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The Journal of Chemical Physics

Absorption and Fluorescence Spectra of Er3+(4f11) in LaF3

William F. Krupke, John B. Gruber

Published Aug 15, 1963• 78 citations
Publisher

Abstract

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.

DOI
10.1063/1.1734352

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The energy levels of the I4 ground term of Er3+ in single crystals of CaWO4 were established by absorption and fluorescence spectra measurements. The measurements were made using crystals at temperatures of 2, 20, and 85°K. The energy level scheme allows an interpretation of the 1.612-μ four-level CaWO4:Er3+ laser transition and shows the terminal energy level of this transition to be 318 cm−1 above the ground state rather than 375 cm−1 as reported by Kiss and Duncan. An effective Hamiltonian of the form suggested by Karayianis was diagonalized in a basis of Russell–Saunders wavefunctions to obtain the calculated energy levels and wavefunctions for the entire ground term of Er3+. The calculation takes into account the complete J mixing of the states within the ground term and is equivalent to determining the effects of the spin–orbit interaction to better than second order. An rms deviation of 18 cm−1 was found as the best agreement between the calculated and experimental energy levels using the Hamiltonian: H = λ1(L·S) + λ2(L·S)2 + λ3(L·S)3 + ΣlmBlm†Clm. The empirically determined parameters are (in cm−1) λ1 = − 613, λ2 = − 19.3, λ3 = − 0.499, B20 = 404, B40 = − 685, B60 = 12.4, B44 = 728, ReB64 = 452, and ImB64 = 164. Using wavefunctions determined with these parameters, the g factors were calculated for the states of the ground term. The calculated and measured g factors for the two lower energy states are in good agreement where the calculated values are g‖ (ground state) = 1.265, g⊥ (ground state) = 8.487, g‖* (first excited state) = 3.22, and g⊥* (first excited state) = 7.06, and the measured values in the same order are g‖ = 1.247, g⊥ = 8.400, g‖* = 3.42, and g⊥* = 6.98. A Γ5,6 ground state wavefunction is compatible with the results obtained here, whereas a Γ7,8 ground state wavefunction is not. Previous studies had not established the ground state wavefunction uniquely.

The Journal of Chemical Physics•Jan 1, 1971•20 citations
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.
The analysis of the absorption spectrum of Er3+ in LaF3 is extended into the ultraviolet region to 2000 Å. A number of fluorescence lines recently observed in the region from 3000 to 25 000 Å is also reported. Based on the best over-all agreement between the predicted ``free-ion'' 4f11 SLJ states and 21 experimentally observed levels for Er3+ in LaF3, one finds a set of atomic wavefunctions for the ion based on F2 = 435.7 cm—1, F4 = 67.21 cm—1, F6 = 7.388 cm—1, and ζ = 2350.8 cm—1. Laser experiments are described and the details of coherent emission found at 1.61 μ are presented.
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.
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.
We use upconversion fluorescence excitation and IR absorption to make precise measurements of the Stark components of the 4I11/2 level of the Er3+ ion in YLiF4. We are able to specify all six components of this system unambiguously and to establish their energies to ±0.5 cm−1. By so doing, we are able to resolve discrepancies of greater than 100 cm−1 in the energies that are reported in the literature. A consistent interpretation of both the emission and the absorption data was possible with the Stark components of 4I11/2 found from our analysis.
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 energy levels of the I4 ground term of Er3+ in single crystals of CaWO4 were established by absorption and fluorescence spectra measurements. The measurements were made using crystals at temperatures of 2, 20, and 85°K. The energy level scheme allows an interpretation of the 1.612-μ four-level CaWO4:Er3+ laser transition and shows the terminal energy level of this transition to be 318 cm−1 above the ground state rather than 375 cm−1 as reported by Kiss and Duncan. An effective Hamiltonian of the form suggested by Karayianis was diagonalized in a basis of Russell–Saunders wavefunctions to obtain the calculated energy levels and wavefunctions for the entire ground term of Er3+. The calculation takes into account the complete J mixing of the states within the ground term and is equivalent to determining the effects of the spin–orbit interaction to better than second order. An rms deviation of 18 cm−1 was found as the best agreement between the calculated and experimental energy levels using the Hamiltonian: H = λ1(L·S) + λ2(L·S)2 + λ3(L·S)3 + ΣlmBlm†Clm. The empirically determined parameters are (in cm−1) λ1 = − 613, λ2 = − 19.3, λ3 = − 0.499, B20 = 404, B40 = − 685, B60 = 12.4, B44 = 728, ReB64 = 452, and ImB64 = 164. Using wavefunctions determined with these parameters, the g factors were calculated for the states of the ground term. The calculated and measured g factors for the two lower energy states are in good agreement where the calculated values are g‖ (ground state) = 1.265, g⊥ (ground state) = 8.487, g‖* (first excited state) = 3.22, and g⊥* (first excited state) = 7.06, and the measured values in the same order are g‖ = 1.247, g⊥ = 8.400, g‖* = 3.42, and g⊥* = 6.98. A Γ5,6 ground state wavefunction is compatible with the results obtained here, whereas a Γ7,8 ground state wavefunction is not. Previous studies had not established the ground state wavefunction uniquely.