunable cw dye laser pump. The quantum efficiency of the upconversion process at 2.03 μ in LaCl3 : Pr3+ is 1.2×10−3, which is an improvement of 4×105 over the highest efficiency found previously with incoherent sources. It is shown that an efficiency of 1 can be easily obtained with higher fluxes and improved crystal quality. Direct excitation of the output fluorescence from the 3P0 level is observed in both LaCl3 : Pr3+ and LaF3 : Pr3+ when the dye laser frequency is resonant with the states of the lower-lying 1D2 manifold in the absence of the infrared input. Detailed assignments of the observed double-resonance transitions have been made from wavelength and polarization measurements.
A mechanism for laser cooling of crystals doped with rare-earth ions is proposed. The mechanism involves two-photon Raman scattering through the dipole-allowed 5d ion level, electron–phonon transitions between the Stark-split sublevels, and fluorescence from the excited ion level. It is shown that, under the conditions of coherent pumping, the total population of the ground level is transferred to the excited level of the rare-earth ion, thus increasing the cooling power and accelerating the cooling process. The involvement of dipole-allowed transitions yields an increase in the cooling efficiency by 14% compared to the efficiency of direct pumping at transitions between the 4f levels. Estimations show that the temperature of the sample cooled by the proposed mechanism can reach 82.9 K for current materials with a background absorption coefficient of 4.0×10−4 cm−1.
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.
We study the photon-echo attenuation by various dynamical processes in rare-earth-ion-doped crystals. The experimental investigations concentrate on a Pr3+:Eu3+:Nd3+{\mathrm{Pr}}^{3+}:{\mathrm{Eu}}^{3+}:{\mathrm{Nd}}^{3+}Pr3+:Eu3+:Nd3+ codoped Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ crystal at low temperatures. Two-pulse photon-echo intensities are measured as a function of the pulse intensities when either the Pr3+{\mathrm{Pr}}^{3+}Pr3+ or the Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions are excited. For the quantitative interpretation we consider primarily excitation-induced frequency shifts (EFS) by diagonal and off-diagonal interactions and show that for the systems under consideration EFS are dominated by diagonal interactions. The observed echo attenuation by EFS is compared with the predictions calculated from independent Stark-field measurements and reasonable agreement is obtained. The broadening by spin-ion interactions, by nonequilibrium phonons and the dependence of the echo attenuation on the frequency position in the inhomogeneously broadened band are further investigated.