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Quantum Electronics

Inhomogeneous broadening and splitting of lines in spectra of YAG : Tm

Marina N. Popova, E. P. Chukalina, С. А. Климин, M.-Ch. Chou

Published Mar 1, 2020• 4 citations
Publisher

Abstract

Abstract The shape and fine structure of lines due to Tm3+ f −f electronic transitions in multifunctional Y3Al5O12 garnet crystals have been studied by high-resolution spectroscopy. The observed inhomogeneously broadened lines have a Lorentzian shape, suggesting that point defects make a predominant contribution to the inhomogeneous broadening. Moreover, YAl antisite defects, which are formed during high-temperature melt growth, produce spectral satellites near the main lines.

DOI
10.1070/qel17271

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Applied Spectroscopy•Nov 1, 1987•0 citations
Abstract The shape and fine structure of lines due to Tm3+ f −f electronic transitions in multifunctional Y3Al5O12 garnet crystals have been studied by high-resolution spectroscopy. The observed inhomogeneously broadened lines have a Lorentzian shape, suggesting that point defects make a predominant contribution to the inhomogeneous broadening. Moreover, YAl antisite defects, which are formed during high-temperature melt growth, produce spectral satellites near the main lines.
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.
Optically active defects in solid-state systems have many applications in quantum information and sensing. However, unlike free atoms, which have fixed optical transition frequencies, the inhomogeneous broadening of the transitions in solid-state environments limit their use as identical scatterers for such applications. Here we show that crystals of argon and neon prepared in a closed-cycle cryostat doped with thulium atoms at cryogenic temperatures are an exception. High resolution absorption and emission spectroscopy show that the 1140 nm magnetic dipole transition is split into multiple components. The origin of this splitting is likely a combination of different classes of trapping sites, crystal field effects within each site, and hyperfine interactions. The individual lines have ensemble widths as small as 0.6GHz0.6\phantom{\rule{4.pt}{0ex}}\text{GHz}0.6GHz, which temperature dependence and pump-probe spectroscopy indicate is likely a homogeneous effect, suggesting inhomogeneity is well below the GHz scale.
The procedure of calculation of the spectral line shape in optical spectra of rare-earth ions in crystals with the inclusion of random deformations of an elastically anisotropic crystal lattice caused by point defects is developed. The distribution function of components of the random strain tensor in the case of a low defect concentration is obtained as the generalized six-dimensional Lorentz distribution. The distribution function parameters are represented by the integral functional of the strain tensor components on a sphere of unit radius containing an isotropic point defect in its center. The numerical calculations of the strain tensors induced by point defects and the parameters of the distribution functions of random strains in LiLuF4 and LaAlO3 crystals have been performed. The calculated envelope with the doublet structure corresponding to the Γ2(3H4) → Γ34(3H5) singlet–doublet transition in the absorption spectrum of Pr3+ ions in the LiLuF4 crystal agrees well with the data of the measurements.
The detailed site-selective and time-resolved fluorescence laser spectroscopy and kinetic measurements with high spectral and nanosecond temporal resolution were applied to analyze the M and N absorption bands at the 4I9/2(1) yields 4G5/2(1) crystal field (CF) transition in the CaF2:Nd3+ crystal at 4.2 K. It was found that at helium temperatures the dynamically split spectral line at the 4I9/2(1) yields 4G5/2(1) CF transition of coherently coupled Nd3+ ions in the pair M- and quartet N-centers is inhomogeneously broadened. Small variation of fluorescence lifetimes of the 4F3/2 and 4D3/2 levels due to small variation of distances between Nd3+ ions in the pairs was found. Approximately 1 percent variation of the Nd-Nd distance in the pair -center was determined form lifetime variation of the 4F3/2 manifold.
Spectroscopy and Coherence of an Excited-State Transition in Tm3+^{3+}3+:YAlO3_33​ at Telecommunication Wavelength
We characterize spectroscopic and coherence properties of the 1451.37 nm excited-state zero-phonon line (ZPL) between the 3F4^{3}F_{4}3F4​ and the 3H4^{3}H_{4}3H4​ manifolds of a thulium-doped yttrium aluminum perovskite (Tm3+^{3+}3+:YAlO3_33​) crystal at temperatures around 1.5 K. We measure the absorption spectrum between the 3H6^{3}H_{6}3H6​ - 3F4^{3}F_{4}3F4​ and 3F4^{3}F_{4}3F4​ - 3H4^{3}H_{4}3H4​ manifolds, the inhomogeneous broadening of the 3F4^{3}F_{4}3F4​ - 3H4^{3}H_{4}3H4​ (excited-state) ZPL, and the lifetimes of the higher-lying and lower-lying excited states. We also investigate level shifts caused by the quadratic Zeeman interaction as well as spectral hole-burning spectra with varying magnetic fields, providing insights into hyperfine interactions. Using again spectral holes but also optical free induction decays (FIDs), we assess optical coherence times, finding a maximum of 4.75±0.07 μs4.75 \pm 0.07~μs4.75±0.07 μs at B=2T and low ion concentration in the 3F4^{3}F_{4}3F4​ level. Our results -- the first to demonstrate coherence of an excited-state transition in a rare-earth crystal -- suggest the possibility of exploiting such transitions for quantum technology.
Fluorescence studies of the R-line emission of ruby laser rods over the temperature range of 77 to 300 K have disclosed several new features. In particular, for most of the ruby rods, the fluorescent decay time, τ, was not strictly exponential. Effects of this kind have been observed in the fluorescent decay of the 4F3/2 level of Nd3+ in YAG (yttrium aluminum garnet) and in Nd-doped glasses. In both cases, the nonexponential decay was interpreted as evidence for inhomogeneous line broadening effects, among which are strains, ion clustering, and other defects that modify the crystal field at the ion site. Our observations of nonexponential fluorescent decay in ruby are indicative of inhomogeneous line broadening effects in lightly doped (0/05%) ruby. In fact, inhomogeneous line broadening was observed in ruby at liquid helium temperatures, in the spectroscopic studies of A. L. Schawlow.