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Optics Letters

Measurement of nuclear and electronic Zeeman effects using optical hole-burning spectroscopy

R. M. Macfarlane, Robert M. Shelby

Published Feb 1, 1981• 42 citations
Publisher

Abstract

The excited-state nuclear Zeeman effect and quadratic-electronic Zeeman effect were studied in Pr(3+):LaF(3) using laser-induced hole burning. Hole burning in an external magnetic field gave values for the excited-state enhanced nuclear g tensor of g(x)beta/h = 2.2, g(y)beta/h = 1.9, and g(z)beta/h = 3.6 kHz/G. By applying the field after hole burning, quadratic-electronic Zeeman coefficients as small as 0.1 Hz/G(2) were measured. The hyperfine coupling constant in the excited (1)D(2) level was found to be A(J) = 600 MHz.

DOI
10.1364/ol.6.000096

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The hyperfine splitting of the ground state and the lowest electronic component of the (1)D(2) excited state have been measured for Pr(3+) in YAG. We show that a particularly simple and powerful technique is the production of sublevel coherence by short-pulse (impact) excitation, which is detected by coherent forward scattering of a weak probe beam and Fourier transformation of the resulting quantum-beat signal. This yielded excited-state splittings of 6.49 and 8.29 MHz. The ground state shows large pseudoquadrupole splittings of 33.4 and 41.6 MHz, which were obtained by optically detected nuclear quadrupole resonance.

Optics Letters•Jun 1, 1983•48 citations
The excited-state nuclear Zeeman effect and quadratic-electronic Zeeman effect were studied in Pr(3+):LaF(3) using laser-induced hole burning. Hole burning in an external magnetic field gave values for the excited-state enhanced nuclear g tensor of g(x)beta/h = 2.2, g(y)beta/h = 1.9, and g(z)beta/h = 3.6 kHz/G. By applying the field after hole burning, quadratic-electronic Zeeman coefficients as small as 0.1 Hz/G(2) were measured. The hyperfine coupling constant in the excited (1)D(2) level was found to be A(J) = 600 MHz.
Persistent spectral hole burning has been observed in CaF(2):Sm(2+) and originates from photoionization of the Sm(2+) ion. This represents a new class of persistent hole-burning materials. We have used hole burning to measure the nonlinear Zeeman effect of the (7)F(0)A(1g) ? A(1u) transition at 695.8 nm with a resolution of ~100 MHz. We find a nonlinear coefficient of 0.93 Hz/G(2), which is close to the value of 1.0 Hz/G(2) calculated for the (7)F(0)-(7)F(1) interaction. This shows that the dominant contribution to the nonlinear Zeeman effect comes from the ground state.
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.
The recently demonstrated process of photon-gated spectral hole burning has been used to measure the small frequency shifts necessary for the determination of linear Stark and nonlinear Zeeman coefficients of the 4f6{f}^{6}f6 7{}^{7}7F0{F}_{0}F0​A1{A}_{1}A1​\ensuremath{\rightarrow}5{}^{5}5D0{D}_{0}D0​A1{A}_{1}A1​, 5D1^{5}\mathrm{D}_{1}5D1​A2{\mathrm{A}}_{2}A2​, and 5D1^{5}\mathrm{D}_{1}5D1​E transitions of Sm2+{\mathrm{Sm}}^{2+}Sm2+ in BaClF. The nonlinear Zeeman coefficients obtained in this way agree, to better than 12%, with those calculated assuming free-ion 4f6{f}^{6}f6 wave functions for Sm2+{\mathrm{Sm}}^{2+}Sm2+. The Stark splitting coefficients (0.068--0.074 MHz/V ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) are smaller than the few previously reported for fn{f}^{n}fn\ensuremath{\rightarrow}fn{f}^{n}fn transitions of rare-earth ions.
The theory of how excited-state hyperfine structure can be determined using a magnetic field to decouple the nuclear and electronic angular momentum is presented. The initial excited state is assumed to have an anisotropic Zeeman sublevel population distribution, which can be conveniently created by a laser-induced multiphoton excitation of an unpolarized atom. The Zeeman sublevel populations are subsequently mixed by the hyperfine interaction. The degree of mixing is controlled by a magnetic field applied along the quantization axis. The relative Zeeman sublevel populations can be monitored by detecting the polarization of fluorescence emitted when the excited state radiatively decays. It is convenient to take the ratio of two time-integrated fluorescent signals measured for orthogonal linear polarizations, since this is independent of the excited-state number density. The plot of this ratio versus magnetic field is very well approximated by a Lorentzian curve whose half-width is proportional to the magnetic dipole hyperfine coupling constant. This method was used to determine the magnitude of the magnetic dipole constant of the cesium 8D3/2{\mathit{D}}_{3/2}D3/2​ state to be 3.92\ifmmode\pm\else\textpm\fi{}0.10 MHz, which is in excellent agreement with previous results.
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.
The hyperfine splitting of the ground state and the lowest electronic component of the (1)D(2) excited state have been measured for Pr(3+) in YAG. We show that a particularly simple and powerful technique is the production of sublevel coherence by short-pulse (impact) excitation, which is detected by coherent forward scattering of a weak probe beam and Fourier transformation of the resulting quantum-beat signal. This yielded excited-state splittings of 6.49 and 8.29 MHz. The ground state shows large pseudoquadrupole splittings of 33.4 and 41.6 MHz, which were obtained by optically detected nuclear quadrupole resonance.