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Physical Review Letters

Photochemical and Population Hole Burning in the Zero-Phonon Line of a Color Center— F3+ in NaF

R. M. Macfarlane, Robert M. Shelby

Published Mar 19, 1979• 61 citations
Publisher

Abstract

We report reversible hole burning in the inhomogeneously broadened zero-phonon line of ${{F}_{3}}^{+}$ in NaF at 5456 \AA{}. The hole recovery time shows two components: 2.5 sec assigned to triplet-state relaxation and 70 min assigned to electron tunneling from an adjacent center. These holes were used to measure the homogeneous linewidth (17 MHz) and the linear Stark effect. We find the excited $^{1}E$ level has a distribution of zero-field splittings inside the inhomogeneous lines, which quenches the first-order Zeeman effect.

DOI
10.1103/physrevlett.42.788

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NASA STI/Recon Technical Report N•Feb 1, 1983•0 citations
We report reversible hole burning in the inhomogeneously broadened zero-phonon line of F3+{{F}_{3}}^{+}F3​+ in NaF at 5456 \AA{}. The hole recovery time shows two components: 2.5 sec assigned to triplet-state relaxation and 70 min assigned to electron tunneling from an adjacent center. These holes were used to measure the homogeneous linewidth (17 MHz) and the linear Stark effect. We find the excited 1E^{1}E1E level has a distribution of zero-field splittings inside the inhomogeneous lines, which quenches the first-order Zeeman effect.
We have measured the optical dephasing time T2{T}_{2}T2​ of the $^{1}A_{1}\ensuremath{\leftrightarrow}^{1}E$ zero-phonon transition of the F3+{F}_{3}^{+}F3+​ color center in NaF by optical free-induction decay. In this way we eliminate the effect of the 54-GHz inhomogeneous broadening, and find a homogeneous linewidth of 20 \ifmmode\pm\else\textpm\fi{} 5 MHz ${T}_{2}=16\ifmmode\pm\else\textpm\fi{}4$ nsec). We have also measured a spontaneous emission lifetime of ${T}_{1}=10\ifmmode\pm\else\textpm\fi{}2$ nsec. In the range 1.5-4 K, our results are consistent with the relation T2=2T1{T}_{2}=2{T}_{1}T2​=2T1​, indicating that optical dephasing is limited by population-decay processes. This relation was even more clearly demonstrated by performing the same experiment on the DDD lines of sodium vapor at 3 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}5}$ Torr, where the effects of collisions are negligible. We find that the dephasing is again limited by radiative decay, and that ${T}_{2}(32\ifmmode\pm\else\textpm\fi{}3 \mathrm{nsec})=2{T}_{1}(16.3\ifmmode\pm\else\textpm\fi{}0.4 \mathrm{nsec})$.
A polarized laser beam can bleach narrow, long-lived, anisotropic holes in the 607-nm zero-phonon line of the NaF N1{N}_{1}N1​ center. The width of these holes is twice the homogeneous linewidth, and three orders of magnitude less than the inhomogeneous width of the line. We report a polarization-spectroscopy technique which detects the dichroism and birefringence of the hole with better sensitivity than absorption spectroscopy. A simple rateequation model is developed to account for hole burning, but the recovery of the initial isotropic absorption profile appears to be a complex, slow, and intractable process.
Luminescence and absorption spectra of LiF crystals with F2− color centers (CCs) were studied in the 14–300 K temperature range. The Huang–Rhys factors measured from absorption and emission spectra were equal in magnitude and calculated to be 3.2 and 2.72 at 77 and 300 K, respectively. It was shown that below 40 K inhomogeneous broadening of the zero phonon line of the F2− CC prevails over homogeneous broadening. Inhomogeneous broadening of the zero phonon line was observed to vary from 5 to 15 cm−1 for different crystal preparations. Persistent spectral hole burning stable at room temperature was realized in LiF:F2− crystals.
With a ring dye laser persistent spectral hole-burning was measured by fluorescence excitation spectroscopy in the zero-phonon lines of the 2llg ↔ 2llu transition in KI:S2 − and of the 3H4 → 3P0 transition of a defect center with three D− ions in SrF2:Pr3+:D−and also in the zero-phonon line at 462.5 nm of a color center in neutron-irradiated and annealed α-Al2O3. In all three lines holes with a width in the order of 1 GHz could be obtained at 1.5 K with single frequency laser. With broad-band laser in KI:S2 − and SrF2:Pr3+:D− spectral redistribution within the full range of inhomogeneous broadening could be observed which are explained by a photophysical model based on barrier crossing in asymmetric double-well-potentials. In the case of sapphire a photobleaching process is dominant which is effective also for nonselective excitation, and the holes are thermoresistant up to 300 K.