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Journal de physique

Double excitation of Nd3+ pairs in LaF3 by two step and double quantum processes

R. Buisson, J.Q. Liu, Jean‐Claude Vial

Published Jan 1, 1984• 22 citations
Publisher

Abstract

Using the energy level shift induced by a Nd3+ ion on a neighbour ion, the selective excitation of a class of (Nd, Nd) pairs is possible in weakly doped samples with a spectrally narrow laser. The observation of an anti-Stokes fluorescence shows that a pair can absorb two photons. From experiments with a magnetic field, it is shown that using a single laser, the double excitation of moderatly coupled pairs is essentially induced by a double quantum process by which two photons are simultaneously absorbed. The strongly coupled pairs, on the contrary, can only be doubly excited by two lasers of different frequencies. Orders of magnitude of the coupling strength between the two ions are deduced from the difference between these frequencies.

DOI
10.1051/jphys:019840045090153300

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•Apr 26, 1987•0 citations
Using the energy level shift induced by a Nd3+ ion on a neighbour ion, the selective excitation of a class of (Nd, Nd) pairs is possible in weakly doped samples with a spectrally narrow laser. The observation of an anti-Stokes fluorescence shows that a pair can absorb two photons. From experiments with a magnetic field, it is shown that using a single laser, the double excitation of moderatly coupled pairs is essentially induced by a double quantum process by which two photons are simultaneously absorbed. The strongly coupled pairs, on the contrary, can only be doubly excited by two lasers of different frequencies. Orders of magnitude of the coupling strength between the two ions are deduced from the difference between these frequencies.
This paper shows that the satellite lines that appear in the absorption and fluorescence spectra of neodymium ions in a LaF3 crystal at concentrations of about 0.5 at.% and the accompanying lines of the isolated ion are caused by pairwise interaction of the Nd3+ ions. Double optical resonance is used to study the structure of the satellite lines in the neighborhood of the 4I9/2→4G5/2 transition of the isolated ion (wavelength 5777.1 Å), hidden by inhomogeneous broadening. When neodymium ion pairs are excited by resonance laser radiation, the presence of anti-Stokes components is recorded in the fluorescence spectrum (up-conversion). It is shown that the main up-conversion mechanism is cumulative pair excitation. These results are convincing evidence that the suppression of absorption from excited levels can be experimentally observed in condensed media.
When the coupling between two ions associated in pair exceeds a given value, the excitation of both ions of the pair is impossible when using a single narrow laser. This double excitation was obtained with two lasers of different wavelengths. A narrowing of the inhomogeneous broadened lines is observed which gives information on the strain field in the crystal. From the difference between the wavelengths, the order of magnitude of the coupling is deduced and compared with phonon assisted transfer rates.
Up to now, only quantum computing using few quantum bits have been realized [1]. Main obstacles to increase the size of quantum register are fast decoherence and difficulties to control many-qubits entanglement. The clusters of the Nd3+ions formed in the Nd3+:LaF3crystal can be a candidate for many-qubit CNOT-gate, because of their entangled states due to strong coherent interaction (Davydov's splitting; bright and dark states with their own lifetimes τ and ra), weak electron-phonon coupling and long coherence time of the excited states. It was shown earlier that satellite lines of the main spectral line for single-site optical center of absorption [2, 3] and fluorescence excitation spectra [2] of Nd3+:LaF3crystals can be attributed to Nd3+ion pairs. The direct measurement of the fluorescence decay times for various classes of Nd3+pairs was made [2] since the pairs are well selected by fluorescence excitation wavelength.
We consider the possible physical processes that may arise in a three-level atom when only two of its levels interact with a strong electromagnetic field and when the atomic transition frequency is nearly equal to once and twice the frequency of the laser field, respectively. There have been found pronounced cooperative effects in the spectrum of the two-level system, which is in resonance with the laser field, arising from the presence of the third level. The excitation spectra describing the transitions from the first excited state into the second excited state and from that to the ground state consist, apart from the two central peaks, of two pairs of sidebands which are induced by the laser field of the neighbouring system. Detailed expressions of the spectral functions for the physical processes of one- and two-photon resonance fluorescence have been derived and discussed in the limit of high photon densities. The excitation spectrum of the low frequency modes has been considered and discussed in detail. It is found that quantum beats in spontaneous emission may appear in the spectra of the one- and two-photon resonance fluorescence arising from the interference between the two atomic transition frequencies and the frequency of the laser field. The importance of the low frequency modes that occur in the processes in question has been pointed out.
CsCdBr3 : Nd3+ crystals have been studied by laser selective excitation and time resolved spectroscopy. Due to the charge compensation resulting from the Nd3+ / Cd2+ substitution, the proportion of Nd3+ pairs is very large and does not follow the statistical laws. This proportion has been measured, its variation with concentration has been established and the effect of codoping with a monovalent metal observed. From a comparison between the properties of single ions and pairs, energy transfers have been analysed. De-excitation channels have been determined for some excited levels from the dynamics and the relative intensities of luminescence lines. An unusual behaviour, which can lead to applications, has been observed : the 4F3/2 luminescence of pairs if favoured with respect to that of single ions. This behaviour is well explained.
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.