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Physical review. B, Condensed matter

Spectral hole burning by population storage in Zeeman sublevels of LaFsub3: Nd3+

R. M. Macfarlane, J. C. Vial

Published Sep 1, 1987• 33 citations
Publisher

Abstract

We demonstrate a new mechanism for optical spectral hole burning in which population is stored in electronic Zeeman sublevels. This is shown by optical pumping the ground-state Kramers doublet of the $^{4}\mathrm{I}_{9/2}$${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$${\mathrm{H}}_{11/2}$ (6248.9 A\r{}) and $^{4}\mathrm{I}_{9/2}$${\mathrm{\ensuremath{\leftrightarrows}}}^{4}$${\mathrm{G}}_{5/2}$ (5777.1 A\r{}) transitions of ${\mathrm{LaF}}_{3}$:${\mathrm{Nd}}^{3+}$ with a narrow-band cw dye laser. Experiments were carried out at 1.6 K in external fields of \ensuremath{\sim}100 G. The Zeeman shift of the resulting antiholes and holes makes an assignment of these structures possible. Hole recovery times of hundreds of milliseconds are shorter than expected at these low temperatures and fields and provide evidence for optical spectral diffusion caused by mutual spin flips in the ground state.

DOI
10.1103/physrevb.36.3511

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Physical review. B, Condensed matter•Dec 1, 1991•48 citations
We demonstrate a new mechanism for optical spectral hole burning in which population is stored in electronic Zeeman sublevels. This is shown by optical pumping the ground-state Kramers doublet of the ^{4}\mathrm{I}_{9/2}$${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$${\mathrm{H}}_{11/2} (6248.9 A\r{}) and ^{4}\mathrm{I}_{9/2}$${\mathrm{\ensuremath{\leftrightarrows}}}^{4}$${\mathrm{G}}_{5/2} (5777.1 A\r{}) transitions of LaF3{\mathrm{LaF}}_{3}LaF3​:Nd3+{\mathrm{Nd}}^{3+}Nd3+ with a narrow-band cw dye laser. Experiments were carried out at 1.6 K in external fields of \ensuremath{\sim}100 G. The Zeeman shift of the resulting antiholes and holes makes an assignment of these structures possible. Hole recovery times of hundreds of milliseconds are shorter than expected at these low temperatures and fields and provide evidence for optical spectral diffusion caused by mutual spin flips in the ground state.
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We have measured spectral diffusion in Er3+-doped YLiF4 from the time dependence of spectral hole shapes. The holes were burned in the absorption corresponding to the transition between the lowest Zeeman components of the 4I15/2(1) and 4F9/2(1) levels of Er3+:YLiF4 at 15298.6 cm−1 and were scanned by rapid Zeeman tuning of the erbium energy levels. In an external magnetic field of 26 kG, which supresses erbium–erbium spin flips, the mechanism for spectral diffusion involved local field fluctuations that are due to 19F nuclear spin flips in the perturbing field of the erbium electron spins. Numerical simulation of the fluorine spin dynamics gives semiquantitative agreement with the observed time-dependent hole shapes.
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Frequency-domain optical hole burning of the R1{\mathit{R}}_{1}R1​ line [4{[}^{4}[4A2{\mathit{A}}_{2}A2​(-1/2)\ensuremath{\leftrightarrows}E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) transition] in dilute ruby is studied at 2 K and with a field of 3.6 kG applied along the c axis. A pump-probe (PP) technique is used with precise probe-frequency shifting obtained by an acousto-optic modulator. For sufficiently short PP pulses (50 \ensuremath{\mu}s), two holes (narrow and wide) are observed. The narrow (\ensuremath{\sim}20 kHz half width at half maximum at low power) hole-width dependence on Rabi frequency approximately agrees with that inferred from free-induction-decay measurements. For the present concentration (0.0034 wt. % Cr2{\mathrm{Cr}}_{2}Cr2​O3{\mathrm{O}}_{3}O3​) and field, the narrow hole width is determined by fluctuating fields produced by Cr-Cr spin flips [A. Szabo, T. Muramoto, and R. Kaarli, Phys. Rev. B 42, 7769 (1990)]. When the PP delay time is varied, the amplitude of the narrow hole decays with a 1/e time constant of \ensuremath{\sim}300 \ensuremath{\mu}s compared to the E\ifmmode\bar\else\textasciimacron\fi{} fluorescence lifetime of 4 ms. The wide hole (\ensuremath{\sim}500 kHz half width at half maximum) is due to Al-Cr superhyperfine interactions and is created by a spectral diffusion mechanism driven by Al-spin flipping in the host lattice.