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Physical Review A

Optically induced homogeneous line narrowing

A. Szabó, Johann Heber

Published Jun 1, 1984• 19 citations
Publisher

Abstract

The ${R}_{1}$ dephasing time in ruby (0.05 wt.% ${\mathrm{Cr}}_{2}$${\mathrm{O}}_{3}$) is observed to increase by an order of magnitude when selected transitions of the ${R}_{2}$ line are pumped. Spin flip-flop dephasing in the ground state is suppressed by optically induced depopulation of the $^{4}A_{2}(\ifmmode\pm\else\textpm\fi{}\frac{1}{2})$ levels.

DOI
10.1103/physreva.29.3452

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Optically Induced Homogeneous Line Narrowing

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Recently there has been growing interest in optical dephasing (homogeneous linewidth) mechanisms in solids, both for scientific and technological1 reasons. The role of spin flip-flops (SFF) in producing dephasing has long been recognized in nuclear and electron magnetic resonance, and these studies are now being extended to optical transitions. In particular direct proof of host nuclear SFF optical dephasing of unlike dopant nuclei has been achieved by the observation of magic- angle homogeneous line narrowing.2 This work reports on a new technique for homogeneous line narrowing that demonstrates the existence of electronic SFF optical dephasing by like spins in ruby. The technique relies on selective depopulation of ground- state levels by R2 optical pumping as well as on novel spin thermodynamics in the ground state produced by the strong dipolar coupling between electron spins.

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Magnetic-field dependence of photon-echo decays in ruby

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Measurements of photon-echo decays in dilute ruby (${\mathrm{Cr}}_{2}$${\mathrm{O}}_{3}$ concentration of 0.018 at. %) in magnetic fields up to 29.5 kG are reported. Echoes from the $^{4}$${\mathit{A}}_{2}$(-3/2)${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$E,E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) and $^{4}$${\mathit{A}}_{2}$(-1/2)${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$E,E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) transitions have dephasing times (${\mathit{T}}_{2}$) that are directly proportional to the ratio of the magnetic field (B) to the temperature (T), for the range 2.5B/T20 kG/K. A transition in the decay from exponential to nonexponential behavior for B/T>10 kG/K is observed. Decay times for the $^{4}$${\mathit{A}}_{2}$(-1/2)${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$E,E(-1/2) echo are roughly a factor of 3 longer than for the $^{4}$${\mathit{A}}_{2}$(-3/2)${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$E,E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) echo. We attribute the lengthening of ${\mathit{T}}_{2}$ with increasing B/T to the suppression of Cr-Cr spin flip-flops as the population of the upper $^{4}$${\mathit{A}}_{2}$ levels decreases.

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Optical hole burning and spectral diffusion in ruby

A. Szabó, Rein K. Kaarli

Frequency-domain optical hole burning of the ${\mathit{R}}_{1}$ line ${[}^{4}$${\mathit{A}}_{2}$(-1/2)\ensuremath{\leftrightarrows}E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) transition] in dilute ruby is studied at 2 K and with a field of 3.6 kG applied along the c axis. A pump-probe (PP) technique is used with precise probe-frequency shifting obtained by an acousto-optic modulator. For sufficiently short PP pulses (50 \ensuremath{\mu}s), two holes (narrow and wide) are observed. The narrow (\ensuremath{\sim}20 kHz half width at half maximum at low power) hole-width dependence on Rabi frequency approximately agrees with that inferred from free-induction-decay measurements. For the present concentration (0.0034 wt. % ${\mathrm{Cr}}_{2}$${\mathrm{O}}_{3}$) 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.

Physical review. B, Condensed matter•Dec 1, 1991•48 citations

Numerical studies of optical dephasing in ruby

Shihua Huang, Alex Szabo

Journal of Luminescence•Jul 1, 1996•6 citations
The R1{R}_{1}R1​ dephasing time in ruby (0.05 wt.% {\mathrm{Cr}}_{2}$${\mathrm{O}}_{3}) is observed to increase by an order of magnitude when selected transitions of the R2{R}_{2}R2​ line are pumped. Spin flip-flop dephasing in the ground state is suppressed by optically induced depopulation of the 4A2(\ifmmode±\else\textpm\fi12)^{4}A_{2}(\ifmmode\pm\else\textpm\fi{}\frac{1}{2})4A2​(\ifmmode±\else\textpm\fi21​) levels.
Recently there has been growing interest in optical dephasing (homogeneous linewidth) mechanisms in solids, both for scientific and technological1 reasons. The role of spin flip-flops (SFF) in producing dephasing has long been recognized in nuclear and electron magnetic resonance, and these studies are now being extended to optical transitions. In particular direct proof of host nuclear SFF optical dephasing of unlike dopant nuclei has been achieved by the observation of magic- angle homogeneous line narrowing.2 This work reports on a new technique for homogeneous line narrowing that demonstrates the existence of electronic SFF optical dephasing by like spins in ruby. The technique relies on selective depopulation of ground- state levels by R2 optical pumping as well as on novel spin thermodynamics in the ground state produced by the strong dipolar coupling between electron spins.
Measurements of photon-echo decays in dilute ruby (Cr2{\mathrm{Cr}}_{2}Cr2​O3{\mathrm{O}}_{3}O3​ concentration of 0.018 at. %) in magnetic fields up to 29.5 kG are reported. Echoes from the 4^{4}4A2{\mathit{A}}_{2}A2​(-3/2)${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$E,E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) and 4^{4}4A2{\mathit{A}}_{2}A2​(-1/2)${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$E,E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) transitions have dephasing times (T2{\mathit{T}}_{2}T2​) that are directly proportional to the ratio of the magnetic field (B) to the temperature (T), for the range 2.5B/T20 kG/K. A transition in the decay from exponential to nonexponential behavior for B/T>10 kG/K is observed. Decay times for the 4^{4}4A2{\mathit{A}}_{2}A2​(-1/2)${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$E,E(-1/2) echo are roughly a factor of 3 longer than for the 4^{4}4A2{\mathit{A}}_{2}A2​(-3/2)${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$E,E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) echo. We attribute the lengthening of T2{\mathit{T}}_{2}T2​ with increasing B/T to the suppression of Cr-Cr spin flip-flops as the population of the upper 4^{4}4A2{\mathit{A}}_{2}A2​ levels decreases.
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.