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Physical Review Letters

Ion Pair Absorption in Pr Cl3

G. H. Dieke, E. Dorman

Published Jul 1, 1963• 25 citations
Publisher

Abstract

One photon was known to be able to excite two Pr/sup 3+/ ions to different levels, one of which was always /sup 3/Po as detected by fluorescence. Using crystals of pure PrCl/sub 3/, 90 absorption lines corresponding to ion pair absorption were detected in the region between 22, 220, and 28,100 cm/sup -1/. Classifications and wave numbers of the lines are given. The lines show no polarization, and most of their frequencies can be written as the sum of two ordinary absorption frequencies. The width of the lines is about 6 cm/sup -1/. (D.C.W.)

DOI
10.1103/physrevlett.11.17

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One photon was known to be able to excite two Pr/sup 3+/ ions to different levels, one of which was always /sup 3/Po as detected by fluorescence. Using crystals of pure PrCl/sub 3/, 90 absorption lines corresponding to ion pair absorption were detected in the region between 22, 220, and 28,100 cm/sup -1/. Classifications and wave numbers of the lines are given. The lines show no polarization, and most of their frequencies can be written as the sum of two ordinary absorption frequencies. The width of the lines is about 6 cm/sup -1/. (D.C.W.)
The absorption of single photons by coupled pairs of ions in rare-earth solids was first observed by Varsanyi and Dieke.1 They noticed that weak absorption of light occurred in PrCl3 at frequencies close to the sum of transition frequencies of individual Pr ions, giving rise to rare-earth fluorescence. This effect was explained by the perturbation theory of Dexter.2 He showed that weak multipole or exchange interactions between rare-earth ions permitted the simultaneous promotion of two ions to excited states by the action of one absorbed photon in an electric dipole allowed transition. Similarly, two ions initially in excited states could emit one sum frequency photon in a cooperative manner.
tion of a single photon by a pair of rare-earth ions in a crystal, acting in cooperation. Neither ion by itself could possibly absorb the photon, since no single-ion state exists at the photon energies involved. Absorption of light occurs discretely at sums of energy-level separations in the two ions and is detected experimentally by the excitation spectrum of one of the emission lines. This is an extremely important new effect which will doubtless have important practical applications in the future as well as obvious scientific implications. It should be emphasized that this is not, in any significant degree, excitation of a molecular state. The basic reason this phenomenon is so unusual is related to the fact that the interaction of radiation with matter consists of a sum of one-electron operators, A Vi, where A is the vector potential. From this point of view, only one electron at a time could possibly be excited, hence only one ion. In this paper a procedure for computing the probability of this effect is outlined, and some of the implications of the associated phenomena are discussed. These views can be found expressed in greater detail in ref. 2.
Time-resolved fluorescence line narrowing is used to study spectral energy transfer in PrF3{\mathrm{F}}_{3}F3​ and PrCl3{\mathrm{Cl}}_{3}Cl3​. The excitation spectrum of PrF3{\mathrm{F}}_{3}F3​ in the region of the ${(^{3}H_{4})}_{1}\ensuremath{\rightarrow}^{3}P_{0}$ absorption indicates that several strong satellite lines accompany the main transition, their origin being ascribed to different Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions lying in strongly perturbed lattice sites. The spectral transfer within the inhomogeneously broadened main transiton is measured, where the energy mismatch is about 2 ${\mathrm{cm}}^{\ensuremath{-}1}$. This process is characterized by a strong ($\ensuremath{\sim}{T}^{4.3}$) dependence of the transfer probability on sample temperature. The growth of the full inhomogeneous emission profile accompanies a uniform decay of the donor line shape. A transfer process between the lowest-energy satellite ions is also measured. Here the energy mismatch is 32 ${\mathrm{cm}}^{\ensuremath{-}1}$ resulting in a weak temperature dependence for the transfer rate. Both the intraline and intersatellite transfer are characterized by simple exponential rate equations. Recent calculations of phonon-assisted transfer probabilities are compared to our measurements, with the intersatellite transfer ascribed to a "one-phonon direct" process whereas the transfer within the main transition occurs by a "one-phonon second-order" mechanism. In PrCl3{\mathrm{Cl}}_{3}Cl3​ the transfer times are faster than the 15-nsec response time of our detection system indicating a much stronger ion-ion coupling.
Two-photon excitation (TPE) spectra of the 4f 1 -?5d 1 transitions of Ce 3 + in LuP0 4 and YP0 4 have been investigated.For Ce3+ in LuP04, transitions to four out of the five 5d 1 levels are observed as zero-phonon lines.The symmetry properties of the levels were obtained from the polarization dependence of the TPE signals.Measurements on Ce 3 + inYP0 4 support the given assignments.Although a crystal-field fit yields a satisfactory RMS energy deviation, an unrealistic value of the spin-orbit coupling parameter, ( 5 d1, is obtained.The • vibronic coupling appears to be smaller than for the single-photon absorption spectra, and the vibronic bands show a rich structure.There are striking differences between the energies and the relative intensities of the vibronic lines and the associated zero-phonon lines.The vibronic coupling is also found to be strongly dependent on the Ce 3 + concentration.78.50.Ec,42.65.-k