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Physical review. B, Condensed matter

Spectral hole burning of Eu2+ in Ca F2

D.M. Boye, R. M. Macfarlane, Yazhou Sun, Richard S. Meltzer

Published Sep 1, 1996• 23 citations
Publisher

Abstract

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.

DOI
10.1103/physrevb.54.6263

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Spectral hole burning on the 4f7(8S72)\ensuremath→4f65d4{f}^{7}(^{8}S_{\frac{7}{2}})\ensuremath{\rightarrow}4{f}^{6}5d4f7(8S27​​)\ensuremath→4f65d 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 MS=\ensuremath−72{M}_{S}=\ensuremath{-}\frac{7}{2}MS​=\ensuremath−27​ and MS=\ensuremath−52{M}_{S}=\ensuremath{-}\frac{5}{2}MS​=\ensuremath−25​ 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.
Persistent and time-resolved transient holes were burnt into the 1D2^{1}\mathrm{D}_{2}1D2​${\ensuremath{\leftarrow}}^{3}$H4{\mathrm{H}}_{4}H4​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+ and the 5D0^{5}\mathrm{D}_{0}5D0​${\ensuremath{\leftarrow}}^{7}$F0{\mathrm{F}}_{0}F0​ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ in silicate glasses. The holewidths were studied as a function of burning-fluence density, wavelength, and temperature between 0.4 and 12 K. Transient holes arising from optical pumping of ground-state nuclear hyperfine levels were found for both ions at T3 K. Their lifetime decreases with increasing temperature. They are accompanied by symmetrically placed antiholes. For Eu3+{\mathrm{Eu}}^{3+}Eu3+, two pairs of antiholes were found which are attributed to the two europium isotopes, 151Eu^{151}\mathrm{Eu}151Eu and 153Eu^{153}\mathrm{Eu}153Eu. For Pr3+{\mathrm{Pr}}^{3+}Pr3+, an additional mechanism leading to persistent hole burning dominates above 3 K. The holewidth follows a ${\mathit{T}}^{(1.3\ifmmode\pm\else\textpm\fi{}0.1)}$ dependence for Pr3+{\mathrm{Pr}}^{3+}Pr3+ and a ${\mathit{T}}^{(1.0\ifmmode\pm\else\textpm\fi{}0.1)}$ dependence for Eu3+{\mathrm{Eu}}^{3+}Eu3+. The temperature dependence is the same as that of the contribution of the two-level systems to the specific heat measured on the same samples and in the same temperature range. The quadrupole splittings of the 7F0^{7}\mathrm{F}_{0}7F0​ ground state and the crystal-field splittings of the 7F1^{7}\mathrm{F}_{1}7F1​ and 7F2^{7}\mathrm{F}_{2}7F2​ levels of Eu3+{\mathrm{Eu}}^{3+}Eu3+ as a function of excitation wavelength indicate that the strength of the noncubic component of the crystal field varies monotonically for excitation across the 5D0^{5}\mathrm{D}_{0}5D0​${\ensuremath{\leftarrow}}^{7}$F0{\mathrm{F}}_{0}F0​ absorption band, falling to zero at the long-wavelength edge. The hole width shows a similar variation with excitation frequency. No influence of the experimental time scale on the hole width was detected for either sample between ${10}^{\mathrm{\ensuremath{-}}2}$ and 102{10}^{2}102 s.
Optical hole burning has been observed in the 5941-A transition of Pr(3+) in a charge-compensated tetragonal site of CaF(2) . The Pr(3+) ground state is doubly degenerate and shows a large first-order hyperfine splitting, which is clearly resolved because of the very narrow inhomogeneous linewidth of 650 MHz. The hole burning involves a new mechanism, in which optically induced spin flips of neighboring nuclei (here (19)F) shift the optical transition frequency outside its homogeneous linewidth. This mechanism was confirmed by optical rf double resonance.
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.
Photon-gated hole burning, or selective bleaching enabled by a second light source, has been observed in Co2+{\mathrm{Co}}^{2+}Co2+ in tetrahedral sites of LiGa5{\mathrm{LiGa}}_{5}LiGa5​O8{\mathrm{O}}_{8}O8​. This leads to long-lived spectral holes with a width of \ensuremath{\sim}1 GHz at 1.6 K. It is proposed that two-step photoionization of Co2+{\mathrm{Co}}^{2+}Co2+ is responsible for the hole burning. Much narrower (\ensuremath{\sim}40 MHz) transient holes and antiholes were burned using population storage in nuclear hyperfine levels. These two mechanisms of hole burning are reported here for transition-metal ions for what is believed to be the first time.
Photon-gated hole burning, or selective bleaching enabled by a second light source, has been observed in Co2+{\mathrm{Co}}^{2+}Co2+ in tetrahedral sites of LiGa5{\mathrm{LiGa}}_{5}LiGa5​O8{\mathrm{O}}_{8}O8​. This leads to long-lived spectral holes with a width of \ensuremath{\sim}1 GHz at 1.6 K. It is proposed that two-step photoionization of Co2+{\mathrm{Co}}^{2+}Co2+ is responsible for the hole burning. Much narrower (\ensuremath{\sim}40 MHz) transient holes and antiholes were burned using population storage in nuclear hyperfine levels. These two mechanisms of hole burning are reported here for transition-metal ions for what is believed to be the first time.
It is demonstrated that persistent hole burning in the zero-phonon line of Eu2+ in SLs of CaF2:Eu/CdF2 with uniformly doped CaF2 layers is mainly due to tunneling of electrons from the 4f65d excited state of Eu2 to the conduction band of adjacent CdF2 layer. However in selectively doped suoerlattices (SLs), the two-step photoionization process dominates in the formation of spectral holes. Two mechanisms of spectral hole broadening were discussed. These are the Stark-shifting of the Eu2 f-d transition energy induced by internal electric field and phonon assisted transitions.