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arXiv:2007.07493

Spin thermometry and spin relaxation of optically detected Cr3+ ions in Al2O3 (ruby)

Vikas K. Sewani, Rainer Stöhr, Roman L. Kolesov, Hyma Harish Vallabhapurapu, Tobias Simmet, Andrea Morello, Arne Laucht

Published Jul 15, 2020• 1 citation
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Abstract

Paramagnetic ions in solid state crystals form the basis for many advanced technologies like lasers, masers, frequency standards, and quantum-enhanced sensors. One of the most-studied examples is the Cr3+ ion in sapphire (Al2O3), also known as ruby, which has been intensely studied in the 1950s and 1960s. However, despite decades of research on ruby, some of its fundamental optical and spin properties have not been characterized at ultra low-temperatures, yet. In this article, we present optical measurements on a ruby crystal in a dilution refrigerator at ultra-low temperatures down to 20 mK. Analysing the relative populations of its 4A2 ground state spin levels, we extract a lattice temperature of 143(7) mK under continuous laser excitation. We perform spin lattice relaxation T1 measurements in excellent agreement with the direct, one-phonon model. Furthermore, we perform optically detected magnetic resonance measurements showing magnetically driven transitions between the ground state spin levels for various magnetic fields. Our measurements characterize some of ruby's low temperature spin properties, and lay the foundations for more advanced spin control experiments.

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Ultra-slow electron spin-lattice relaxation in a low magnetic field enables massive optical spin polarization in the 4A2 ground state of Cr3+ in ruby*

Hans Riesen

Abstract Ruby (α-Al2O3 doped with Cr3+) has been an archetypal material in the development of optical spectroscopy of the solid state for the last 150 years and was the first material that was demonstrated to lase. Notwithstanding the vast literature on ruby, one effect was somehow missed: in a magnetic field B ∥c ∼ 235 mT, the spin-lattice relaxation time T 1 for the |+3/2⟩ level in the 4A2 ground state is massively lengthened to ∼12 s at 1.4 K as demonstrated in this study. This very long relaxation time enables optical pumping of the |+3/2⟩ level via the R 1(±1/2) lines and a considerable +3/2 spin polarization of ∼95% is readily achieved. The observed magnetic field dependence can be quantitatively described using the one-phonon relaxation process.

Journal of Physics Condensed Matter•Jan 19, 2022•2 citations

Paramagnetic Spectra of Substituted Sapphires-Part I: Ruby*

E. O. Schulz-DuBois

The paramagnetic resonance properties of Cr+++ions in Al2O3(ruby) were investigated theoretically and experimentally in order to obtain information necessary for the application of this material as active material in a three-level solid-state maser (3LSSM). Numerically computed energy levels, together with their associated eigenvectors, are presented as a function of applied magnetic field for various orientations of the magnetic field with respect to the crystalline symmetry axis. A more detailed discussion is devoted to energy levels, eigenvectors and transition probabilities at angles O°, 54.74° and 90°, where certain simple relations and symmetries hold. Paramagnetic spectra for signal frequencies between 5 and 24 kmc are shown; agreement between computed and measured resonance fields is satisfactory.

Bell System Technical Journal•Jan 1, 1959•120 citations

Optical detection and phonon bottleneck of the direct decay within the E¯(E2) state of ruby

J. I. Dijkhuis, K. Huibregtse, H. W. de Wijn

Direct relaxation within the optically excited $\overline{E}(^{2}E)$ level of 700-ppm ruby is investigated in magnetic fields up to 65 kG making an angle to the $c$ axis. At low pump intensities, the experimental relaxation rates are found to be in excellent agreement with the theory by Blume et al., predicting a fifth-power dependence on field and a ${cos}^{3}\ensuremath{\theta}{sin}^{2}\ensuremath{\theta}$ dependence on orientation. The observed proportionality constant of 4.7 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}19}$ ${\mathrm{G}}^{\ensuremath{-}5}$${\mathrm{s}}^{\ensuremath{-}1}$ is close to the theoretical estimate based on static experiments in ruby. When increasing optical pumping, the phonon-bath conduction is demonstrated to become the limiting process due to resonant trapping of the phonons. Following pulsed excitation, a prolonging of the decay time by a factor up to 13 is attained at excited-state concentrations ${N}^{*}\ensuremath{\sim}2\ifmmode\times\else\texttimes\fi{}{10}^{17}/{\mathrm{cm}}^{3}$. In stationary experiments, a nonlinear increase with ${N}^{*}$ is observed of the equilibrium population of the upper Zeeman level of $\overline{E}$ to over a decade above the nonbottlenecked value, corresponding to bottlenecking factors of over \ensuremath{\sim}200. Under the assumption of a constant phonon lifetime of the order of the flight time through the illuminated region, rate equations appear to consistently account for the experiments. A Gaussian-type resonance line, fully homogenized supposedly by magnetic interactions with the surrounding Al nuclei and ${\mathrm{Cr}}^{3+}$ ions, explains the lattice-bath equilibration. Finally, the prospect is discussed of using the $\overline{E}$ direct transition in ruby as a tunable phonon generator and detector with bandwidth 0.002 ${\mathrm{cm}}^{\ensuremath{-}1}$ in the practical frequency range of 2-15 ${\mathrm{cm}}^{\ensuremath{-}1}$.

Physical review. B, Condensed matter•Sep 1, 1979•19 citations

Optical-Microwave Double-Resonance Studies of Ruby

A. Szabó

Studies of the resonant interaction of radiation from a liquid-nitrogen-cooled ruby laser with a ruby crystal in the temperature range 4.2°–100°K are described. The interaction was measured by observation of the change which occurs in the Cr3+ ground state EPR absorption on laser irradiation. At low radiation intensities, the temperature dependence of this change is shown to be determined by the well-known thermal tuning behavior of the R lines. Precise measurement of the relative laser and ruby-sample absorption frequencies by this technique of double-resonance spectroscopy is described. Under optical saturation conditions, additional temperature-dependent pumping effects occur at low temperatures. In particular, as the ruby temperature is increased from 4.2° to 40°K, the laser-induced change in EPR absorption is observed to undergo a large increase. This increase cannot be explained by a relative thermal shift of the laser and absorption frequencies which is known to be very small in this temperature range. The phenomena are attributed in part to the temperature-dependent homogeneous linewidth which determines the widths of the holes burnt into the inhomogeneous strain-broadened R lines. Calculations indicate that the related temperature-dependent thermalization process which redistributes excited Cr3+ among the 2E levels quantitatively accounts for most of the increase.

Journal of Applied Physics•Nov 1, 1968•3 citations

Optically pump-induced athermal and nonresonant refractive index changes in the reference Cr-doped laser materials: Cr:GSGG and ruby

Thomas Godin, R. Moncorgé, J.L. Doualan +4 more

The refractive index of most ion-doped materials increases with the excited state population. This effect was studied in many laser materials, particularly those doped with Cr3+ and rare earth ions, using several techniques, such as interferometry, wave mixing, and Z-scans. This refractive index variation is athermal (has an electronic origin) and is associated with the difference in the polarizabilites of the Cr3+ ion in its excited and ground states, Δαp. The Cr3+ optical transitions in the visible domain are electric-dipole forbidden, and they have low oscillator strengths. Therefore, the major contribution to Δαp has been assigned to allowed transitions to charge transfer bands (CTBs) in the UV with strengths ∼3 orders of magnitude higher. Although this CTB model qualitatively explains the main observations, it was never quantitatively tested. In order to further investigate the physical origin of Δαp in Cr3+-doped crystals, excited state absorption (ESA) and Z-scan measurements were thus performed in Cr:Al2O3 (ruby) and Cr:GSGG. Cr:GSGG was selected because of the proximity of its E2 and T24 emitting levels, and thus the possibility to explore the role of the spin selection rule in the ESA spectra and the resulting variations in polarizability by comparing low and room temperature data, which were never reported before. On the other hand, Cr:Al2O3 (ruby) was selected because it is the only crystal for which it is possible to obtain CTB absorption data from both ground and excited states, and thus for which it is possible to check the CTB model more accurately. Thanks to these more accurate and more complete data, we came to the first conclusion that the spin selection rule does not play any significant role in the variation of the polarizability with the E2–T24 energy mismatch. We also discovered that using the CTB model in the case of ruby would lead to a negative Δαp value, which is contrary to all refractive index variation (including Z-scan) measurements.

Journal of the Optical Society of America B•Apr 23, 2012•22 citations

Electron spin dynamics of Ce3+ ions in YAG crystals studied by pulse-EPR and pump-probe Faraday rotation

Д. В. Азамат, V. V. Belykh, Dmitri R. Yakovlev +6 more

The spin relaxation dynamics of ${\mathrm{Ce}}^{3+}$ ions in heavily cerium-doped YAG crystals is studied using pulse-electron paramagnetic resonance and time-resolved pump-probe Faraday rotation. Both techniques address the $4f$ ground state, while pump-probe Faraday rotation also provides access to the excited $5d$ state. We measure a millisecond spin-lattice relaxation time ${T}_{1}$, a microsecond spin coherence time ${T}_{2}$, and a $\ensuremath{\sim}10$ ns inhomogeneous spin dephasing time ${T}_{2}^{*}$ for the ${\mathrm{Ce}}^{3+}$ ground state at low temperatures. The spin-lattice relaxation of ${\mathrm{Ce}}^{3+}$ ions is due to modified Raman processes involving the optical phonon mode at $\ensuremath{\sim}\phantom{\rule{0.16em}{0ex}}125\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. The relaxation at higher temperature goes through a first excited level of the $^{2}\mathrm{F}_{\frac{5}{2}}$ term at about $\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\approx}228\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. Effects provided by the hyperfine interaction of the ${\mathrm{Ce}}^{3+}$ with the $^{27}\mathrm{Al}$ nuclei are observed.

arXiv:1709.01997•Physical review. B./Physical review. B•Aug 30, 2017•11 citations
Paramagnetic ions in solid state crystals form the basis for many advanced technologies like lasers, masers, frequency standards, and quantum-enhanced sensors. One of the most-studied examples is the Cr3+ ion in sapphire (Al2O3), also known as ruby, which has been intensely studied in the 1950s and 1960s. However, despite decades of research on ruby, some of its fundamental optical and spin properties have not been characterized at ultra low-temperatures, yet. In this article, we present optical measurements on a ruby crystal in a dilution refrigerator at ultra-low temperatures down to 20 mK. Analysing the relative populations of its 4A2 ground state spin levels, we extract a lattice temperature of 143(7) mK under continuous laser excitation. We perform spin lattice relaxation T1 measurements in excellent agreement with the direct, one-phonon model. Furthermore, we perform optically detected magnetic resonance measurements showing magnetically driven transitions between the ground state spin levels for various magnetic fields. Our measurements characterize some of ruby's low temperature spin properties, and lay the foundations for more advanced spin control experiments.
Abstract Ruby (α-Al2O3 doped with Cr3+) has been an archetypal material in the development of optical spectroscopy of the solid state for the last 150 years and was the first material that was demonstrated to lase. Notwithstanding the vast literature on ruby, one effect was somehow missed: in a magnetic field B ∥c ∼ 235 mT, the spin-lattice relaxation time T 1 for the |+3/2⟩ level in the 4A2 ground state is massively lengthened to ∼12 s at 1.4 K as demonstrated in this study. This very long relaxation time enables optical pumping of the |+3/2⟩ level via the R 1(±1/2) lines and a considerable +3/2 spin polarization of ∼95% is readily achieved. The observed magnetic field dependence can be quantitatively described using the one-phonon relaxation process.
The paramagnetic resonance properties of Cr+++ions in Al2O3(ruby) were investigated theoretically and experimentally in order to obtain information necessary for the application of this material as active material in a three-level solid-state maser (3LSSM). Numerically computed energy levels, together with their associated eigenvectors, are presented as a function of applied magnetic field for various orientations of the magnetic field with respect to the crystalline symmetry axis. A more detailed discussion is devoted to energy levels, eigenvectors and transition probabilities at angles O°, 54.74° and 90°, where certain simple relations and symmetries hold. Paramagnetic spectra for signal frequencies between 5 and 24 kmc are shown; agreement between computed and measured resonance fields is satisfactory.
Direct relaxation within the optically excited E‾(2E)\overline{E}(^{2}E)E(2E) level of 700-ppm ruby is investigated in magnetic fields up to 65 kG making an angle to the ccc axis. At low pump intensities, the experimental relaxation rates are found to be in excellent agreement with the theory by Blume et al., predicting a fifth-power dependence on field and a ${cos}^{3}\ensuremath{\theta}{sin}^{2}\ensuremath{\theta}$ dependence on orientation. The observed proportionality constant of 4.7 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}19}$ ${\mathrm{G}}^{\ensuremath{-}5}$${\mathrm{s}}^{\ensuremath{-}1}$ is close to the theoretical estimate based on static experiments in ruby. When increasing optical pumping, the phonon-bath conduction is demonstrated to become the limiting process due to resonant trapping of the phonons. Following pulsed excitation, a prolonging of the decay time by a factor up to 13 is attained at excited-state concentrations ${N}^{*}\ensuremath{\sim}2\ifmmode\times\else\texttimes\fi{}{10}^{17}/{\mathrm{cm}}^{3}$. In stationary experiments, a nonlinear increase with N∗{N}^{*}N∗ is observed of the equilibrium population of the upper Zeeman level of E‾\overline{E}E to over a decade above the nonbottlenecked value, corresponding to bottlenecking factors of over \ensuremath{\sim}200. Under the assumption of a constant phonon lifetime of the order of the flight time through the illuminated region, rate equations appear to consistently account for the experiments. A Gaussian-type resonance line, fully homogenized supposedly by magnetic interactions with the surrounding Al nuclei and Cr3+{\mathrm{Cr}}^{3+}Cr3+ ions, explains the lattice-bath equilibration. Finally, the prospect is discussed of using the E‾\overline{E}E direct transition in ruby as a tunable phonon generator and detector with bandwidth 0.002 ${\mathrm{cm}}^{\ensuremath{-}1}$ in the practical frequency range of 2-15 ${\mathrm{cm}}^{\ensuremath{-}1}$.
Studies of the resonant interaction of radiation from a liquid-nitrogen-cooled ruby laser with a ruby crystal in the temperature range 4.2°–100°K are described. The interaction was measured by observation of the change which occurs in the Cr3+ ground state EPR absorption on laser irradiation. At low radiation intensities, the temperature dependence of this change is shown to be determined by the well-known thermal tuning behavior of the R lines. Precise measurement of the relative laser and ruby-sample absorption frequencies by this technique of double-resonance spectroscopy is described. Under optical saturation conditions, additional temperature-dependent pumping effects occur at low temperatures. In particular, as the ruby temperature is increased from 4.2° to 40°K, the laser-induced change in EPR absorption is observed to undergo a large increase. This increase cannot be explained by a relative thermal shift of the laser and absorption frequencies which is known to be very small in this temperature range. The phenomena are attributed in part to the temperature-dependent homogeneous linewidth which determines the widths of the holes burnt into the inhomogeneous strain-broadened R lines. Calculations indicate that the related temperature-dependent thermalization process which redistributes excited Cr3+ among the 2E levels quantitatively accounts for most of the increase.
The refractive index of most ion-doped materials increases with the excited state population. This effect was studied in many laser materials, particularly those doped with Cr3+ and rare earth ions, using several techniques, such as interferometry, wave mixing, and Z-scans. This refractive index variation is athermal (has an electronic origin) and is associated with the difference in the polarizabilites of the Cr3+ ion in its excited and ground states, Δαp. The Cr3+ optical transitions in the visible domain are electric-dipole forbidden, and they have low oscillator strengths. Therefore, the major contribution to Δαp has been assigned to allowed transitions to charge transfer bands (CTBs) in the UV with strengths ∼3 orders of magnitude higher. Although this CTB model qualitatively explains the main observations, it was never quantitatively tested. In order to further investigate the physical origin of Δαp in Cr3+-doped crystals, excited state absorption (ESA) and Z-scan measurements were thus performed in Cr:Al2O3 (ruby) and Cr:GSGG. Cr:GSGG was selected because of the proximity of its E2 and T24 emitting levels, and thus the possibility to explore the role of the spin selection rule in the ESA spectra and the resulting variations in polarizability by comparing low and room temperature data, which were never reported before. On the other hand, Cr:Al2O3 (ruby) was selected because it is the only crystal for which it is possible to obtain CTB absorption data from both ground and excited states, and thus for which it is possible to check the CTB model more accurately. Thanks to these more accurate and more complete data, we came to the first conclusion that the spin selection rule does not play any significant role in the variation of the polarizability with the E2–T24 energy mismatch. We also discovered that using the CTB model in the case of ruby would lead to a negative Δαp value, which is contrary to all refractive index variation (including Z-scan) measurements.
The spin relaxation dynamics of Ce3+{\mathrm{Ce}}^{3+}Ce3+ ions in heavily cerium-doped YAG crystals is studied using pulse-electron paramagnetic resonance and time-resolved pump-probe Faraday rotation. Both techniques address the 4f4f4f ground state, while pump-probe Faraday rotation also provides access to the excited 5d5d5d state. We measure a millisecond spin-lattice relaxation time T1{T}_{1}T1​, a microsecond spin coherence time T2{T}_{2}T2​, and a $\ensuremath{\sim}10$ ns inhomogeneous spin dephasing time T2∗{T}_{2}^{*}T2∗​ for the Ce3+{\mathrm{Ce}}^{3+}Ce3+ ground state at low temperatures. The spin-lattice relaxation of Ce3+{\mathrm{Ce}}^{3+}Ce3+ ions is due to modified Raman processes involving the optical phonon mode at $\ensuremath{\sim}\phantom{\rule{0.16em}{0ex}}125\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. The relaxation at higher temperature goes through a first excited level of the 2F52^{2}\mathrm{F}_{\frac{5}{2}}2F25​​ term at about $\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\approx}228\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. Effects provided by the hyperfine interaction of the Ce3+{\mathrm{Ce}}^{3+}Ce3+ with the 27Al^{27}\mathrm{Al}27Al nuclei are observed.