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Optics and Spectroscopy

Magnetooptics of the 1 D 2 → 3 F 4 radiative transition in thulium:yttrium-aluminum garnet Tm3+:YAG

Uygun V. Valiev, John B. Gruber, I. R. Gapdulkhakov, Nafisa Inoyatovna Juraeva, Anvar K. Mukhammadiev, Sh. A. Rakhimov, I. S. Édelman

Published Jun 1, 2009• 9 citations
Publisher

Abstract

The spectra of luminescence and magnetic circular polarization of luminescence in the 1 D 2 → 3 F 4 emission band in thulium:yttrium-aluminum garnet Tm3+:YAG (Tm3+:Y3Al5O12) have been investigated at temperatures T = 78 and 293 K, respectively. Based on the analysis of the magnetooptical and optical spectra, the optical transitions between the Stark sublevels of the 3 F 4 and 1 D 2 multiplets in Tm3+:YAG were identified. It is shown that the symmetry and energies of the Stark sublevels of the 3 F 4, 1 D 2, and 3 H 6 multiplets, found experimentally from magnetic and magnetooptical studies, confirm the results of theoretical calculations of the energy spectrum of the rare earth Tm3+ ion in YAG.

DOI
10.1134/s0030400x09060101

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Physical review. B, Solid state•Mar 1, 1970•31 citations
The spectra of luminescence and magnetic circular polarization of luminescence in the 1 D 2 → 3 F 4 emission band in thulium:yttrium-aluminum garnet Tm3+:YAG (Tm3+:Y3Al5O12) have been investigated at temperatures T = 78 and 293 K, respectively. Based on the analysis of the magnetooptical and optical spectra, the optical transitions between the Stark sublevels of the 3 F 4 and 1 D 2 multiplets in Tm3+:YAG were identified. It is shown that the symmetry and energies of the Stark sublevels of the 3 F 4, 1 D 2, and 3 H 6 multiplets, found experimentally from magnetic and magnetooptical studies, confirm the results of theoretical calculations of the energy spectrum of the rare earth Tm3+ ion in YAG.
The Zeeman effect has been studied within the “green” range of luminescence due to the radiative 4f→4f transitions D54→F75 for the rare earth ion Tb3+ in yttrium aluminum garnet (Y3Al5O12) at a sample temperature of 85 K. The special features associated with the magnetic field dependence of the Zeeman splitting have been explained for transitions observed in the geometry of the longitudinal and transverse Zeeman effect. An analysis of the results obtained from the magneto-optical data indicates that in a magnetic field a nonequilibrium population distribution occurs between the sublevels of the quasidoublet state (Γ1,Γ4) in the D54 manifold. The energy of the quasidoublet state is approximately 20 585 cm−1.
Rare-earth-doped crystals have been used for optical signal processing and storage applications. In this dissertation, their potential for quantum computing applications is explored. In one quantum computing scheme, information is stored in nuclear spin states and this information is then processed by using optical pulses through the coupling of these nuclear spin states to a common electronic level. To implement this scheme, nuclear spin states and coupling of these nuclear spin states to a common electronic level is required. Preliminary work in rare-earth materials like Pr3+ and Eu3+ has shown promising results regarding their suitability for quantum computing applications. One particular problem with these materials is that their transition wavelengths are only accessible with dye lasers. These lasers are inherently unstable, and currently few available systems exhibit the stability required for quantum computing applications. An alternative choice was to investigate other rare-earth ions like thulium. Thulium has a transition wavelength that can be accessed with diode lasers, which are commercially available, easy to stabilize, and compact. This dissertation is based on our investigations of Tm3+:YAG for quantum computing applications. Investigations involved a detailed characterization of the material. Nuclear spin states, in Tm3+:YAG, were obtained by applying an external magnetic field to the sample. First, interaction of an external magnetic field with the thulium ions at various sites in the crystal was analyzed. This analysis was used to measure the magnetic anisotropy in the material. These results show that it is possible, with the suitable choice of the magnetic orientation and the site in the crystal, to build a working 3-level quantum system. In the demonstration of single qubit operations in Tm3+:YAG, we first theoretically studied the effect of Gaussian spatial beam on the single qubit operations. Later on, we experimentally prepared a single isolated ensemble of ions in the inhomogeneously broadened absorption profile of the medium. This single isolated ensemble of ions was used as a test-bed to implement the single qubit operations. We also isolated two ensembles of ions in the inhomogeneous absorption profile of the medium. The interaction between these two isolated ensembles of ions was also studied.
An investigation was made of the absorption spectrum of Cr 3+ ions in the ground ( 4 A 2 ) and metastable ( 2 E) states, and of the luminescence spectrum of the same ions in Y 3 Al 5 O 12 crystals at 300 and 77°K. The effective absorption cross sections were determined for the 4 A 2 state. The luminescence deexcitation time was found to be 1.5 and 9 msec at 300 and 77°K, respectively. The absorption spectrum of the 2 E state had four wide absorption bands with maxima at 16,700, 23,300, 28,600, and 40,500 cm –1 . The theoretical energy level scheme of Cr 3+ was calculated for Dq = 1725 cm –1 , G = 640 cm –1 , C = 3200 cm –1 , v = 495 cm –1 , and v' = 259 cm –1 , making an allowance for the mixing of the Γ trig S states. The experimentally observed absorption bands were attributed to specific transitions and the theoretical and experimental intensities were compared.
Yttrium aluminum garnet (YAG): Pr3+ is synthesized by codeposition me thod. Vacuum ultraviolet (VUV) excitation and emission spectra of YAG: Pr3+ at different temperatures are measured using synchrotron radiation as an excitation source. We analyze the transition process after excitation to 4f5d en ergy band and estimate the Huang-Rhys factor S and phonon energy ηω of YAG: Pr 3+ by multi-phonon relaxation. Emission of self-trapped exciton (STE) and 3P0→3H4,5,6 emission transferr ed from the STE energy appear when YAG: Pr3+is excited by 170nm, whic h is a different transition process from those excited by 240nm and 289nm.
Optical absorption and emission spectra are used to determine the energy levels of the 5I8^{5}I_{8}5I8​ ground state and 5I7^{5}I_{7}5I7​ excited state of Ho3+{\mathrm{Ho}}^{3+}Ho3+ in diamagnetic yttrium gallium garnet (YGaG) and ferrimagnetic yttrium iron garnet (YIG). The results for YGaG are consistent with the D2{D}_{2}D2​ site symmetry of the dodecahedral site in the garnet structure. Energy levels in YIG which are separated by site inequivalency are identified from spectra observed as the Fe3+{\mathrm{Fe}}^{3+}Fe3+ magnetization is rotated in the (11‾01\overline{1}0110) plane. Stimulated emission is observed from Ho3+{\mathrm{Ho}}^{3+}Ho3+ in YGaG at 2.086 and 2.114 \ensuremath{\mu} and from Ho3+{\mathrm{Ho}}^{3+}Ho3+ in YIG at 2.086, 2.089, and 2.107 \ensuremath{\mu}. Each of the lines in YIG is composed of two superimposed electronic transitions. The exchange field in YIG makes possible magnetic tuning of coherent emission over a range of 70 \AA{}.