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Register a new userFourier-transform spectroscopy of Sr2 and revised ground state potential
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Alexander Stein Mr.
Publication date
2009
fields
Physics
and research's language is
English
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Precise potentials for the ground state X1Sigma+g and the minimum region of the excited state 2_1Sigma+u of Sr2 are derived by high resolution Fourier-transform spectroscopy of fluorescence progressions from single frequency laser excitation of Sr2 produced in a heat pipe at 950 Celsius. A change of the rotational assignment by four units compared to an earlier work (G. Gerber, R. Moller, and H. Schneider, J. Chem. Phys. 81, 1538 (1984)) is needed for a consistent description leading to a significant shift of the potentials towards longer inter atomic distances. The huge amount of ground state data derived for the three different isotopomers 88Sr2, 86Sr88Sr and 87Sr88Sr (almost 60% of all excisting bound rovibrational ground state levels for the isotopomer 88Sr2) fixes this assignment undoubtedly. The presented ground state potential is derived from the observed transitions for the radial region from 4 to 11 A (9 cm-1 below the asymptote) and is extended to the longe range region by the use of theoretical dispersion coefficients together with already available photoassociation data. New estimations of the scattering lengths for the complete set of isotopic combinations are derived by mass scaling with the derived potential. The data set for the excited state 2_1Sigma+u was sufficient to derive a potential energy curve around the minimum.
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Fourier transform spectroscopy with classical interferometry corresponds to the measurement of a single-photon intensity spectrum from the viewpoint of the particle nature of light. In contrast, the Fourier transform of two-photon quantum interference patterns provides the intensity spectrum of the two photons as a function of the sum or difference frequency of the constituent photons. This unique feature of quantum interferometric spectroscopy offers a different type of spectral information from the classical measurement and may prove useful for nonlinear spectroscopy with two-photon emission. Here, we report the first experimental demonstration of two-photon quantum interference of photon pairs emitted via biexcitons in the semiconductor CuCl. Besides applying Fourier transform to quantum interference patterns, we reconstruct the intensity spectrum of the biexciton luminescence in the two-photon sum or difference frequency. We discuss the connection between the reconstructed spectra and exciton states in CuCl as well as the capability of quantum interferometry in solid-state spectroscopy.
We report on the creation of ultracold 84Sr2 molecules in the electronic ground state. The molecules are formed from atom pairs on sites of an optical lattice using stimulated Raman adiabatic passage (STIRAP). We achieve a transfer efficiency of 30% and obtain 4x10^4 molecules with full control over the external and internal quantum state. STIRAP is performed near the narrow 1S0-3P1 intercombination transition, using a vibrational level of the 0u potential as intermediate state. In preparation of our molecule association scheme, we have determined the binding energies of the last vibrational levels of the 0u, 1u excited-state, and the 1Sigma_g^+ ground-state potentials. Our work overcomes the previous limitation of STIRAP schemes to systems with Feshbach resonances, thereby establishing a route that is applicable to many systems beyond bi-alkalis.
The Ti:Saphire laser operated within 13800 - 11800 cm$^{-1}$ range was used to excite the $c^3Sigma^+$ state of KCs molecule directly from the ground $X^1Sigma^+$ state. The laser-induced fluorescence (LIF) spectra of the $c^3Sigma^+ rightarrow a^3Sigma^+$ transition were recorded with Fourier-transform spectrometer within 8000 to 10000 cm$^{-1}$ range. Overall 673 rovibronic term values belonging to both $e/f$-components of the $c^3Sigma^+(Omega=1^{pm})$ state of $^{39}$KCs, covering vibrational levels from $v$ = 0 to about 45, and rotational levels $Jin [11,149]$ were determined with the accuracy of about 0.01 cm$^{-1}$; among them 7 values for $^{41}$KCs. The experimental term values with $vin [0,22]$ were involved in a direct point-wise potential reconstruction for the $c^3Sigma^+(Omega=1^{pm})$ state, which takes into account the $Omega$-doubling effect caused by the spin-rotational interaction with the nearby $c^3Sigma^+(Omega=0^-)$ state. The analysis and interpretation were facilitated by the fully-relativistic coupled cluster calculation of the potential energy curves for the $B^1Pi$, $c^3Sigma^+$, and $b^3Pi$ states, as well as of spin-forbidden $c-X$ and spin-allowed $c-a$ transition dipole moments; radiative lifetimes and vibronic branching ratios were calculated. A comparison of relative intensity distributions measured in vibrational $c-a$ LIF progressions with their theoretical counterparts unambiguously confirms the vibrational assignment suggested in [emph{J. Szczepkovski, et. al.}, JQSRT, textbf{204}, 133-137 (2018)].
The lowest doublet electronic state for the lithium trimer (2A) is calculated for use in three-body scattering calculations using the valence electron FCI method with atomic cores represented using an effective core potential. It is shown that an accurate description of core-valence correlation is necessary for accurate calculations of molecular bond lengths, frequencies and dissociation energies. Interpolation between 2A ab initio surface data points in a sparse grid is done using the global interpolant moving least squares method with a smooth radial data cutoff function included in the fitting weights and bivariate polynomials as a basis set. The Jahn-Teller splitting of the 2E surface into the 2A1 and 2B2 states is investigated using a combination of both CASSCF and FCI levels of theory. Additionally, preliminary calculations of the 2A surface are also presented using second order spin restricted open-shell Moller-Plesset perturbation theory.
Accurate Fourier-transform spectroscopic absorption measurements of vacuum ultraviolet transitions in atomic nitrogen and carbon were performed at the Soleil synchrotron. For $^{14}$N transitions from the $2s^22p^3,^4$S$_{3/2}$ ground state and from the $2s^22p^3,^2$P and $^2$D metastable states were determined in the $95 - 124$ nm range at an accuracy of $0.025,mathrm{cm}^{-1}$. Combination of these results with data from previous precision laser experiments in the vacuum ultraviolet range reveal an overall and consistent offset of -0.04 wn from values reported in the NIST database. %The splitting of the $2s^22p^3,^4$S$_{3/2}$ -- %$2s2p^4,^4$P$_{5/2,3/2,1/2}$ The splittings of the $2s^22p^3,^4$S$_{3/2}$ -- $2s2p^4,^4$P$_{J}$ transitions are well-resolved for $^{14}$N and $^{15}$N and isotope shifts determined. While excitation of a $2p$ valence electron yields very small isotope shifts, excitation of a $2s$ core electron results in large isotope shifts, in agreement with theoretical predictions. For carbon six transitions from the ground $2s^22p^2,^3$P$_{J}$ and $2s^22p3s, ^3$P$_{J}$ excited states at $165$ nm are measured for both $^{12}$C and $^{13}$C isotopes.
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