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Radiation effects and defects in solids

Persistent spectral hole-burning in electronic tranisitions of different types of lattice defects

T. Attenberger, Ilmo Sildos, Glynn D. Jones, Udo Bogner, Max Maier

Published Nov 1, 1991• 4 citations
Publisher

Abstract

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.

DOI
10.1080/10420159108224895

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Physical review. B, Condensed matter•Nov 15, 1997•21 citations
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.
In different color centers of neutron- irradiated and annealed sapphire crystals persistent spectral holes could be burned which were thermoresistant up to 670K [1]. In the 755.6nm zero-phonon line (ZPL) two-color photon-gated persistent spectral hole-burning (PSHB) was obtained with pulsed dye-lasers [2]. Preliminary results of PSHB with a cw laser were reported for the 462.5nm ZPL [3]. The present study concerns a investigation of PSHB with cw-lasers in different ZPL, including the 755.6nm ZPL, which is interesting for potential applications in particular because diode lasers are available in this spectral range.
The persistent spectral hole burning effect has been observed for the nitrogen vacancy (NV) center and the 2.16 eV center in chemical-vapor deposited (CVD) diamond. This sideband is the first observation of spectral hole burning in CVD diamond. Holes are burned in the inhomogeneously broadened zero-phonon lines of both the centers by dye lasers. The holes were observed by photoluminescence excitation spectroscopy, with monitoring of the phonon-sideband emission, at temperatures up to 130 K for the NV center and up to 100 K for the 2.16 eV center.
Persistent spectral hole burning in the $f\ensuremath{\rightarrow}f$ transition and changes in the $f\ensuremath{\rightarrow}d$ transition spectra upon laser irradiation were investigated in Sm2+{\mathrm{Sm}}^{2+}Sm2+-doped ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}$ glasses prepared by a sol-gel process. The hole was burned in the ${}^{7}{F}_{0}{\ensuremath{\rightarrow}}^{5}{D}_{0}$ line of Sm2+{\mathrm{Sm}}^{2+}Sm2+ ions using a DCM dye laser at 77 K and the dependence of the burning efficiency on laser power and burning time was measured. The hole depth increased with increasing laser irradiation time, reaching up to $\ensuremath{\sim}12%$ of the total intensity within a few hundred seconds. Neither an antihole around the burned hole nor a change in the fluorescence line narrowing spectrum were observed after hole burning. The hole depth linearly increased with increasing the incident laser power up to $\ensuremath{\sim}1{\mathrm{W}/\mathrm{m}\mathrm{m}}^{2},$ indicating a single-photon hole-burning process. On the other hand, laser irradiation with a wavelength corresponding to the energy of the ${4f}^{6}\ensuremath{\rightarrow}{4f}^{5}5d$ transition resulted in a decrease of both the absorption and fluorescence intensities but no formation of a hole. It was concluded that the electrons excited in the 4f55d{4f}^{5}5d4f55d level were further excited into the conduction band of the host matrix by a two-photon absorption process and then captured in the trapping center.
In the first experimental search for persistent spectral hole burning in an elemental semiconductor, we examined a variety of electronic defects in Si and in a Si:Ge alloy. No persistent spectral changes have been observed for Be-Li, Se0, or thermal donors in Si; however, spectral holes which persist for ~5 ms have been produced in the 1s-2p absorption lines of a sulfur-hydrogen complex in Si. The addition of 0.7% Ge to the Si host ensures that an inhomogeneously broadened system is being studied. Measurements combining a CO2 laser pump with a Fourier transform spectrometer probe reveal that the hole burning is due to migration of electrons from the S-H centers to shallow traps. The large observed hole width (4.6 cm−1) is attributed to spectral diffusion by resonant excitation transfer. The hole burning behavior of the 2p± line is temperature independent below 30 K, whereas the hole burning of the 2p0 line exhibits strong temperature dependence, suggesting that the ionization of the laser-excited centers in the 2p± hole burning process occurs via energy transfer between neighboring excited centers rather than by thermal ionization.
We have observed persistent spectral hole burning in a family of centers in CaF2:Pr3+:D− and SrF2:Pr3+:D− crystals in which the Pr3+ ion has multiple D−-ion near neighbors. The hole burning is caused by light-induced D- motion that leads to persistent changes in the local crystal field of the Pr3+ ion. Depending on the center and the temperature, side-hole or antihole structure is observed that has its origin in the second-order hyper-fine interaction. The variation in the hyperfine splittings between centers is consistent with the separation between the ground state and the first excited state.
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.