This thesis reports the investigation of the scattering properties of a mixture of Rb and Cs and the formation of ultracold Feshbach molecules. The production of Feshbach molecules is a crucial step towards the production of ultracold polar molecules, which is of significant interest for a wide range of potential applications. We have investigated the scattering properties of a mixture of
85Rb and
133Cs in their lowest spin channel in a magnetic field range from 0 to 700\,G. Furthermore, we explored the Feshbach spectrum of
85Rb alone in both, the
(f=2,mf=−2) and
(2,+2) states up to a magnetic field of 1000\,G. Additionally a Feshbach resonance in a
(2,+2)+(3,+3) spin mixture was experimentally confirmed. We associated Cs
2 Feshbach molecules using a Feshbach resonance at 19.9\,G. \mbox{
2.1(1)×104} molecules with a temperature of
∼60\,nK were produced from a sample of
3.28(2)×105 Cs atoms with a PSD of 0.20(1). Due to a magnetic field gradient, the molecules `bounce' at an avoided crossing between two states at 13.5\,G. This gradient field was also used to produce multiple molecular clouds from one atomic sample. A combination of both techniques led to a `collision' between two Cs
2 clouds. Furthermore, we associated up to
∼5000 heteronuclear
87RbCs Feshbach molecules using an interspecies resonance at 197.1\,G. Confined in the dipole trap the molecules have a lifetime of 0.21(1)\,s. We have measured the magnetic moment of the molecules in different internal states in a magnetic field range from 181 to 185\,G. Molecular loss spectroscopy on electronically excited states was performed to identify candidates for the intermediate state of a STIRAP transfer of the molecules into their rovibrational ground state. Subsequently, the binding energy of the rovibrational ground state was measured to be 3811.574(1)\,cm
−1, using two-photon spectroscopy.
We have studied interspecies scattering in an ultracold mixture of
87Rb and
133Cs atoms, both in their lowest-energy spin states. The three-body loss signatures of 30 incoming
s- and
p-wave magnetic Feshbach resonances over the range 0 to 667 G have been cataloged. Magnetic field modulation spectroscopy was used to observe molecular states bound by up to 2.5 $\text{MHz}\ifmmode\times\else\texttimes\fi{}h$. We have created RbCs Feshbach molecules using two of the resonances. Magnetic moment spectroscopy along the magnetoassociation pathway from 197 to 182 G gives results consistent with the observed and calculated dependence of the binding energy on magnetic field strength. We have set up a coupled-channel model of the interaction and have used direct least-squares fitting to refine its parameters to fit the experimental results from the Feshbach molecules, in addition to the Feshbach resonance positions and the spectroscopic results for deeply bound levels. The final model gives a good description of all the experimental results and predicts a large resonance near 790 G, which may be useful for tuning the interspecies scattering properties. Quantum numbers and vibrational wave functions from the model can also be used to choose optimal initial states of Feshbach molecules for their transfer to the rovibronic ground state using stimulated Raman adiabatic passage.
We report the successful production of an ultracold sample of absolute ground-state ^{23}Na^{87}Rb molecules. Starting from weakly bound Feshbach molecules formed via magnetoassociation, the lowest rovibrational and hyperfine level of the electronic ground state is populated following a high-efficiency and high-resolution two-photon Raman process. The high-purity absolute ground-state samples have up to 8000 molecules and densities of over 10^{11} cm^{-3}. By measuring the Stark shifts induced by external electric fields, we determined the permanent electric dipole moment of the absolute ground-state ^{23}Na^{87}Rb and demonstrated the capability of inducing an effective dipole moment over 1 D. Bimolecular reaction between ground-state ^{23}Na^{87}Rb molecules is endothermic, but we still observed a rather fast decay of the molecular sample. Our results pave the way toward investigation of ultracold molecular collisions in a fully controlled manner and possibly to quantum gases of ultracold bosonic molecules with strong dipolar interactions.
We report the binding energy of
87Rb133Cs molecules in their rovibrational ground state measured using an offset-free optical frequency comb based on difference frequency generation technology. We create molecules in the absolute ground state using stimulated Raman adiabatic passage (STIRAP) with a transfer efficiency of 88%. By measuring the absolute frequencies of our STIRAP lasers, we find the energy-level difference from an initial weakly bound Feshbach state to the rovibrational ground state with a resolution of $\ensuremath{\sim}5$ kHz over an energy-level difference of more than
114THz; this lets us discern the hyperfine splitting of the ground state. Combined with theoretical models of the Feshbach-state binding energies and ground-state hyperfine structure, we determine a zero-field binding energy of $h\ifmmode\times\else\texttimes\fi{}114\phantom{\rule{0.16em}{0ex}}268\phantom{\rule{0.16em}{0ex}}135.24(4)(3)\phantom{\rule{0.28em}{0ex}}\mathrm{M}\mathrm{Hz}$. To our knowledge, this is the most accurate determination to date of the dissociation energy of a molecule.
This thesis reports the creation and trapping of 87RbCs molecules in the absolute ground state with a temperature of 1 uK. We build a tunable narrow-linewidth laser system at 1550 nm and 980 nm, using a single high-finesse optical cavity as a reference for both colours. We use fibre-coupled electro-optic modulators to continuously tune both lasers. These allow a novel measurement of the free spectral range of the cavity to better than 1 part in 10^6. We perform one- and two-photon spectroscopy on 87RbCs Feshbach molecules and identify a suitable intermediate state for transfer to the molecular ground state. We measure the electric dipole moment of the molecular ground state as 1.225(3)(8) D, and demonstrate the highest lab-frame dipole moment of any ultracold molecular system at the time of measurement. We transfer the molecules to the electronic, rovibrational and hyperfine ground state using stimulated Raman adiabatic passage, with 88% efficiency. We measure the transition strengths and excited state linewidth for this transfer route. We develop a model for the transfer which includes the effect of laser linewidth, and find excellent agreement with experimental data. The molecular sample is trapped in an optical dipole potential, and has a lifetime of 0.89(6) s. We reference the STIRAP lasers to a novel design of frequency comb which uses difference frequency generation to cancel the carrier-envelope offset. We use this to measure the binding energy of the molecules as h x 114 268 135.24(4)(3) MHz. To our knowledge, this is the most precise determination of the dissociation energy of a molecule to date. Finally, we report progress toward loading the molecules into a 1D optical lattice at 1064 nm. We develop the tools and methods to characterise a lattice, and demonstrate trapping of Feshbach molecules in both a 1D optical lattice and a harmonic optical potential at 1064 nm.
We produce ultracold dense trapped samples of ^{87}Rb^{133}Cs molecules in their rovibrational ground state, with full nuclear hyperfine state control, by stimulated Raman adiabatic passage (STIRAP) with efficiencies of 90%. We observe the onset of hyperfine-changing collisions when the magnetic field is ramped so that the molecules are no longer in the hyperfine ground state. A strong quadratic shift of the transition frequencies as a function of applied electric field shows the strongly dipolar character of the RbCs ground-state molecule. Our results open up the prospect of realizing stable bosonic dipolar quantum gases with ultracold molecules.