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arXiv:2302.09113

High resolution photoassociation spectroscopy of the excited $c^3Σ_{1}^+$ potential of $^{23}$Na$^{133}$Cs

Lewis R. B. Picard, Jessie T. Zhang, William B. Cairncross, Kenneth Wang, Gabriel E. Patenotte, Annie Jihyun Park, Yichao Yu, Lee R. Liu, Jonathan D. Hood, Rosario González‐Férez, Kang-Kuen Ni

Published Feb 17, 2023• 0 citations
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Abstract

We report on photoassociation spectroscopy probing the $c^3Σ_{1}^+$ potential of the bi-alkali NaCs molecule, identifying eleven vibrational lines between $v' = 0$ and $v' = 25$ of the excited $c^3Σ_{1}^+$ potential, and resolving their rotational and hyperfine structure. The observed lines are assigned by fitting to an effective Hamiltonian model of the excited state structure with rotational and hyperfine constants as free parameters. We discuss unexpected broadening of select vibrational lines, and its possible link to strong spin-orbit coupling of the $c^3Σ_{1}^+$ potential with the nearby $b^3Π_1$ and $B^1Π_1$ manifolds. Finally we report use of the $v' = 22$ line as an intermediate state for two-photon transfer of weakly bound Feshbach molecules to the rovibrational ground state of the $X^1Σ^+$ manifold.

DOI
10.48550/arxiv.2302.09113

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We report on photoassociation spectroscopy probing the c3Σ1+c^3Σ_{1}^+c3Σ1+​ potential of the bi-alkali NaCs molecule, identifying eleven vibrational lines between v′=0v' = 0v′=0 and v′=25v' = 25v′=25 of the excited c3Σ1+c^3Σ_{1}^+c3Σ1+​ potential, and resolving their rotational and hyperfine structure. The observed lines are assigned by fitting to an effective Hamiltonian model of the excited state structure with rotational and hyperfine constants as free parameters. We discuss unexpected broadening of select vibrational lines, and its possible link to strong spin-orbit coupling of the c3Σ1+c^3Σ_{1}^+c3Σ1+​ potential with the nearby b3Π1b^3Π_1b3Π1​ and B1Π1B^1Π_1B1Π1​ manifolds. Finally we report use of the v′=22v' = 22v′=22 line as an intermediate state for two-photon transfer of weakly bound Feshbach molecules to the rovibrational ground state of the X1Σ+X^1Σ^+X1Σ+ manifold.
We report on photoassociation spectroscopy probing the ${c}^{3}{\mathrm{\ensuremath{\Sigma}}}_{1}^{+}$ potential of the bialkali NaCs molecule, identifying 11 vibrational lines between ${v}^{\ensuremath{'}}=0$ and ${v}^{\ensuremath{'}}=25$ of the excited ${c}^{3}{\mathrm{\ensuremath{\Sigma}}}_{1}^{+}$ potential and fitting their rotational and hyperfine structure. The observed lines are assigned by fitting to an effective Hamiltonian model of the excited-state structure with rotational and hyperfine constants as free parameters. We discuss unexpected broadening of select vibrational lines and its possible link to strong spin-orbit coupling of the ${c}^{3}{\mathrm{\ensuremath{\Sigma}}}_{1}^{+}$ potential with the nearby ${b}^{3}{\mathrm{\ensuremath{\Pi}}}_{1}$ and ${B}^{1}{\mathrm{\ensuremath{\Pi}}}_{1}$ manifolds. Finally, we report use of the ${v}^{\ensuremath{'}}=22$ line as an intermediate state for two-photon transfer of weakly bound Feshbach molecules to the rovibrational ground state of the ${X}^{1}{\mathrm{\ensuremath{\Sigma}}}^{+}$ manifold.
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We report on high-resolution spectroscopy of ultracold fermionic 23 Na 40 K Feshbach molecules, and identify a two-photon pathway to the rovibrational singlet ground state via a resonantly mixed B 1 Π ∼ c 3 Σ + intermediate state.Photoassociation in a 23 Na-40 K atomic mixture and one-photon spectroscopy on 23 Na 40 K Feshbach molecules reveal about 20 vibrational levels of the electronically excited c 3 Σ + state.Two of these levels are found to be strongly perturbed by nearby B 1 Π levels via spinorbit coupling, resulting in additional lines of dominant singlet character in the perturbed complex. The dominantly singlet level is used to locate the absolute rovibrational singlet ground state v J X 0, 0via Autler-Townes spectroscopy.We demonstrate coherent two-photon coupling via dark state spectroscopy between the predominantly triplet Feshbach molecular state and the singlet ground state.Its binding energy is measured to be 5212.0447(1)cm -1 , a thousand-fold improvement in accuracy compared to previous determinations.In their absolute singlet ground state, 23 Na 40 K molecules are chemically stable under binary collisions and possess a large electric dipole moment of 2.72 Debye.Our work thus paves the way towards the creation of strongly dipolar Fermi gases of NaK molecules.
We have performed a type of Autler–Townes spectroscopy to locate a number of rovibrational-hyperfine levels of the a 3Σu+ potential, the lowest triplet potential of the Na2 dimer. The spectroscopy starts with the photoassociation of ultracold atoms in a magneto-optical trap. We have measured the binding energies of over 100 individual states spanning the vibrational levels v=8–15 of this potential (binding energies up to 27 cm−1). We obtain a typical accuracy of 15 MHz and a typical resolution of 20 MHz, improving on the 10 GHz accuracy and 30 GHz resolution previously available for the vibrational states v<12. Vibrational, rotational, and hyperfine structures are resolved. Additionally, we have been able to resolve the magnetic electron–electron spin–spin dipole splitting of a number of these hyperfine levels. The measured rotational and hyperfine structures show good agreement with theoretical calculations. An analysis of the remaining discrepancies indicates where possible refinements to the potentials can be made. We also observe evidence for the presence of second-order spin–orbit coupling.
We spectroscopically investigate the hyperfine, rotational, and Zeeman structure of the vibrational levels ${v}^{\ensuremath{'}}=0,7,13$ within the electronically excited $c{\phantom{\rule{0.222222em}{0ex}}}^{3}{\mathrm{\ensuremath{\Sigma}}}_{g}{}^{+}$ state of 87Rb2^{87}\mathrm{Rb}_{2}87Rb2​ for magnetic fields of up to 1000G1000\phantom{\rule{0.28em}{0ex}}\text{G}1000G. As spectroscopic methods we use short-range photoassociation of ultracold Rb atoms as well as photoexcitation of ultracold molecules which have been previously prepared in several well-defined quantum states of the $a{\phantom{\rule{0.222222em}{0ex}}}^{3}\mathrm{\ensuremath{\Sigma}}{}_{u}^{+}$ potential. As a by-product, we present optical two-photon transfer of weakly bound Feshbach molecules into $a{\phantom{\rule{0.222222em}{0ex}}}^{3}\mathrm{\ensuremath{\Sigma}}{}_{u}^{+}$, v=0v=0v=0 levels featuring different nuclear spin quantum numbers. A simple model reproduces well the molecular level structures of the $c{\phantom{\rule{0.222222em}{0ex}}}^{3}{\mathrm{\ensuremath{\Sigma}}}_{g}{}^{+}$ vibrational states and provides a consistent assignment of the measured resonance lines. Furthermore, the model can be used to predict the relative transition strengths of the lines. From fits to the data we extract for each vibrational level the rotational constant, the effective spin-spin interaction constant, as well as the Fermi contact parameter and the anisotropic hyperfine constant. In an alternative approach, we perform coupled-channel calculations where we fit the relevant potential energy curves, spin-orbit interactions, and hyperfine functions. The calculations reproduce the measured hyperfine level term frequencies with an average uncertainty of $\ifmmode\pm\else\textpm\fi{}9\phantom{\rule{0.28em}{0ex}}\mathrm{MHz}$, similar as for the simple model. From these fits we obtain a section of the potential energy curve for the $c{\phantom{\rule{0.222222em}{0ex}}}^{3}{\mathrm{\ensuremath{\Sigma}}}_{g}{}^{+}$ state which can be used for predicting the level structure for the vibrational manifold ${v}^{\ensuremath{'}}=0$ to 13 of this electronic state.
We present the formation of ultracold (85)Rb(133)Cs molecules in the (5)0(+) electronic state by photoassociation and their detection via resonance-enhanced two-photon ionization. Up to v = 47 vibrational levels including the lowest v = 0 vibrational and lowest J = 0 levels are identified with rotationally resolved high resolution photoassociation spectra. Precise Dunham coefficients are determined for the (5)0(+) state with high accuracy, then the Rydberg-Klein-Rees potential energy curve is derived. The electric dipole moments with respect to the vibrational numbers of the (5)0(+) electronic state of (85)Rb(133)Cs molecule are also measured in the range between 1.9 and 4.8 D. These comprehensive studies on previously unobserved rovibrational levels of the (5)0(+) state are helpful to understand the molecular structure and discover suitable transition pathways for transferring ultracold atoms to deeply bound rovibrational levels of the electronic ground state.