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Quantum Electronics

One- and two-photon spectra of Nd3+clusters in CaF2and SrF2crystals

Tasoltan T. Basiev, В. В. Воронов, M. Yu. Glotova, A.G. Papashvili, Aleksandr Ya Karasik

Published Aug 31, 2003• 8 citations
Publisher

Abstract

The polarised two-photon (IR) and one-photon (visible) luminescence excitation spectra of Nd 3+ nanoclusters in CaF 2 and SrF 2 crystals are measured at 10 K using a :LiF colour centre laser tunable in spectral ranges 1090 — 1230 nm and 545 — 615 nm with an emission linewidth of ~0.02 — 0.03 cm -1 , an average output power of ~55 mW, and a pulse repetition rate of 10 Hz. The two-photon excitation spectra at the 4 I 9/2 → 4 G 5/2 transition reveal the structure, which is absent upon one-photon excitation, which can be explained by different selection rules for some Stark — Stark transitions upon one- and two-photon absorption.

DOI
10.1070/qe2003v033n08abeh002478

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The polarised two-photon (IR) and one-photon (visible) luminescence excitation spectra of Nd 3+ nanoclusters in CaF 2 and SrF 2 crystals are measured at 10 K using a :LiF colour centre laser tunable in spectral ranges 1090 — 1230 nm and 545 — 615 nm with an emission linewidth of ~0.02 — 0.03 cm -1 , an average output power of ~55 mW, and a pulse repetition rate of 10 Hz. The two-photon excitation spectra at the 4 I 9/2 → 4 G 5/2 transition reveal the structure, which is absent upon one-photon excitation, which can be explained by different selection rules for some Stark — Stark transitions upon one- and two-photon absorption.
The excited-state absorption (ESA) in Nd 3+ :SrF 2 crystals was investigated in the 1280 — 1320 nm spectral wavelength range by selective laser excitation. It was found that, on excitation at wavelengths of 743 and 800.5 nm, there is no ESA in the ranges 1304 — 1309 and 1295 — 1297 nm. Weak ESA bands are observed in the 1297 — 1304 and 1309 — 1320 nm ranges and the differential ESA cross section does not exceed 0.3 × 10 -21 cm 2 . The results indicate that the ESA does not preclude the use of an Nd 3+ :SrF 2 crystal as the amplifying medium in the wavelength range 1280 — 1320 nm.
Accumulated photon echoes have been used to investigate the mechanisms of optical dephasing in CaF2 crystals activated by Nd3+ ions. Tunable picosecond laser radiation, which permits the selective excitation of various Nd3+ optical centers in the 4 I 9/2→4 G 5/2, 2 G 7/2 transition, is used. The optical phase relaxation times measured at temperatures from 9 to 50 K permit determination of the homogeneous widths of the transitions between the low-lying 4 I 9/2 Stark level and three excited 4 G 5/2, 2 G 7/2 levels, and calculation of the constants of the inter-Stark relaxation transitions in the ground and excited multiplets for the rhombic N and M Nd3+ centers in CaF2 crystals. An analysis of the temperature dependence of the homogeneous linewidth of the transitions between low-lying Stark levels of the ground and excited states shows that the mechanism of optical dephasing in the crystals investigated is described well by direct relaxation processes with resonant inter-Stark absorption of one phonon in the ground and excited states. At T=9 K, the homogeneous linewidth Γh in CaF2 crystals is almost an order of magnitude smaller than Γh in disordered CaF2-YF3 crystals. This difference can be attributed to the significantly greater spectral phonon density of states in disordered crystals.
The observation of two-photon absorption by a very efficient up-converted emission is reported for Ho3+{\mathrm{Ho}}^{3+}Ho3+ in CaF2{\mathrm{F}}_{2}F2​, SrF2{\mathrm{F}}_{2}F2​, and CdF2{\mathrm{F}}_{2}F2​ with both cw- and pulse-laser excitations. The two-photon excitation spectra are found to be highly structured and consist of two bands: The band AAA is excited by the dye-laser photons of frequencies 15 400-15 700 ${\mathrm{cm}}^{\ensuremath{-}1}$: The band BBB is excited by the dye-laser photons of frequencies 15 800-16 400 ${\mathrm{cm}}^{\ensuremath{-}1}$. No one-photon absorption is observed for Ho3+{\mathrm{Ho}}^{3+}Ho3+ in the above lattices at twice these frequencies. Studies of concentration dependence, temperature dependence, and dependence on the pulse repetition rate are used for the assignment of the band. The investigation shows that the two bands AAA and BBB arise from two different modes of two-photon excitation. The band AAA is assigned to arise from a sequential (stepwise) two-photon excitation $^{5}I_{8}\ensuremath{\rightarrow}^{5}F_{5}\ensuremath{\rightarrow}^{5}D_{2}$. The band BBB is assigned to arise from the direct two-photon absorption $^{5}I_{8}\ensuremath{\rightarrow}^{3}L_{8}$. Our results are in agreement with the prediction of the Judd-Ofelt theory of lanthanide transition intensities.
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.
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.