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Physics of the Solid State

Two-photon excitation of the anti-Stokes photoluminescence of Ca1–x Er x F2 + x crystals

А. Н. Грузинцев, Denis N. Karimov

Published Jan 1, 2017• 3 citations
Publisher

Abstract

Crystals of the composition Ca1–x Er x F2 + x (0 < x ≤ 0.02) have been grown from the melt by the Bridgman method. The absorption, luminescence excitation, and photoluminescence spectra of this material in the case of the Stokes and anti-Stokes mechanisms of the optical excitation from two radiation sources simultaneously have been analyzed. It has been found that the visible luminescence manifests itself upon sequential absorption of two resonance infrared photons with different energies. This effect is associated with the fact that, in this material, there are metastable states of the excited levels 4 I 11/2 of the Er3+ ions, from which transitions to higher energy levels occur due to the absorption of infrared photons.

DOI
10.1134/s1063783417010103

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Journal of Physics Condensed Matter•Jun 30, 2006•11 citations
Crystals of the composition Ca1–x Er x F2 + x (0 < x ≤ 0.02) have been grown from the melt by the Bridgman method. The absorption, luminescence excitation, and photoluminescence spectra of this material in the case of the Stokes and anti-Stokes mechanisms of the optical excitation from two radiation sources simultaneously have been analyzed. It has been found that the visible luminescence manifests itself upon sequential absorption of two resonance infrared photons with different energies. This effect is associated with the fact that, in this material, there are metastable states of the excited levels 4 I 11/2 of the Er3+ ions, from which transitions to higher energy levels occur due to the absorption of infrared photons.
Abstract Emission and visible photoluminescence excitation spectra of CaF2:Er (0.5 at %) crystals have been studied under different optical pumping conditions. The results demonstrate that anti-Stokes luminescence of the erbium-doped crystals has higher intensity in the case of pumping of the 4I13/2 metastable state of the dopant. Resonance IR photon wavelengths have been determined for two-photon excitation of visible emission in CaF2:Er. A method has been developed for the optical modulation of anti-Stokes luminescence, which allows the nature of the corresponding electron transitions in emission centers to be identified.
A new method was developed for determining the mechanism of anti-Stokes filling of luminescent levels of an activator in a rare-earth crystal. An investigation was made of the dependences of the absolute populations of the 4 I 13/2 , 4 I 11/2 , 4 F 9/2 , 4 S 3/2 , H 9/2 , 4 G 11/2 , and 2 P 3/2 levels of Er 3+ in a BaYb 2 F 8 crystal on the energy absorbed within the Yb 3+ sensitizer band. The mechanisms of anti-Stokes filling of the 4 I 13/2 , 4 F 9/2 , 4 S 3/2 , and 2 H 9/2 levels of Er 3+ were determined under conditions of weak (1 mJ/cm 3 ) and strong (∼10 J/cm 3 ) pumping.
Abstract Theoretical and experimental investigations are made of two‐photon absorption spectra of trivalent rare‐earth ions in crystals. Effective cross‐sections, selection rules, and relative intensities of the components are found. The most intensive two‐photon transitions are established. Two‐photon excitation spectra of luminescence of Er3+ and Ho3+ ions in CaF2 are obtained and effective excitation cross‐sections are measured using a tunable dye laser (715 to 850 nm). It is shown that the spectra have a peculiar structure which differs considerably from that of the one‐photon absorption spectra. The experimental results agree with theory. It is established that one of the levels in Ho3+ is the level 5G6 rather than 3K7 usually assumed.
To study the role of stepwise and relaxation processes under effective excitation of anti-Stokes luminescence of rare-earth (RE) ions in crystals the time-shifted pulse method is used. It is shown that direct comparison of measured single- and two-photon luminescence excitation spectra often enables one to make immediate conclusions on the position and classification of electron levels of RE ions. The Tb3+ and Eu3− level structures (crystal CaF2) in the near ultraviolet are considered as an example. The peculiarities connected with the polarization characteristics of the two-photon absorption of radiation by the trivalent RE ions in a crystal matrix are discussed. To obtain the two-photon spectra a frequency-tunable organic dye solution laser (ODSL) is used.
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 are interested, in this work, in determining the Stark sub-level of Er3+ ions doping a KY3F10 single crystal with a molar concentration of 1%. We have used a new method of measurement of energies of the ground level and emitting levels from excitation and anti-Stokes emission spectra recorded at liquid nitrogen temperature. This technique is based on a spectral analysis of the anti-Stokes emissions recorded after selective excitation with a red dye tunable laser. Thus, we could determine the Stark sub-levels of the ground and the principal emitting levels in the infrared, visible and near-UV ranges with a very good precision.