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Applied Physics Letters

The photon avalanche: A new phenomenon in Pr3+-based infrared quantum counters

Jay S. Chivian, William E. Case, Dayton D. Eden

Published Jul 15, 1979• 421 citations
Publisher

Abstract

Studies of laser-pumped Pr3+ infrared quantum counters have led to the discovery of a new photon avalanche region, occurring when pump flux exceeds a certain critical value. Infrared output near 4.5 μm is associated with the large visible output, and pump power is strongly absorbed. Critical pump power density is in the range 1.2–12.2 W/cm2.

DOI
10.1063/1.91044

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Studies of laser-pumped Pr3+ infrared quantum counters have led to the discovery of a new photon avalanche region, occurring when pump flux exceeds a certain critical value. Infrared output near 4.5 μm is associated with the large visible output, and pump power is strongly absorbed. Critical pump power density is in the range 1.2–12.2 W/cm2.
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 an investigation of a nonlinear optical absorption phenomenon observed in LaCl3 crystals doped with Pr. When these crystals are illuminated with a laser beam of 529 nm wavelength and intensity in excess of a certain critical value, the light is strongly absorbed. The laser radiation is resonant with a Pr3+ transition from the first excited state (3H5) to a high optical state (3P1), and absorption is accompanied by strong fluorescence output from 3p1 and 3p0 to several lower-lying levels. Since the resonant transition does not include the ground state, it is not expected a priori that any absorption should occur (see Fig. 1). This is an example of the so-called photon avalanche phenomenon1.
We present a new infrared (IR) detection scheme based on the infrared quantum counter (IRQC) detector and utilizing the photon avalanche process. At the time of its discovery, the phenomenon of photon avalanche was considered a limitation rather than an advantage for the development of IRQC. Both the experimental results and the numerical modeling presented demonstrate that the process responsible for photon avalanche can be used to enhance the detection of an IR signal. A new room-temperature IR detection scheme is proposed on the basis of the results of this research. The novel detection scheme presented demonstrates an increase in detectivity and a decrease in the noise-equivalent power when compared with the IRQC schemes previously discussed in the literature.
High resolution spectroscopy of quantum systems is a key point in the quantum information field. Rare earth ions in crystals are interesting candidates for this application because of the long coherence lifetime of some of their transitions. These ions can also be manipulated by optical excitation which has, however, to be produced by ultra-stable laser sources. This proves to be a very difficult task in the case of dye lasers which are necessary to excite Pr3+ doped crystals and especially Pr3+:Y2SiO5. This compound is by far the most used host in rare earth based quantum information studies. In this paper, we discuss the use of Pr3+,Yb3+ codoped materials to build an infrared pumped solid state laser suitable to excite Pr3+:Y2SiO5 around 606 nm. We show by the analysis of a rate equation model that avalanche upconversion is not very efficient to obtain a high power laser. This is more easily obtained if a second laser is set to pump resonantly Yb3+ ions. The spectroscopic properties of a new matrix Pr3+,Yb3+:PbF2 are also investigated. We found that this compound emits at 606.18 nm with a width of 5 nm and would be therefore suitable to excite Pr3+:Y2SiO5. Moreover, it can be excited at 857 nm and 975 nm, i.e. in the range of high power laser diodes.
The phenomenon of photon avalanche, which involves both an excited state absorption process from a metastable level and a cross relaxation energy transfer process responsible for the large increases in population of this metastable level, has been investigated in LaCl3:Pr3+.{\mathrm{LaCl}}_{3}:{\mathrm{Pr}}^{3+}.LaCl3​:Pr3+. In this paper, we report on the intensity dependence of both the steady-state fluorescence and the temporal evolution of the avalanche signal as a function of temperature (80 K to room temperature). Comparisons are made between experimental results and mathematical models based on a six-level system described by a series of coupled rate equations combined with the propagation of a Gaussian beam. We develop a model with only one adjustable parameter, the excited state absorption cross section, which provides a good description of all of our experimental data. We have estimated values of the excited state absorption cross section for the various ${}^{3}{\stackrel{\ensuremath{\rightarrow}}{{\mathrm{H}}_{5}}}^{3}{\mathrm{P}}_{0}$ pumping transitions at different temperatures.
Laser output at 4.9 μm has been obtained from a Pr doped LaCl3 crystal. Pump laser energy at 529 nm is coupled into the crystal via the photon avalanche process. This process involves metastable state ion absorption of a pump photon and subsequent ion‐ion energy transfer. The latter step generates two metastable state ions (self‐induced absorption). This highly nonlinear process is characterized by a sharp onset with pump intensity and, at higher intensities, depopulation of the ionic ground state. Experimental results will be compared with predictions from an existing rate equation model.