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Physical review. B, Condensed matter

Electronic Zeeman and Stark spectroscopy of BaClF: Sm2+ using photon-gated hole burning

R. M. Macfarlane, Robert M. Shelby, Albrecht Winnacker

Published Mar 15, 1986• 26 citations
Publisher

Abstract

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 4${f}^{6}$ ${}^{7}$${F}_{0}$${A}_{1}$\ensuremath{\rightarrow}${}^{5}$${D}_{0}$${A}_{1}$, $^{5}\mathrm{D}_{1}$${\mathrm{A}}_{2}$, and $^{5}\mathrm{D}_{1}$E transitions of ${\mathrm{Sm}}^{2+}$ in BaClF. The nonlinear Zeeman coefficients obtained in this way agree, to better than 12%, with those calculated assuming free-ion 4${f}^{6}$ wave functions for ${\mathrm{Sm}}^{2+}$. The Stark splitting coefficients (0.068--0.074 MHz/V ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) are smaller than the few previously reported for ${f}^{n}$\ensuremath{\rightarrow}${f}^{n}$ transitions of rare-earth ions.

DOI
10.1103/physrevb.33.4207

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A new mechanism of spectral holeburning by 2-step photoionization ("photon-gated" holeburning) has recently been demonstrated. In BaClF : Sm2+, this leads to permanent spectral holes 25 MHz wide which we have used to measure small linear Stark and nonlinear Zeeman coefficients of the 7F0↔5D0 transition of Sm2+. The Zeeman coefficients agree within 4% with those calculated assuming free ion 4f6 wave functions for 7F0 and 5D0.

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Persistent spectral hole burning (PSHB) was discovered in organic molecular system in 1974[1]. Five years later, PSHB in inorganic materials was discovered in NaF by R. M. Macfarlane et al [2]. In 1985, A. Winnacker et al [3] first observed photon gated spectral hole burning in BaFCl: Sm2+ at 2K. Hole burning(HB) is useful in high resolution spectroscopy. It is also of crucial importance for the application to frequency domain optical storage. The storage density is proportional to the ratio of inhomogeneous linewidth(Γi) to the homogeneous linewidth(Γh), N(= Γi/Γh). The inhomogeneous linewidth of 5D0-TF0 transition of Sm2+ is 16GHz and the hole width is 25MHz in BaFCl at 2K[3]. For this material, the inhomogeneous linewidth changes only moderately with the temperature; On the other hand, the homogeneous linewidth increases rapidly as the temperature rises. Then, a small value of N(~2) can be estimated when HB temperature is raised to 77K. That means, it is difficult to burn a hloe in the inhomogeneous line in BaFCl:Sm2+ at 77K. To maintain a reasonable storage capacity or to study HB at a quite high temperature, a large inhomogeneous linewidth is in great request.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1991•0 citations
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}$${F}_{0}$${A}_{1}\ensuremath{\rightarrow}{}^{5}$${D}_{0}$${A}_{1}, ^{5}\mathrm{D}_{1}$${\mathrm{A}}_{2}, 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 cm\ensuremath−1{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}cm\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.
Spectral hole burning in solids is a selective bleaching of a small portion of an inhomogeneously broadened optical transition by a laser. In the photon gated holeburning process spectral holes are burned in two steps. The first is provided by a narrow band laser resonant with the inhomogeneously broadened transition and the second (gating) can be initiated by a broad band light source. Photon gated spectral hole burning was reported recently in 7F0→5D0 and 7F0→5D1 absorption lines of Sm2+ in BaClF(1). In this poster we report on the spectral holeburning behaviour of 1F0→5D2 transition. We found that even in absence of additional light source for gating, permanent holes can be burned. This self gating behaviour is consistent with the observation that the optimum frequency following 5D0 excitation is ≈ 22 000cm-1 so that two photons of energy 5D2 - 7F0 are sufficient to produce photoionisation. We have analysed the light intensity dependance of hole area and a simple model indicate that the electron transfer following the photoionisation is strongly dependant on the ion - electron trap distance.
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.
One-color two-photon excitation spectra of the 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D0{\mathit{D}}_{0}D0​ and 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​ transitions of Sm2+{\mathrm{Sm}}^{2+}Sm2+ in SrF2{\mathrm{SrF}}_{2}SrF2​ have been measured at low temperature and their dependences upon photon polarization analyzed. Linewidths on the order of 0.2, 0.6, and 1.0 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ are obtained for the 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D0{\mathit{D}}_{0}D0​(A1g{\mathit{A}}_{1\mathit{g}}A1g​), 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​(Eg{\mathit{E}}_{\mathit{g}}Eg​), and 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​(T2g{\mathit{T}}_{2\mathit{g}}T2g​) Stark components observed at 15 K, respectively. The 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D0{\mathit{D}}_{0}D0​(A1g{\mathit{A}}_{1\mathit{g}}A1g​) transition is observed to be isotropic within experimental error, while the Eg{\mathit{E}}_{\mathit{g}}Eg​ and T2g{\mathit{T}}_{2\mathit{g}}T2g​ components of the 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​ transition exhibit the anisotropic patterns expected in Oh{\mathrm{O}}_{\mathit{h}}Oh​ symmetry. Calculations of two-photon transition intensities are conducted within the framework of the phenomenological model previously used for Sm2+{\mathrm{Sm}}^{2+}Sm2+ in MClF (M=Ba,Sr) and Eu3+{\mathrm{Eu}}^{3+}Eu3+ in LuPO4{\mathrm{LuPO}}_{4}LuPO4​, where the rare-earth ion occupies sites of C4v{\mathit{C}}_{4\mathit{v}}C4v​ and D2d{\mathit{D}}_{2\mathit{d}}D2d​ symmetries, respectively. The present results are compared and contrasted with those obtained in these previous cases.
The two-photon transitions between the Stark levels of the 7F0^{7}\mathrm{F}_{0}7F0​ and 5D2^{5}\mathrm{D}_{2}5D2​ multiplets of the Sm2+{\mathrm{Sm}}^{2+}Sm2+ ion in BaClF are investigated both from an experimental and theoretical viewpoint. Direct two-photon excitation spectra of the 5D2^{5}\mathrm{D}_{2}5D2​ fluorescence resulting from an optical excitation with an infrared laser beam are presented and the polarization dependence of the observed transitions is analyzed. These new data are interpreted along the lines of a simple model which originates in the second-order theory developed by Axe [Phys. Rev. 136, A42 (1964)] for two-photon processes in complex atoms. The extension of this theory to the case of rare-earth ions embedded in crystalline fields is carried out by use of symmetry-adaptation techniques based on the use of an SU(2)\ensuremath{\supset}G∗{\mathrm{G}}^{\mathrm{*}}G∗ chain of groups. It is shown that the resulting model (limited up to second-order terms) describes correctly the relative intensities of the two-photon transitions between the Stark levels of the 7F0^{7}\mathrm{F}_{0}7F0​ and 5D2^{5}\mathrm{D}_{2}5D2​ multiplets of Sm2+{\mathrm{Sm}}^{2+}Sm2+ in BaClF.
Persistent spectral hole burning (PSHB) was discovered in organic molecular system in 1974[1]. Five years later, PSHB in inorganic materials was discovered in NaF by R. M. Macfarlane et al [2]. In 1985, A. Winnacker et al [3] first observed photon gated spectral hole burning in BaFCl: Sm2+ at 2K. Hole burning(HB) is useful in high resolution spectroscopy. It is also of crucial importance for the application to frequency domain optical storage. The storage density is proportional to the ratio of inhomogeneous linewidth(Γi) to the homogeneous linewidth(Γh), N(= Γi/Γh). The inhomogeneous linewidth of 5D0-TF0 transition of Sm2+ is 16GHz and the hole width is 25MHz in BaFCl at 2K[3]. For this material, the inhomogeneous linewidth changes only moderately with the temperature; On the other hand, the homogeneous linewidth increases rapidly as the temperature rises. Then, a small value of N(~2) can be estimated when HB temperature is raised to 77K. That means, it is difficult to burn a hloe in the inhomogeneous line in BaFCl:Sm2+ at 77K. To maintain a reasonable storage capacity or to study HB at a quite high temperature, a large inhomogeneous linewidth is in great request.