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The Journal of Chemical Physics

Oscillator strength determination in LaCl3:Pr3+ by photon upconversion

Jeffrey A. Sell, Francis K. Fong

Published May 15, 1975• 4 citations
Publisher

Abstract

In this paper, we outline a novel method for the determination of oscillator strengths in rare-earth crystals. This method involves the observation of fluorescence resulting from a sequential two-photon excitation process. The rate equations are analyzed and a simple linear relationship between the laser flux, the fluorescent intensity, and the oscillator strength is derived. The equations are applied to LaCl3:Pr3+ and the resulting oscillator strength measured for the 3H6→3P1 transition is found to be in good agreement with the value measured by conventional absorption techniques. One advantage of the present method is the elimination of the need to determine the dopant concentration.

DOI
10.1063/1.430296

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Jun 22, 1988•2 citations
In this paper, we outline a novel method for the determination of oscillator strengths in rare-earth crystals. This method involves the observation of fluorescence resulting from a sequential two-photon excitation process. The rate equations are analyzed and a simple linear relationship between the laser flux, the fluorescent intensity, and the oscillator strength is derived. The equations are applied to LaCl3:Pr3+ and the resulting oscillator strength measured for the 3H6→3P1 transition is found to be in good agreement with the value measured by conventional absorption techniques. One advantage of the present method is the elimination of the need to determine the dopant concentration.
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.
Studies of infrared quantum counter upconversion in LaF3:Pr3+ and LaCl3:Pr3+ have led to the discovery of a process in which a red excitation photon results in the emission of a blue photon. When the 1D2 level of Pr3+ is excited by a cw rhodamine 6-G dye laser, blue fluorescence from the 3P0 level is observed. From the flux dependence and lifetime of the induced fluorescence, we conclude that the observed phenomenon arises from excitation annihilation involving pairs of ions in the 3H6 and the 1D2 states.
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.
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.
Rare-earth-doped laser materials show strong prospects for quantum information storage and processing, as well as for biological imaging, due to their high-Q 4f↔4f optical transitions. However, the inability to optically detect single rare-earth dopants has prevented these materials from reaching their full potential. Here we detect a single photostable Pr3+ ion in yttrium aluminium garnet nanocrystals with high contrast photon antibunching by using optical upconversion of the excited state population of the 4f↔4f optical transition into ultraviolet fluorescence. We also demonstrate on-demand creation of Pr3+ ions in a bulk yttrium aluminium garnet crystal by patterned ion implantation. Finally, we show generation of local nanophotonic structures and cell death due to photochemical effects caused by upconverted ultraviolet fluorescence of praseodymium-doped yttrium aluminium garnet in the surrounding environment. Our study demonstrates versatile use of rare-earth atomic-size ultraviolet emitters for nanoengineering and biotechnological applications. The optical transitions that occur in rare-earth-doped crystals offer promise for quantum information storage and processing. Kolesovet al.report the optical detection of a single praseodymium ion residing in a crystal host by using an excited-state absorption process to enhance its fluorescence yield.
We have used two methods to measure the oscillator strength of the transition between the ground and 17992 cm-1 level in 174Yb. The first technique involves exciting the transition with a laser pulse that is nearly time-bandwidth limited, of uniform intensity, and has a reproducible shape from shot to shot. The population left in the excited state after the pulse varies sinusoidally with a period that depends on the integral over time of the electric field amplitude and the transition oscillator strength. These are the Rabi oscillations that are predicted by application of the Schrodinger equation to the two-level atom. The excited-state population is probed using a two-step photoionization to the continuum. The electric field amplitude is determined from the temporal profile and the intensity of the laser pulse. The second method involves observation of the polarization rotation of a set of degenerate sublevels brought about by a time-bandwidth limited light-shift laser. One sublevel (mj = 0) of the J = 1 level at 17992 cm-1 is populated by a linearly polarized laser. A second copropagating light-shift laser, which is linearly polarized at an angle to the first laser, is tuned between 7.5 and 30 GHz off-resonance with the transition. The light-shift laser causes population to be promoted into the mi = ±1 levels by a virtual transition through the ground J = 0, = 0 level. Two linearly polarized photoionizing lasers photoionize the population only from the mi = ±1 levels. The photoion signal oscillates sinusoidally with a period that depends only on the integrated pulse intensity, the laser detuning, and the transition oscillator strength.