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Journal of Physics C Solid State Physics

Investigation of Zeeman second-order effects in Pr3+:LaCl3using the fluorescence-line-narrowing technique

Nicole Pelletier-Allard, R. Pelletier

Published Nov 14, 1979• 4 citations
Publisher

Abstract

A technique involving the laser-induced narrowing of a fluorescence line is used to obtain high-resolution spectra of Pr3+:LaCl3. The second-order effects caused by Zeeman and nuclear interactions are systematically investigated in the 3H4E2 to or from 1D2A1 transition. A non-zero perpendicular Zeeman splitting of the ground level, proportional to the square of the magnetic field, is measured and interpreted as being caused by the perturbation by the four upper Stark levels belonging to the 3H4 multiplet. The variation of the number and of the relative intensities of the hyperfine lines is demonstrated to be closely related to the angle between the external magnetic field direction and the crystal axis. It is unambiguously attributed to an angular dependence, with regard to the magnetic field direction, of the hyperfine states of the excited level. The importance of the effect, caused by a very distant perturbing level, is shown to be a result of the quasidegeneracy of the mu =0 excited level.

DOI
10.1088/0022-3719/12/21/029

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Physical Review B•May 12, 2005•56 citations
A technique involving the laser-induced narrowing of a fluorescence line is used to obtain high-resolution spectra of Pr3+:LaCl3. The second-order effects caused by Zeeman and nuclear interactions are systematically investigated in the 3H4E2 to or from 1D2A1 transition. A non-zero perpendicular Zeeman splitting of the ground level, proportional to the square of the magnetic field, is measured and interpreted as being caused by the perturbation by the four upper Stark levels belonging to the 3H4 multiplet. The variation of the number and of the relative intensities of the hyperfine lines is demonstrated to be closely related to the angle between the external magnetic field direction and the crystal axis. It is unambiguously attributed to an angular dependence, with regard to the magnetic field direction, of the hyperfine states of the excited level. The importance of the effect, caused by a very distant perturbing level, is shown to be a result of the quasidegeneracy of the mu =0 excited level.
Laser-induced fluorescence line narrowing of the ruby R1{R}_{1}R1​ Zeeman spectra at 693.4 nm is reported using a continuous, stable, single-frequency ruby laser for resonant excitation. A resolution in excess of 107{10}^{7}107 corresponding to a linewidth of \ensuremath{\sim} 30 MHz has been achieved. The linewidths are anisotropic with respect to the relative magnetic-field-crystal-axis orientation and, at low Cr concentrations, are expected to be determined by Cr-Al superhyperfine interactions.
Subnatural-width resonances due to coherent effects in optical pumping at hyperfine (hf) transitions of Rb are investigated using a linearly or circularly polarized single-frequency diode laser beam. The sign and amplitude of the resonances in the fluorescence are measured by scanning the laser frequency over the hf transitions of the Rb D 1 and D 2 lines. The fluorescence perpendicular to the laser beam is detected as a function of magnetic field parallel to the beam propagation and scanned around zero value. In the case of linear polarization of the field, dark resonances are observed for hf transitions with F g → F e = F g -1 and F g → F e = F g , and bright resonances are observed for transitions with F g → F e = F g + 1. This is in agreement with the recently developed theories. For all (except F g = 2→ F e = 3, 85 Rb, D 1 line) hf transitions the sign of the resonances reverses when the polarization of the field changes to circular. The amplitudes of the resonances correspond to the probability of the hf transitions and to the calculated loss rate of the population to the ground hf level not excited by the laser field. The observed narrow resonances (FWHM: few tens of kHz) and their sensitivity to weak magnetic fields are interesting for high-resolution spectroscopy and for development of simple and precise magnetometers.
A simple and straightforward method is presented for determining the electric-dipole moments of phototransitions between degenerate levels in atoms. In the present method, the dynamic Stark effect (DSE) is induced by a high-fluence laser light in the presence of a strong external magnetic field. The energy splitting caused by the DSE is measured by sweeping the frequency of the probe laser. As the separation width of the DSE peak is essentially given by a product of the dipole moment , the relevant Wigner 3- j symbol and the square root of the laser intensity, we are able to determine the value of in a direct way. As the DSE is induced between a pair of non-degenerate Zeeman sublevels, which is singled out by the external magnetic field, the result is free from any ambiguities brought about by the degeneracy such as the smoothing out of DSE peaks caused by the overlapping of the sublevel contributions. The method was tested against the transition between the 17 362 and levels in atomic uranium, giving the electric dipole moment .
The influence of an external magnetic field on the hyperfine structure of the 3 H4(0) and 1D2(0) crystal field states of Pr3+ in LiYF4 is studied in order to find an efficient three-level Λ system. Using an experimentally determined spin Hamiltonian, we show that three-level Λ systems can be obtained with equal strengths for the optically excited transitions under various magnetic field magnitudes and orientations. An analytical analysis based on two levels is proposed to find useful magnetic fields without extensive numerical calculations and to understand the general behaviour of the system. Pr3+ hyperfine structure has also been directly calculated using a complete Hamiltonian including free ion, crystal field and magnetic interactions. A good agreement with the spin Hamiltonian approach is found for the ground state whereas the excited state results poorly reproduce the experiment. This is attributed to the low accuracy of 1D2 crystal field wavefunctions. This suggests that transition strengths ratios could be calculated directly from the crystal field Hamiltonian with improved crystal field parameters.
The influence of magnetic interactions in rare-earth-doped crystals under an external magnetic field has been studied in order to obtain an efficient three-level $\ensuremath{\Lambda}$ system with the hyperfine levels of the rare earth. Nuclear Zeeman effect under the action of an external magnetic field removes the nuclear degeneracy. This interaction does not provide an efficient $\ensuremath{\Lambda}$ system because nuclear-spin flipping such as $\ensuremath{\mid}{M}_{I}⟩=\ifmmode\pm\else\textpm\fi{}\frac{1}{2}\ensuremath{\rightarrow}\ensuremath{\mid}{M}_{I}⟩=\ensuremath{\mp}\frac{1}{2}$ (MI{M}_{I}MI​ is the nuclear-spin projection) cannot be induced by an optical transition. However, this selection rule only applies to pure nuclear Zeeman effect. Indeed, it is shown that the coupling of the electronic Zeeman and of the hyperfine interactions releases the nuclear-spin selection rules $\ensuremath{\Delta}{M}_{I}=0$. This can be described in terms of a pseudonuclear Zeeman effect induced by an effective magnetic field. The relative strengths of the two optical transitions involved in the three-level system can be controlled by the orientation of the external magnetic field. The particular case of the Tm3+{\mathrm{Tm}}^{3+}Tm3+ ion in the Y3Al5O12{\mathrm{Y}}_{3}{\mathrm{Al}}_{5}{\mathrm{O}}_{12}Y3​Al5​O12​ host (YAG) is discussed. Tm3+{\mathrm{Tm}}^{3+}Tm3+ hyperfine structure is determined using a complete Hamiltonian including free-ion, crystal-field, and magnetic interactions. A good three-level $\ensuremath{\Lambda}$ system is obtained in Tm:YAG with a transition strength ratio of 0.24 $(\ensuremath{\sim}1:4)$ between the two optical transitions. An analytical analysis based on a spin-Hamiltonian approach is proposed to explain the results of the complete crystal-field calculations. Finally, an experimental protocol that makes a crystal similar to the atomic samples used in previous quantum information investigations, with the additional benefits of absence of motion and long coherence time, is described.