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Journal of the Optical Society of America B

Spectral hole burning in emerald

N E Rigby, Lucjan Dubicki, GORDON J. TROUP, Donald R Hutton, Neil B. Manson

Published May 1, 1992• 14 citations
Publisher

Abstract

Spectral hole burning in the 4A2–2E(2A) zero-phonon line for Cr3+ in Be3Al2(SiO3)6 is reported. Persistent holes with a linewidth of 0.5 GHz were observed when the crystal temperature was below 4 K. The burning is attributed to photoionization of Cr3+ from the 2E state and trapping of the released charge at other sites. The changes in the Coulomb field are the main factors contributing to the hole linewidth. High-resolution axial and transverse Zeeman measurements of the 4A2–2E(2A) transition performed by using the spectral hole are found to be consistent with the known g values.

DOI
10.1364/josab.9.000775

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Persistent spectral hole burning has been observed on the zero-phonon lines of the main site and several perturbed sites of ${\mathrm{Eu}}^{2+}$ in CaS:Eu single crystals. Hole burning occurs by two-step photoionization, can be strongly gated with IR irradiation, and takes place by excited-state absorption from the metastable ${4f}^{6}5d$ excited state to the conduction band followed by electron transport to ${\mathrm{Eu}}^{3+}$ centers which are the dominant traps. A complex hole structure consisting of a narrow feature (200 MHz), and broader features ($\ensuremath{\approx}5$ and $\ensuremath{\approx}100\mathrm{GHz}$) is observed. A mechanism is described for the occurrence of these unusually broad features. Time-varying internal electric fields which occur during the hole burning due to photoionization and trapping can lead to burning of holes at frequencies non-resonant with that of the laser. In addition, a mechanism for hole erasure, tunneling between Eu ions, is demonstrated. This mechanism is identified from the frequency dependence of the hole erasure which follows the ${\mathrm{Eu}}^{2+}$ absorption, and the linear dependence of the photoconductivity and hole erasure efficiency on irradiation power, both of which indicate erasure in a single-photon process.

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Side-hole to anti-hole conversion in time-resolved transient spectral hole-burning of emerald: ground state level versus excited state population storage in low magnetic fields

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Time-resolved transient spectral hole-burning experiments in zero field and in low magnetic fields B( parallelc) are reported for the chromium(III) R(1)-line, 2A((2)E)<-- 2A((4)A(2)) of Chatham lab created emerald, Be(3)Al(2)Si(6)O(18)ratio Cr(III)(0.0017% per weight), in the temperature range of 3 to 12 K. In low magnetic fields and temperatures >5 K conversion of side-holes to anti-holes is observed with progressing time. Anti-holes are due to the population stored in ground state levels. The dynamics of the hole pattern can be well modelled by a set of coupled differential equations for the levels of the (4)A(2) and (2)E multiplets. The measurements allow the simultaneous determination of g-factors and spin-lattice relaxation rates in the excited state and the ground state. At 6 K the relaxation times between the split +/-1/2 2A((2)E) excited state levels and +/-3/2 2A((4)A(2)) levels of the ground state are about 0.16 ms and 9 ms, respectively. From the temperature dependence it follows that the spin-lattice relaxation rates are dominated by Orbach processes in the experimental temperature range.

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Wavelength-selective excited-state lifetime measurements and absorption, luminescence, and hole-burning spectra of a natural African emerald crystal are reported. The (2)E excited-state lifetime displays an extreme wavelength dependence, varying from 190 to 37 μs within 1.8 nm of the R(1)-line. Overall, the excited state is strongly quenched, in comparison to laboratory-created emerald (τ=1.3 ms), with an average quenching rate of ∼6 × 10(3) s(-1) at 2.5 K. This quenching is attributed to photoinduced electron transfer caused by a relatively high concentration of Fe(2+) ions. The forward electron-transfer rate, k(f), from the nearest possible Fe(2+) sites at around 5 Å is estimated to be ∼20 × 10(3) s(-1) at 2.5 K. The photoreductive quenching of the excited Cr(3+) ions by Fe(2+) is followed by rapid electron back-transfer in the ground state upon deactivation. The exchange interaction based quenching can be modeled by assuming a random quencher distribution within the possible Fe(2+) sites with the forward electron-transfer rate, k(f), given as a function of acceptor-donor separation R by exp[(R(f)-R)/a(f)]; R(f) and a(f) values of 13.5 and 2.7 Å are obtained at 2.5 K. The electron transfer/back-transfer reorganizes the local crystal lattice, occasionally leading to a minor variation of the short-range structure around the Cr(3+) ions. This provides a mechanism for spectral hole-burning for which a moderately high quantum efficiency of about ∼0.005% is observed. Spectral holes are subject to spontaneous hole-filling and spectral diffusion, and both effects can be quantified within the standard two-level systems for non-photochemical hole-burning. Importantly, the absorbance increases on both sides of broad spectral holes, and isosbestic points are observed, in accord with the expected distribution of the "photoproduct" in a non-photochemical hole-burning process.

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Spectral hole burning on the $4{f}^{7}(^{8}S_{\frac{7}{2}})\ensuremath{\rightarrow}4{f}^{6}5d$ transition of ${\mathrm{Eu}}^{2+}$ is observed to occur by two mechanisms in Ca${\mathrm{F}}_{2}$:${\mathrm{Eu}}^{2+}$. At zero magnetic field, persistent spectral hole burning occurs by two-step photoionization where the hole burning survives cycling to room temperature. The observed hole spectrum is compared with a calculation which considers the small ${\mathrm{Eu}}^{2+}$ ground-state splitting and both the ground- and excited-state hyperfine interactions. In a magnetic field above 1 T, transient spectral hole burning occurs by population redistribution among the ground-state hyperfine levels. Long-lived (minutes) holes are observed for a half integral spin system. The resulting hole spectrum consists of holes, antiholes, and a nuclear spin-flip sideband and can be explained from the hyperfine interactions in the ground and excited states. The dominant hole decay occurs by phonon-induced transitions among hyperfine levels of the ${M}_{S}=\ensuremath{-}\frac{7}{2}$ and ${M}_{S}=\ensuremath{-}\frac{5}{2}$ electron-spin sublevels. Central hole linewidths of 200 MHz are observed at zero magnetic field. Hole linewidths at high magnetic fields are as narrow as 40 MHz but these are inhomogenously broadened by superhyperfine interactions with the $F$ nuclear spins. Estimates of hole-burning quantum efficiency are also obtained.

Physical review. B, Condensed matter•Sep 1, 1996•23 citations
Spectral hole burning in the 4A2–2E(2A) zero-phonon line for Cr3+ in Be3Al2(SiO3)6 is reported. Persistent holes with a linewidth of 0.5 GHz were observed when the crystal temperature was below 4 K. The burning is attributed to photoionization of Cr3+ from the 2E state and trapping of the released charge at other sites. The changes in the Coulomb field are the main factors contributing to the hole linewidth. High-resolution axial and transverse Zeeman measurements of the 4A2–2E(2A) transition performed by using the spectral hole are found to be consistent with the known g values.
Persistent spectral hole burning has been observed on the zero-phonon lines of the main site and several perturbed sites of Eu2+{\mathrm{Eu}}^{2+}Eu2+ in CaS:Eu single crystals. Hole burning occurs by two-step photoionization, can be strongly gated with IR irradiation, and takes place by excited-state absorption from the metastable 4f65d{4f}^{6}5d4f65d excited state to the conduction band followed by electron transport to Eu3+{\mathrm{Eu}}^{3+}Eu3+ centers which are the dominant traps. A complex hole structure consisting of a narrow feature (200 MHz), and broader features ($\ensuremath{\approx}5$ and $\ensuremath{\approx}100\mathrm{GHz}$) is observed. A mechanism is described for the occurrence of these unusually broad features. Time-varying internal electric fields which occur during the hole burning due to photoionization and trapping can lead to burning of holes at frequencies non-resonant with that of the laser. In addition, a mechanism for hole erasure, tunneling between Eu ions, is demonstrated. This mechanism is identified from the frequency dependence of the hole erasure which follows the Eu2+{\mathrm{Eu}}^{2+}Eu2+ absorption, and the linear dependence of the photoconductivity and hole erasure efficiency on irradiation power, both of which indicate erasure in a single-photon process.
Time-resolved transient spectral hole-burning experiments in zero field and in low magnetic fields B( parallelc) are reported for the chromium(III) R(1)-line, 2A((2)E)<-- 2A((4)A(2)) of Chatham lab created emerald, Be(3)Al(2)Si(6)O(18)ratio Cr(III)(0.0017% per weight), in the temperature range of 3 to 12 K. In low magnetic fields and temperatures >5 K conversion of side-holes to anti-holes is observed with progressing time. Anti-holes are due to the population stored in ground state levels. The dynamics of the hole pattern can be well modelled by a set of coupled differential equations for the levels of the (4)A(2) and (2)E multiplets. The measurements allow the simultaneous determination of g-factors and spin-lattice relaxation rates in the excited state and the ground state. At 6 K the relaxation times between the split +/-1/2 2A((2)E) excited state levels and +/-3/2 2A((4)A(2)) levels of the ground state are about 0.16 ms and 9 ms, respectively. From the temperature dependence it follows that the spin-lattice relaxation rates are dominated by Orbach processes in the experimental temperature range.
Wavelength-selective excited-state lifetime measurements and absorption, luminescence, and hole-burning spectra of a natural African emerald crystal are reported. The (2)E excited-state lifetime displays an extreme wavelength dependence, varying from 190 to 37 μs within 1.8 nm of the R(1)-line. Overall, the excited state is strongly quenched, in comparison to laboratory-created emerald (τ=1.3 ms), with an average quenching rate of ∼6 × 10(3) s(-1) at 2.5 K. This quenching is attributed to photoinduced electron transfer caused by a relatively high concentration of Fe(2+) ions. The forward electron-transfer rate, k(f), from the nearest possible Fe(2+) sites at around 5 Å is estimated to be ∼20 × 10(3) s(-1) at 2.5 K. The photoreductive quenching of the excited Cr(3+) ions by Fe(2+) is followed by rapid electron back-transfer in the ground state upon deactivation. The exchange interaction based quenching can be modeled by assuming a random quencher distribution within the possible Fe(2+) sites with the forward electron-transfer rate, k(f), given as a function of acceptor-donor separation R by exp[(R(f)-R)/a(f)]; R(f) and a(f) values of 13.5 and 2.7 Å are obtained at 2.5 K. The electron transfer/back-transfer reorganizes the local crystal lattice, occasionally leading to a minor variation of the short-range structure around the Cr(3+) ions. This provides a mechanism for spectral hole-burning for which a moderately high quantum efficiency of about ∼0.005% is observed. Spectral holes are subject to spontaneous hole-filling and spectral diffusion, and both effects can be quantified within the standard two-level systems for non-photochemical hole-burning. Importantly, the absorbance increases on both sides of broad spectral holes, and isosbestic points are observed, in accord with the expected distribution of the "photoproduct" in a non-photochemical hole-burning process.
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.
Spectral hole burning on the $4{f}^{7}(^{8}S_{\frac{7}{2}})\ensuremath{\rightarrow}4{f}^{6}5d$ transition of Eu2+{\mathrm{Eu}}^{2+}Eu2+ is observed to occur by two mechanisms in CaF2{\mathrm{F}}_{2}F2​:Eu2+{\mathrm{Eu}}^{2+}Eu2+. At zero magnetic field, persistent spectral hole burning occurs by two-step photoionization where the hole burning survives cycling to room temperature. The observed hole spectrum is compared with a calculation which considers the small Eu2+{\mathrm{Eu}}^{2+}Eu2+ ground-state splitting and both the ground- and excited-state hyperfine interactions. In a magnetic field above 1 T, transient spectral hole burning occurs by population redistribution among the ground-state hyperfine levels. Long-lived (minutes) holes are observed for a half integral spin system. The resulting hole spectrum consists of holes, antiholes, and a nuclear spin-flip sideband and can be explained from the hyperfine interactions in the ground and excited states. The dominant hole decay occurs by phonon-induced transitions among hyperfine levels of the ${M}_{S}=\ensuremath{-}\frac{7}{2}$ and ${M}_{S}=\ensuremath{-}\frac{5}{2}$ electron-spin sublevels. Central hole linewidths of 200 MHz are observed at zero magnetic field. Hole linewidths at high magnetic fields are as narrow as 40 MHz but these are inhomogenously broadened by superhyperfine interactions with the FFF nuclear spins. Estimates of hole-burning quantum efficiency are also obtained.