THE $^{1}\Pi$ STATES OF NaCs: SPECTROSCOPY, LIFETIMES, PERMANENT AND TRANSITION DIPOLE MOMENTS

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\maketitle The NaCs molecule is one of the prospective objects forproduction of ultracold polar molecules. LIF Fourier transform spectroscopy study is presented for the (1,3)$^{1}\Pi$ states with 0.03 cm$^{-1}$ resolution. Potential energy curves (PECs) are obtained by the Inverted Perturbation Approach reproducing (3)$^{1}\Pi$ state}, \underline{\textbf{124}}, 174310, 2006.} energies for $\emph{R}$ = 3 to 11 {\AA}. In the B(1)$^{1}\Pi$ state we accounted for numerous B(1)$^{1}\Pi \sim c^{3}\Sigma^{+}$ perturbations by omitting perturbed levels for the fit to construct the PEC for $\emph{R}$ = 2.6 to 8.4 {\AA}. The permanent electric dipole moments $\emph{d}$ and the $\Lambda$-splitting were measured}, \underline{\textbf{124}}, 184318, 2006.} by dc Stark mixing and electric RF-optical double resonance methods yielding $\emph{d}$ within 5 - 8 D for (3)$^{1}\Pi$ and $\emph{d} \sim$ 1 D for the D(2)$^{1}\Pi$ ($\emph{v} <$ 3) state. The radiative lifetimes $\tau$ were measured from LIF kinetics as $\tau$ = 29 to 21 ns for (3)$^{1}\Pi$ ($\emph{v}$ = 3 to 25) and $\tau$ = 37 ns for D(2)$^{1}\Pi$ ($\emph{v}$ = 0). The measured data are supported by electronic structure calculations for the (1-3)$^{1}\Pi$ states$^{b}$ by many-body multipartitioning perturbation theory of PECs, permanent and transition dipole moments, as well as angular coupling matrix elements for the lowest singlet states. The predicted $\emph{d}$ values reproduce their experimental counterparts within the measurement errors. Lifetimes for the (1-3)$^{1}\Pi$-states have been calculated in Hund's "a" coupling case using the approximate sum rule over the lower vibronic states. The spectra and formation rates of ultracold NaCs in the $X^{1}\Sigma^{+}$ ($\emph{v}$ = 0, $\emph{J}$ = 0) state were simulated for the optical cycle $a^{3}\Sigma^{+} \rightarrow B(1)^{1}\Pi \sim c^{3}\Sigma^{+} \sim b^{3}\Pi \rightarrow X^{1}\Sigma^{+}$. The Riga team and the Moscow team acknowledge support by NATO SfP 978029 Optical Field Mapping grant, the Hannover team support by the DFG through the SFB 407.

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Author Institution: University of Latvia, Department of Physics, LV-1586, Riga, Latvia; Sofia University, Department of Physics, 1164 Sofia, Bulgaria; Leibniz Universitat Hannover, Inst.f. Quantenoptik, 30167 Hannover, Germany; Moscow State University, Department of Chemistry, Moscow, 119899, Russia

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