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Sequential two-photon (730-800-nm) excitation of Nd 3+ :SrF 2

J. H. Schloss, Lloyd L. Chase, Stephen A. Payne

Published May 21, 1990• 0 citations
OpenAlex

Abstract

Sequential two-photon absorption has been recently observed when pumping Nd3+:YAG at ≈ 740 nm.1 In this work, Nd3+:SrF2 is excited with a pulsed (150-μs).

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Journal of the Optical Society of America B•Jul 1, 1999•19 citations
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.
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.
High-power, picosecond-pulse excitation was used to study the dynamics of the pumping and decay processes in Y3{\mathrm{Y}}_{3}Y3​Al5{\mathrm{Al}}_{5}Al5​O12{\mathrm{O}}_{12}O12​:Nd3+{\mathrm{Nd}}^{3+}Nd3+. The observed fluorescence spectral lines are assigned to transitions from three different metastable states excited by both single-photon and two-photon absorption. The branching ratios, lifetimes, and quantum efficiencies of the metastable states are obtained from the data as well as the two-photon absorption cross sections. The results provide useful information concerning ultraviolet pumping efficiencies of the Nd-YAG (Nd-doped yttrium aluminum garnet) laser transition and the $5d\ensuremath{-}4f$ nonradiative decay rate for this material. In addition, the time-resolved spectroscopy method employed here is shown to be an extremely sensitive technique for obtaining two-photon absorption cross sections.
The mechanism for refractive-index changes that accompany changes in population during pumping and amplification of an optical beam is studied in a Nd:YAG laser crystal by both resonant four-wave mixing and interferometric techniques. It is found that these refractive-index changes (connected with the difference in polarizability of excited and unexcited Nd3+ ions) have two components: a small noninertial component that accompanies an amplified optical pulse and the major changes that are intensified with a delay time of ∼3 µs. The latter effect is explained by population (or depopulation) of a higher-lying energy level 2(F2)5/2 of the 4f electron shell of Nd3+ ions, which has large polarizability in near-IR and visible light. The real part of the nonlinear optical resonant susceptibility of the inverted Nd:YAG caused by the refractive-index changes is also discussed.