Abstract We present a study of two-photon pathways for the transfer of NaCs molecules to their rovibrational ground state. Starting from NaCs Feshbach molecules, we perform bound-bound excited state spectroscopy in the wavelength range from 900 nm to 940 nm, covering more than 30 vibrational states of the c 3 Σ + , b 3 Π , and B 1 Π electronic states. Analyzing the rotational substructure, we identify the highly mixed c 3 Σ 1 + | v = 22 ⟩ ∼ b 3 Π 1 | v = 54 ⟩ state as an efficient bridge for stimulated Raman adiabatic passage. We demonstrate transfer into the NaCs ground state with an efficiency of up to 88(4)%. Highly efficient transfer is critical for the realization of many-body quantum phases of strongly dipolar NaCs molecules and high fidelity detection of single molecules, for example, in spin physics experiments in optical lattices and quantum information experiments in optical tweezer arrays.
Abstract We present a study of two-photon pathways for the transfer of NaCs molecules to their rovibrational ground state. Starting from NaCs Feshbach molecules, we perform bound-bound excited state spectroscopy in the wavelength range from 900 nm to 940 nm, covering more than 30 vibrational states of the c 3 Σ + , b 3 Π , and B 1 Π electronic states. Analyzing the rotational substructure, we identify the highly mixed c 3 Σ 1 + | v = 22 ⟩ ∼ b 3 Π 1 | v = 54 ⟩ state as an efficient bridge for stimulated Raman adiabatic passage. We demonstrate transfer into the NaCs ground state with an efficiency of up to 88(4)%. Highly efficient transfer is critical for the realization of many-body quantum phases of strongly dipolar NaCs molecules and high fidelity detection of single molecules, for example, in spin physics experiments in optical lattices and quantum information experiments in optical tweezer arrays.
We demonstrate the coherent creation of a single NaCs molecule in its rotational, vibrational, and electronic (rovibronic) ground state in an optical tweezer. Starting with a weakly bound Feshbach molecule, we locate a two-photon transition via the |c^{3}Σ_{1},v^{'}=26⟩ excited state and drive coherent Rabi oscillations between the Feshbach state and a single hyperfine level of the NaCs rovibronic ground state |X^{1}Σ,v^{''}=0,N^{''}=0⟩ with a binding energy of D_{0}=h×147044.63(11) GHz. We measure a lifetime of 3.4±1.6 s for the rovibronic ground state molecule, which possesses a large molecule-frame dipole moment of 4.6D and occupies predominantly the motional ground state. These long-lived, fully quantum-state-controlled individual dipolar molecules provide a key resource for molecule-based quantum simulation and information processing.
One possibility for the creation of ultracold, high phase space density quantum gases of molecules in the rovibronic ground state relies on first associating weakly-bound molecules from quantum-degenerate atomic gases on a Feshbach resonance and then transferring the molecules via several steps of coherent two-photon stimulated Raman adiabatic passage (STIRAP) into the rovibronic ground state. Here, in ultracold samples of Cs2 Feshbach molecules produced out of ultracold samples of Cs atoms, we observe several optical transitions to deeply-bound rovibrational levels of the excited 0(u)+ molecular potentials with high resolution. At least one of these transitions, although rather weak, allows efficient STIRAP transfer into the deeply-bound vibrational level (see text for symbols)v = 73 > of the singlet X1 sigma(g)+ ground state potential, as recently demonstrated (J. G. Danzl, E. Haller, M. Gustavsson, M. J. Mark, R. Hart, N. Bouloufa, O. Dulieu, H. Ritsch, and H.-C. Nägerl, Science, 2008, 321, 1062). From this level, the rovibrational ground state (see text for symbols)v = 0, J = 0 > can be reached with one more transfer step. In total, our results show that coherent ground state transfer for Cs2 is possible using a maximum of two successive two-photon STIRAP processes or one single four-photon STIRAP process.
We perform one- and two-photon high resolution spectroscopy on ultracold samples of RbCs Feshbach molecules with the aim to identify a suitable route for efficient ground-state transfer in the quantum-gas regime to produce quantum gases of dipolar RbCs ground-state molecules. One-photon loss spectroscopy allows us to probe deeply bound rovibrational levels of the mixed excited (A(1)Σ(+)-b(3)Π)0(+) molecular states. Two-photon dark state spectroscopy connects the initial Feshbach state to the rovibronic ground state. We determine the binding energy of the lowest rovibrational level |v'' = 0, J'' = 0> of the X(1)Σ(+) ground state to be D = 3811.5755(16) cm(-1), a 300-fold improvement in accuracy with respect to previous data. We are now in the position to perform stimulated two-photon Raman transfer to the rovibronic ground state.
Obtaining effective spontaneous radiative transition channels is a fundamental topic in the preparation of ultracold rovibrational ground states of molecules. Herein, the ranges of prospective transition channels in the NaCs dimer are predicted via exploring the complex energy level structure and transition properties. The potential energy curves of \ensuremath{\Lambda}-S states and \ensuremath{\Omega} states, spectroscopy constants, absolute energies of bound states, and transition information (Frank-Condon factors, lifetimes, transition dipole moments) have been researched. With this purpose, the results of our experiment on binding energies of the ${b}^{3}{\mathrm{\ensuremath{\Pi}}}_{0}{}^{+}$ rovibrational states are analyzed; the transition from the higher (photoassociated) ${}^{1}\mathrm{\ensuremath{\Pi}}$ state to the ground ${X}^{1}{\mathrm{\ensuremath{\Sigma}}}^{+}$ state is discussed. The wavelengths of the two lasers are predicted as 622.8-656.7 nm and 896.3-969.8 nm with the ${B}^{1}{\mathrm{\ensuremath{\Pi}}}_{1}$ and ${c}^{3}{\mathrm{\ensuremath{\Sigma}}}_{1}^{+}$ states, respectively, for the stimulated raman adiabatic passage method.
We report on the creation of bosonic NaCs molecules in their absolute rovibrational ground state via stimulated Raman adiabatic passage. We create ultracold gases with up to 22 000 dipolar NaCs molecules at a temperature of 300(50) nK and a peak density of 1.0(4)×10^{12} cm^{-3}. We demonstrate comprehensive quantum state control by preparing the molecules in a specific electronic, vibrational, rotational, and hyperfine state. We measure the ground state ac polarizability at 1064 nm along with the two-body loss rate, which we find to be universal. Employing the tunability and strength of the permanent electric dipole moment of NaCs, we induce dipole moments of up to 2.6 D at a dc electric field of 2.1(2) kV/cm and demonstrate strong microwave coupling between the two lowest rotational states with a Rabi frequency of 2π×45 MHz. A large electric dipole moment, accessible at relatively small electric fields, makes ultracold gases of NaCs molecules well suited for the exploration of strongly interacting phases of dipolar quantum matter.
Abstract We spectroscopically investigate a pathway for the conversion of 23Na39K Feshbach molecules into rovibronic ground state molecules via stimulated Raman adiabatic passage. Using photoassociation spectroscopy from the diatomic scattering threshold in the a 3Σ+ potential, we locate the resonantly mixed electronically excited intermediate states ∣ B 1 Π , v = 8 〉 and ∣ c 3 Σ + , v = 30 〉 which, due to their singlet–triplet admixture, serve as an ideal bridge between predominantly a 3Σ+ Feshbach molecules and pure X 1Σ+ ground state molecules. We investigate their hyperfine structure and present a simple model to determine the singlet–triplet coupling of these states. Using Autler–Townes spectroscopy, we locate the rovibronic ground state of the 23Na39K molecule ( ∣ X 1 Σ + , v = 0 , N = 0 〉 ) and the second rotationally excited state N = 2 to unambiguously identify the ground state. We also extract the effective transition dipole moment from the excited to the ground state. Our investigations result in a fully characterized scheme for the creation of ultracold bosonic 23Na39K ground state molecules.