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Physical review. B, Condensed matter

Laser spectroscopy of thulium atoms implanted in liquid and solid 4 He

Kiyoshi Ishikawa, A. Hatakeyama, Koichi Gosyono-o, Shigeaki Wada, Yoshiro Takahashi, T. Yabuzaki

Published Jul 1, 1997• 36 citations
Publisher

Abstract

The excitation, emission spectra, and decay curves of the emission intensity of thulium atoms implanted in liquid and solid helium were observed in the presence and absence of an external magnetic field. The observed narrow line (width $\ensuremath{\sim}0.1$ nm) of the excitation spectrum at 590.60 nm is assigned as a zero-phonon transition from the electronic ground state ${4f}^{13}{(}^{2}{F}_{7/2}^{o}{)6s}^{2}$, which indicates that the transition between the inner shells is weakly perturbed by surrounding helium atoms. The pressure dependence of the emission wavelength suggests that the symmetry of helium atoms distributed around a thulium atom in the solid phase is similar to that in the liquid phase. The emission intensity was stable and large in the solid phase since thulium atoms were trapped at a density of 10${}^{10}$--10${}^{11}$ atoms/cm${}^{3}$. The lifetime of the excited state was measured to be $7.09\ifmmode\pm\else\textpm\fi{}0.04$ $\ensuremath{\mu}$s, which was longer than that of the ${4f}^{12}{(}^{3}{H}_{6}{)5d}_{5/2}{6s}^{2}$ ${(6,5/2)}_{7/2}$ state of free thulium atoms. The excited state is expected to be a mixed state of the ${4f}^{12}{5d6s}^{2}$ and ${4f}^{13}6s6p$ configurations. The metastable state ${4f}^{13}{(}^{2}{F}_{5/2}^{o}{)6s}^{2}$ is populated by a radiative transition from this excited state and relaxes to the ground state through a magnetic dipole transition. The lifetime of the metastable state of a neutral thulium atom was measured to be $75\ifmmode\pm\else\textpm\fi{}3$ ms.

DOI
10.1103/physrevb.56.780

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The excitation, emission spectra, and decay curves of the emission intensity of thulium atoms implanted in liquid and solid helium were observed in the presence and absence of an external magnetic field. The observed narrow line (width \ensuremath∼0.1\ensuremath{\sim}0.1\ensuremath∼0.1 nm) of the excitation spectrum at 590.60 nm is assigned as a zero-phonon transition from the electronic ground state 4f13(2F7/2o)6s2{4f}^{13}{(}^{2}{F}_{7/2}^{o}{)6s}^{2}4f13(2F7/2o​)6s2, which indicates that the transition between the inner shells is weakly perturbed by surrounding helium atoms. The pressure dependence of the emission wavelength suggests that the symmetry of helium atoms distributed around a thulium atom in the solid phase is similar to that in the liquid phase. The emission intensity was stable and large in the solid phase since thulium atoms were trapped at a density of 1010{}^{10}10--1011{}^{11}11 atoms/cm3{}^{3}3. The lifetime of the excited state was measured to be 7.09\ifmmode±\else\textpm\fi0.047.09\ifmmode\pm\else\textpm\fi{}0.047.09\ifmmode±\else\textpm\fi0.04 \ensuremathμ\ensuremath{\mu}\ensuremathμs, which was longer than that of the 4f12(3H6)5d5/26s2{4f}^{12}{(}^{3}{H}_{6}{)5d}_{5/2}{6s}^{2}4f12(3H6​)5d5/2​6s2 (6,5/2)7/2{(6,5/2)}_{7/2}(6,5/2)7/2​ state of free thulium atoms. The excited state is expected to be a mixed state of the 4f125d6s2{4f}^{12}{5d6s}^{2}4f125d6s2 and 4f136s6p{4f}^{13}6s6p4f136s6p configurations. The metastable state 4f13(2F5/2o)6s2{4f}^{13}{(}^{2}{F}_{5/2}^{o}{)6s}^{2}4f13(2F5/2o​)6s2 is populated by a radiative transition from this excited state and relaxes to the ground state through a magnetic dipole transition. The lifetime of the metastable state of a neutral thulium atom was measured to be 75\ifmmode±\else\textpm\fi375\ifmmode\pm\else\textpm\fi{}375\ifmmode±\else\textpm\fi3 ms.
We investigate the 1140 nm magnetic-dipole transition of thulium atoms trapped in solid argon and neon. These solids can be straightforwardly grown on any substrate at cryogenic temperatures, making them prime targets for surface-sensing applications. Our data are well described by a splitting of the single vacuum transition into three components in both argon and neon, with each component narrower than the 0.8 nm spectrometer resolution. The lifetime of the excited states is 14.6(0.5) ms in argon and 27(3) ms in neon, shorter than in vacuum or in solid helium. We also collected visible laser-induced fluorescence spectroscopy showing broader emission features in the range of 580--600 nm. The narrow infrared features in particular suggest a range of possible applications.
Optically active defects suspended in an inert solid are an interesting system for sensing and magnetometry at the nanometer scale, in addition to being a potential source of high-density, identical quantum emitters for quantum information. Beyond their response to external fields, the optical absorption and emission spectra also reflect information about the host matrix, which is critical to understand for either application. For the particular system of thulium atoms implanted in solid argon, high resolution laser spectroscopy reveals narrow ensemble linewidths of the 1140 nm f to f ground state spin-orbit transition, which is split due to crystal field effects and hyperfine coupling. Pump-probe spectroscopy is used to identify crystal field levels in at least two stable trapping sites, and the crystal field is determined to be nearly axial in both sites. Strong selection rules indicate that this transition becomes magnetic-electric in the argon host, most likely due to dielectric effects. In the presence of mT magnetic fields, Zeeman shifts are resolvable by laser fluorescence, allowing crystal axis selective polarized spectroscopy. These results show that all-optical detection schemes for DC magnetic fields are already possible with thulium-doped argon, and point towards more informed strategies for monitoring and improving crystal growth and annealing.
We present an exhaustive overview of optical absorption and laser-induced fluorescence lines of Ba atoms in liquid and solid helium matrices in visible and near-infrared spectral ranges. Due to the increased density of isolated atoms, we have found a large number of spectral lines that were not observed in condensed helium matrices before. We have also measured the lifetimes of metastable states. The lowest 3D1{}^{3}{D}_{1}3D1​ metastable state has lifetime of 2.6 s and can be used as an intermediate state in two-step excitations of high-lying states. Various matrix-induced radiationless population transfer channels have been identified.
Optically active defects in solid-state systems have many applications in quantum information and sensing. However, unlike free atoms, which have fixed optical transition frequencies, the inhomogeneous broadening of the transitions in solid-state environments limit their use as identical scatterers for such applications. Here we show that crystals of argon and neon prepared in a closed-cycle cryostat doped with thulium atoms at cryogenic temperatures are an exception. High resolution absorption and emission spectroscopy show that the 1140 nm magnetic dipole transition is split into multiple components. The origin of this splitting is likely a combination of different classes of trapping sites, crystal field effects within each site, and hyperfine interactions. The individual lines have ensemble widths as small as 0.6GHz0.6\phantom{\rule{4.pt}{0ex}}\text{GHz}0.6GHz, which temperature dependence and pump-probe spectroscopy indicate is likely a homogeneous effect, suggesting inhomogeneity is well below the GHz scale.
Lineshapes associated with the absorption and emission spectra of neutral atoms in liquid helium and cold helium gas are discussed. A neutral atom in liquid helium forms a microcavity due to a strong short-range repulsive force between the helium and impurity atoms, producing very broad and largely blueshifted absorption bands and relatively narrow emission lines with much smaller shifts. A broad and weak emission band observed by exciting the D2 line of Ag atoms in liquid helium has confirmed the hypothesis that quenching of D2 emission lines for heavy group 1a and 1b atoms are due to the formation of exciplex. In cold helium gas, sudden decrease of the emission lifetimes below 5.2 K by the excitation of the D2 line of Ag atoms is attributed to the condensation of He atoms on the metastable 2D5/2 state. Very narrow absorption lines of Eu innershell electron transitions have revealed that superfluid helium behaves as a static and highly homogeneous low temperature matrix.
Secondary laser cooling has been realised on the weak dipole transition 4f13(2Fo)6s2, J = 7/2, F=4 → 4f12(3H6) 5d5/26s2, J' = 9/2, F' = 5 with the wavelength of 530.7 nm and natural width of 350 kHz. The temperature of the atomic cloud in a magnetooptical trap (MOT) was 30 μK at the lifetime of 2 s and the number of atoms 105. Approximately 1% of atoms from the MOT have been reloaded to an optical dipole trap and to one-dimensional optical lattice at the wavelength of 532 nm. The atom lifetime in the optical lattice was 320 ms. We propose to employ thulium atoms captured in an optical lattice as an optical frequency reference.