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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Time-Resolved Holeburning in YLiF4:Er3+ with Zeeman Scanning

Y. P. Wang, Richard S. Meltzer, Reinhold Wannemacher, R. M. Macfarlane

Published Jan 1, 1991• 0 citations
Publisher

Abstract

We report the results of time–resolved optical holeburning of Er3+ ions in YLiF4 (0.02%). In earlier work for H//c we described the time evolution of holes burned at 33kG using laser scanning over a frequency of 40MHz1 and we reported, using larger scans, the occurence of optical side holes. We now describe results for H⊥c with scans > 400 MHz using a new Zeeman technique for frequency scanning the optical transition frequencies which allow one to study the time evolution of the holes and their associated sideholes. The hole lineshapes evolve with time reaching a linewidth of ≃ 10 MHz after 600 μs. We identify the source of the time evolution of the hole shape as spectral diffusion resulting from mutual spin flips of the surrounding fluorine nuclei whose flip rates are strongly modified from the bulk rates by the presence of the large magnetic moment of the Er3+ ion which produces a "frozen core". A computer simulation which takes into account the details of the dynamics of the frozen core successfully describes the time evolution of the holes, confirming the dominant role of F nuclear spin flips.

DOI
10.1364/pshb.1991.tha4

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We report the results of time–resolved optical holeburning of Er3+ ions in YLiF4 (0.02%). In earlier work for H//c we described the time evolution of holes burned at 33kG using laser scanning over a frequency of 40MHz1 and we reported, using larger scans, the occurence of optical side holes. We now describe results for H⊥c with scans > 400 MHz using a new Zeeman technique for frequency scanning the optical transition frequencies which allow one to study the time evolution of the holes and their associated sideholes. The hole lineshapes evolve with time reaching a linewidth of ≃ 10 MHz after 600 μs. We identify the source of the time evolution of the hole shape as spectral diffusion resulting from mutual spin flips of the surrounding fluorine nuclei whose flip rates are strongly modified from the bulk rates by the presence of the large magnetic moment of the Er3+ ion which produces a "frozen core". A computer simulation which takes into account the details of the dynamics of the frozen core successfully describes the time evolution of the holes, confirming the dominant role of F nuclear spin flips.
We have measured spectral diffusion in Er3+-doped YLiF4 from the time dependence of spectral hole shapes. The holes were burned in the absorption corresponding to the transition between the lowest Zeeman components of the 4I15/2(1) and 4F9/2(1) levels of Er3+:YLiF4 at 15298.6 cm−1 and were scanned by rapid Zeeman tuning of the erbium energy levels. In an external magnetic field of 26 kG, which supresses erbium–erbium spin flips, the mechanism for spectral diffusion involved local field fluctuations that are due to 19F nuclear spin flips in the perturbing field of the erbium electron spins. Numerical simulation of the fluorine spin dynamics gives semiquantitative agreement with the observed time-dependent hole shapes.
Laser induced hole burning in optical absorption bands of low temperature solids has been investigated with emphasis on mechanisms for population hole burning, the interactions with the environment which limit the hole widths and the use of hole burning for ultra high resolution spectroscopy. Hole burning was observed in a wide range of solids including organic and organometallic molecules in crystals and rare earth ions in crystals and glasses. The mechanisms for hole burning also varied widely and a new mechanism involving optically induced nuclear spin flips of near neighbor nuclei was discovered. Examples of hole burning in new classes of materials are presented here for the first time, namely inorganic glasses (silicate glasses containing Nd(3+), Pr(3+) or Eu(3+)) and undoped stoichiometric compounds (e.g., EuP5O14). Hole recovery was used to determine nuclear spin lattice relaxation rates in praseodymium doped crystals. For allowed optical transitions (e.g., singlet states of zinc porphyrin, dibromoindigo and color centers in alkali halides) the hole widths at 2K are limited by population decay to approximately 50 MHz. For longer lived optical levels in crystalline materials, e.g., those containing rare earth ions, the hole widths are narrower (less than 10 MHz) and are limited by dynamical interactions with surrounding nuclei. In amorphous materials such as europium doped silicate glass, hole widths are much broader, being limited by low frequency tunneling motions. Hole burning measurements were complemented by time domain coherent transient (photon echo, and optical free decay) measurements of homogeneous linewidths which enabled us to measure optical resonances as narrow as 760 Hz in Eu(3+):Y2O3.
A new technique for performing optical-free-induction-decay experiments is described whereby the ion transition frequencies are rapidly shifted with a pulsed magnetic field. The technique is demonstrated in YLiF4{\mathrm{YLiF}}_{4}YLiF4​:Er3+{\mathrm{Er}}^{3+}Er3+ and is used to measure the temperature dependence of the homogeneous linewidths, ${\ensuremath{\Gamma}}_{h}$, of the four transitions connecting the Zeeman sublevels of the ground and lowest 4F9/2^{4}\mathrm{F}_{9/2}4F9/2​ excited state. Below 4 K, ${\ensuremath{\Gamma}}_{h}$ is dominated by Er3+{\mathrm{Er}}^{3+}Er3+-Er3+{\mathrm{Er}}^{3+}Er3+ interactions, and evidence for the presence of both direct and indirect contributions is presented.
4fn ⇒ 4fn transitions of trivalent rare earth ions doped in crystals frequently give sharp spectral lines. The transitions associated with the higher levels of a multiplet can be relatively sharp, 10-1000 GHz, where the width is determined by the decay rate of the levels by spontaneous phonon emission to lower levels. The transitions and their linewidth can be determined using conventional absorption or excitation techniques. On the other hand the transitions associated with the meta-stable lower levels typically give much sharper features with linewidths of 1 - 100 GHz and the widths are determined by the inhomogeneities of the crystal field. These inhomogeneous linewdths can be obtained by conventional spectroscopic techniques but the homogeneous linewidth requires more innovative techniques such as optical holeburning or photon echoes. The time domain photon echo measurements do not requiring a high resolution source and have frequently been used to establish that the homogeneous linewidth of such transitions. The lines can be very narrow down to the kHz regime [1,2]. Should complimentary measurements be attempted in the frequency domain utilising holeburning a special frequency stabilised lasers is required and one has been developed in association with the current work [3].
Recent experiments on time-resolved hole-burning (TRHB) [1-3] and nonexponential photon-echo decays [4,5] in low-temperature ion-doped crystals have demonstrated the multi-timescale dynamics of host nuclei whose spin flips provide the main source of stochastic fluctuations Ut of an impurity ion transition frequency ωab(ωabt=ωab+Ut) leading to optical dephasing and spectral diffusion. Such complicated spin dynamics results from the existence around the impurity ion of the "frozen core" of nuclear spins with their flip rates to be greatly slowed compared to the unperturbed bulk spins.
We demonstrate a new mechanism for optical spectral hole burning in which population is stored in electronic Zeeman sublevels. This is shown by optical pumping the ground-state Kramers doublet of the 4I9/2^{4}\mathrm{I}_{9/2}4I9/2​${\mathrm{\ensuremath{\leftrightarrows}}}^{2}$H11/2{\mathrm{H}}_{11/2}H11/2​ (6248.9 A\r{}) and 4I9/2^{4}\mathrm{I}_{9/2}4I9/2​${\mathrm{\ensuremath{\leftrightarrows}}}^{4}$G5/2{\mathrm{G}}_{5/2}G5/2​ (5777.1 A\r{}) transitions of LaF3{\mathrm{LaF}}_{3}LaF3​:Nd3+{\mathrm{Nd}}^{3+}Nd3+ with a narrow-band cw dye laser. Experiments were carried out at 1.6 K in external fields of \ensuremath{\sim}100 G. The Zeeman shift of the resulting antiholes and holes makes an assignment of these structures possible. Hole recovery times of hundreds of milliseconds are shorter than expected at these low temperatures and fields and provide evidence for optical spectral diffusion caused by mutual spin flips in the ground state.