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Physics of the Solid State

Spectra of optical absorption and energy levels diagram of Er3+ ions in bulk crystals of aluminum nitride

Н. К. Полетаев, Alexander P. Skvortsov

Published Dec 1, 2017• 2 citations
Publisher

Abstract

The absorption spectra of the Er3+ ions embedded in the AlN matrix have been investigated. The admixture of erbium was introduced in bulk AlN crystals by diffusion. The absorption lines, which are associated with the intraconfigurational electronic f–f-transitions from the ground 4 I 15/2-state to the levels of ion Er3+ excited states have been observed in the spectral range of 370–700 nm. The transitions to the state levels 4 F 9/2, 2 H 11/2, 4 F 7/2, 4 F 5/2, 2 H 9/2, and 4 G 11/2 have been investigated in detail at the temperature T = 2 K. The number of the observed lines for these transitions coincides with the theoretically possible one for the electronic f–f-transitions in the ions Er3+, which are in the crystal field with the symmetry below cubic. The narrowness of the observed lines and their number convincingly testify the replacement of preferably one regular crystalline position by erbium ions. The implementation of Er3+ in the Al3+ position with the local symmetry C 3v appears the most probable. The energy positions of the levels of excited states for the investigated transitions have been determined. The diagram of the Er3+ ion energy levels in the AlN crystals has been built.

DOI
10.1134/s1063783417120265

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The absorption spectra of the Er3+ ions embedded in the AlN matrix have been investigated. The admixture of erbium was introduced in bulk AlN crystals by diffusion. The absorption lines, which are associated with the intraconfigurational electronic f–f-transitions from the ground 4 I 15/2-state to the levels of ion Er3+ excited states have been observed in the spectral range of 370–700 nm. The transitions to the state levels 4 F 9/2, 2 H 11/2, 4 F 7/2, 4 F 5/2, 2 H 9/2, and 4 G 11/2 have been investigated in detail at the temperature T = 2 K. The number of the observed lines for these transitions coincides with the theoretically possible one for the electronic f–f-transitions in the ions Er3+, which are in the crystal field with the symmetry below cubic. The narrowness of the observed lines and their number convincingly testify the replacement of preferably one regular crystalline position by erbium ions. The implementation of Er3+ in the Al3+ position with the local symmetry C 3v appears the most probable. The energy positions of the levels of excited states for the investigated transitions have been determined. The diagram of the Er3+ ion energy levels in the AlN crystals has been built.
This Letter presents results of analysis of the absorption spectra of AlN:Er 3+ bulk crystals. In the spectral of 370–700 nm, absorption lines responsible for intraconfiguration electron transition from the ground state 4 I 15/2 to the excited states of Er 3+ ions are found. Transitions to the levels of the 4 F 9/2 , 2 H 11/2 , and 4 G 11/2 states at 2 K are studied in detail. The number of observed lines for these transitions fully agrees with that theoretically possible for f – f electron transitions in Er 3+ ions found in a noncubic crystal field. The small width of the observed lines and their number indicate that erbium ions displace mostly one regular crystal position. Most probably, Er 3+ occupies the position of Al. Energy positions of excited states for the considered transitions are determined.
The rare-earth element, erbium (Er), was successfully diffused into GaAs and InP for the first time. Two intense and three weak sharp photoluminescence (PL) lines related with Er were observed at a wavelength of ∼1.55 μm both in GaAs and InP. It was found, for the first time, that the emission energy and the linewidth of the two intense Er-related PL lines do not depend on temperatures up to 220 K. This clearly indicates that these sharp emission lines are due to 4f-intracenter transitions in triply ionized erbium (Er3+) ions, and that the 4f orbitals are well shielded from a crystal field by the outer closed orbitals. Furthermore, it was found that the intensity ratio of the five emission lines from Er3+ is independent of the excitation power density. The results reveal that the Er3+ ion substitutes a cation site both in GaAs and InP, and that the five PL lines correspond to the transitions from the first excited state to the five crystal-field-split ground states of Er3+ ion with a tetrahedral (Td) symmetry.
Photoluminescence (PL) spectra of Er3+ in an Er-doped silicon film were recorded at 2 and 77 K over the wavelength range from 1.52 to 1.68 μm, which includes optical transitions between the Er3+ I13/24 and I15/24 manifolds. These spectra were then analyzed to determine the nature of the electrostatic field at the site of the Er ion that governs the ion’s optical behavior. The PL spectra were analyzed three different ways: by considering the Er3+ ions to be occupying sites of Td, C3, or D2d point group symmetry. Transition energies and magnetic dipole transition probabilities were calculated for each case by diagonalizing a Hamiltonian representing the free-ion and crystal-field interactions in a Russell–Saunders basis of states spanning the lowest 15 J multiplets of the 4f11 electronic configuration of Er3+. Crystal-field parameters were varied in each case to find the best agreement with the experiment. Our results showed that the site symmetry of the Er3+ ions most consistent with the data is D2d. For this case, the rms deviation between the experimental and calculated energy levels is 3.3 cm−1 with the calculated magnetic dipole transition probabilities in qualitative agreement with the experiment.
Temperature dependence of an enhanced excited state absorption was investigated in erbium-doped garnet crystals using 787.3 and 787.8 nm laser diodes. The enhanced absorption was obtained at temperature ranges of 15–570 K, 15–420 K, and 15–1200 K in a yttrium aluminum garnet, a yttrium scandium gallium garnet, and a lutetium aluminum garnet, respectively. Absorption peaks corresponding to both the I1615/2−I49/2 and the I1613/2−I211/2 transitions of Er3+ in garnets were shifted from those for 300 K at high temperature. The enhanced absorption weakened at high temperature because an absorption cross section from the I413/2 level to the H211/2 level decreased due to the shift of the absorption peaks. It has been confirmed that a mechanism of the enhanced absorption can be explained by calculating the rate equations based on an analytical model for a five-level system of the Er3+ ion. It is suggested that the enhanced absorption weakened at temperatures lower than 12 K because the number of phonons decreased due to low temperature.
Erbium ions in crystals show considerable promise for the technologies that will form the backbone of future networked quantum information technology. Despite advances in leveraging erbium’s fibre-compatible infrared transition for classical and quantum applications, the transitions are, in general, not well understood. We present detailed absorption and laser site-selective spectroscopy of the C 3v (O 2 − ) centre in CaF 2 :Er 3 + as an interesting erbium site case study. The 4 I 15 / 2 Z 1 → 4 I 13 / 2 Y 1 transition has a low-temperature inhomogeneous linewidth of 1 GHz with hyperfine structure observable from the 167 Er isotope. A parametrized crystal-field Hamiltonian is fitted to 34 energy levels and the two ground state magnetic splitting factors. The wavefunctions are used to perform a transition intensity analysis and electric-dipole parameters are fitted to absorption oscillator strengths. Simulated spectra for the 4 I 11 / 2 → 4 I 15 / 2 and 4 I 13 / 2 → 4 I 15 / 2 inter-multiplet transitions are in excellent agreement with the experimentally measured spectra. The 4 I 13 / 2 excited state lifetime is 25.0 ms and the intensity calculation is in excellent agreement with this value. • Detailed spectroscopic study of the C 3v (O 2 − ) Centre in CaF 2 :Er 3 + . • Crystal-field fit to 34 energy levels and ground-state magnetic splitting. • Transition intensity analysis for the technologically relevant infrared transitions.
The absorption, fluorescence, and excitation spectra of Er3+(4f11) in LaF3 have been investigated between 3500 and 10 000 Å. Based on an energy-level scheme consistent with all observed spectral lines, a number of states have been identified. The parameters giving the best over-all agreement between the predicted ``free-ion'' spectrum and the spectrum of Er3+ in LaF3 are F2=428.708 cm-1, F4=67.784 cm-1, F6=6.751 cm-1, and ζ=2389.60 cm-1. The average deviation for 11 of these levels is 35.3 cm-1. The possible use of Er3+ in LaF3 for the generation of coherent green light is also discussed.