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Physical review. B, Condensed matter

Optical measurement of the isotope shifts and hyperfine and superhyperfine interactions of Nd in the solid state

R. M. Macfarlane, Richard S. Meltzer, Malkin Boris Zalmanovich

Published Sep 1, 1998• 64 citations
Publisher

Abstract

We report the observation of optically resolved isotope, hyperfine, and superhyperfine structure in the spectrum of ${\mathrm{Nd}}^{3+}$ ions in ${\mathrm{YLiF}}_{4},$ isotopically pure in ${}^{7}\mathrm{Li}.$ This observation was made on the ${(4f}^{3}\ensuremath{-}{4f}^{3}),$ ${}^{4}{I}_{9/2}{(1)}^{4}{F}_{3/2}(1)$ transition of ${\mathrm{Nd}}^{3+}$ ions present as impurities at ppm levels. The optical linewidths of the transitions of the even mass number isotopes, ${}^{142}\mathrm{Nd},$ ${}^{144}\mathrm{Nd},$ ${}^{146}\mathrm{Nd},$ ${}^{148}\mathrm{Nd},$ and ${}^{150}\mathrm{Nd},$ are only 45 MHz which makes it very easy to resolve the isotope shift of 115 MHz/unit mass. The hyperfine structure of the two odd mass number isotopes, ${}^{143}\mathrm{Nd}$ and ${}^{145}\mathrm{Nd},$ are resolved and the hyperfine parameters are determined in both the ground and electronically excited states. Some of the transitions have linewidths as narrow as 10 MHz. These are the narrowest optical inhomogeneous linewidths observed in solids. In addition, each even isotope line is split by 30 MHz. The observed splitting is assigned to a superhyperfine coupling between ${\mathrm{Nd}}^{3+}$ and its nearest-neighbor fluorine nuclei. Here, a superhyperfine splitting has been resolved in an optical spectrum. The optical line shapes for the even isotopes are calculated as the sum of all transitions between the superhyperfine components $({\mathrm{Nd}}^{3+}$ with its eight nearest-neighbor F nuclei) of the ground and excited electronic states, considering both magnetic dipole-dipole (including spin-transfer contributions) and contact interactions. The results are in quantitative agreement with experiment.

DOI
10.1103/physrevb.58.5692

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We report the first observation of electromagnetically induced transparency (EIT) in an isotopically purified Nd3+:YLiF4{\mathrm{Nd}}^{3+}:{\mathrm{YLiF}}_{4}Nd3+:YLiF4​ crystal. This crystal demonstrates inhomogeneous broadening of optical transitions of about 35 MHz. EIT is observed in a symmetrical $\mathrm{\ensuremath{\Lambda}}$-like system formed by two hyperfine sublevels of the ground state corresponding to a zero first-order Zeeman (ZEFOZ) transition and a hyperfine sublevel of the excited state, which is not coupled to other ground-state sublevels. It is found that transmission of the probe field as a function of the two-photon detuning demonstrates a comblike structure that can be attributed to superhyperfine coupling between Nd3+{\mathrm{Nd}}^{3+}Nd3+ ions and fluorine nuclei. The observed structure can be resolved only in the vicinity of the ZEFOZ point where the homogeneous linewidth of the spin transition is sufficiently small. The results pave the way for implementing solid-state quantum memories based on off-resonant Raman interaction without spectral tailoring of optical transitions.
Using a low-strain, isotopically pure crystal of YLiF4{\mathrm{YLiF}}_{4}YLiF4​, we have measured extremely narrow inhomogeneous linewidths (as low as 40 MHz) for the optical transitions of Er3+{\mathrm{Er}}^{3+}Er3+ impurities. Inhomogeneous broadening due to strains and other defects is so low that a new mechanism limits the inhomogeneous linewidth: local magnetic fields due to fluorine nuclear spins. These ultranarrow lines enabled us to make the first direct measurement of the isotope shifts of f-f transitions in a solid, and we find for the isotopes 164Er^{164}\mathrm{Er}164Er, 166Er^{166}\mathrm{Er}166Er, 168Er^{168}\mathrm{Er}168Er, and 170Er^{170}\mathrm{Er}170Er a shift of 76\ifmmode\pm\else\textpm\fi{}2 MHz unit mass on the 4^{4}4I15/2{\mathit{I}}_{15/2}I15/2​(1)4{)}^{4})4F9/2{\mathit{F}}_{9/2}F9/2​(1) transition. We show that this is consistent with a mechanism of coupling to zero-point vibrations.
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