A narrow-linewidth, dual-wavelength laser system is vital for the creation of ultracold ground state molecules via stimulated Raman adiabatic passage (STIRAP) from a weakly bound Feshbach state. Here we describe how a relatively simple apparatus consisting of a single fixed-length optical cavity can be used to narrow the linewidth of the two different wavelength lasers required for STIRAP simultaneously. The frequency of each of these lasers is referenced to the cavity and is continuously tunable away from the cavity modes through the use of non-resonant electro-optic modulators. Self-heterodyne measurements suggest the laser linewidths are reduced to several hundred Hz. In the context of 87Rb133Cs molecules produced via magnetoassociation on a Feshbach resonance, we demonstrate the performance of the laser system through one- and two-photon molecular spectroscopy. Finally, we demonstrate transfer of the molecules to the rovibrational ground state using STIRAP. ar X iv
A narrow-linewidth, dual-wavelength laser system is vital for the creation of ultracold ground state molecules via stimulated Raman adiabatic passage (STIRAP) from a weakly bound Feshbach state. Here we describe how a relatively simple apparatus consisting of a single fixed-length optical cavity can be used to narrow the linewidth of the two different wavelength lasers required for STIRAP simultaneously. The frequency of each of these lasers is referenced to the cavity and is continuously tunable away from the cavity modes through the use of non-resonant electro-optic modulators. Self-heterodyne measurements suggest the laser linewidths are reduced to several hundred Hz. In the context of 87Rb133Cs molecules produced via magnetoassociation on a Feshbach resonance, we demonstrate the performance of the laser system through one- and two-photon molecular spectroscopy. Finally, we demonstrate transfer of the molecules to the rovibrational ground state using STIRAP. ar X iv
A narrow-linewidth, dual-wavelength laser system is vital for the creation of ultracold ground state molecules via stimulated Raman adiabatic passage (STIRAP) from a weakly bound Feshbach state. Here we describe how a relatively simple apparatus consisting of a single fixed-length optical cavity can be used to narrow the linewidth of the two different wavelength lasers required for STIRAP simultaneously. The frequency of each of these lasers is referenced to the cavity and is continuously tunable away from the cavity modes through the use of non-resonant electro-optic modulators. Self-heterodyne measurements suggest the laser linewidths are reduced to several 100 Hz. In the context of 87 Rb 133 Cs molecules produced via magnetoassociation on a Feshbach resonance, we demonstrate the performance of the laser system through one- and two-photon molecular spectroscopy. Finally, we demonstrate transfer of the molecules to the rovibrational ground state using STIRAP.
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.
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.
Ultracold bialkali polar molecules play a leading part at the frontline of quantum physics. They recently attract a lot of attention in the field of ultracold quantum chemistry, quantum many-body physics and quantum simulations. The key for their success is the rich internal level structure with rotational and vibrational degrees of freedom and their large electric dipole moments. Still, only a handful of molecular species are available at ultracold temperatures until now, although it is highly desirable to produce new molecular species to further expand the range of applications. Besides direct laser cooling methods for molecules, the assembly of heteronuclear ground-state molecules from ultracold atomic mixtures is the most promising approach for the creation of polar molecules. It includes the formation of weakly bound Feshbach molecules from the diatomic mixture and the subsequent two-photon stimulated Raman adiabatic passage (STIRAP) transfer to the rovibrational ground state. This creation strategy has been successfully demonstrated for the first time in the pioneering experiments at JILA with ultracold 40K87Rb molecules. Since then, only a few more molecular species from different alkali atoms have been created, namely 6Li23Na, 23Na40K, 23Na87Rb and 87Rb133Cs. In this thesis, I report the successful creation of a new species of ultracold polar ground-state molecules: 23Na39K. Starting from an ultracold mixture of bosonic 23Na and 39K atoms, weakly bound molecules are created. For this purpose, a Feshbach resonance in a high angular momentum scattering channel is chosen, experimentally identified and characterized. Close to this resonance the weakly bound Feshbach molecules are formed using resonant radio frequency radiation. For the two-photon ground-state transfer, a unique, highly specialized two-color laser system is designed and realized. It is used for one- and two-photon spectroscopy to identify the relevant transitions for the ground-state transfer. Based on the obtained data, a local model of the singlet-triplet mixed excited state manifolds is developed, with which the hyperfine structure and the magnetic field dependence is predicted with high accuracy. According to these findings, a suitable pathway to a single hyperfine ground state is chosen considering selection rules and experimental conditions such as laser polarization and beam alignment. To precisely determine the two-photon resonance condition for STIRAP, electromagnetically induced transparency measurements are performed. The ground-state transfer is then performed using STIRAP. The experimental findings regarding the STIRAP are successfully supported theoretically by a model based on a five-level master equation. The pure molecular gas shows evidence for two-body dominated loss mechanisms, such as sticky four-body collisions. The molecule-atom mixture of 23Na39K+39K reveals an unexpectedly low loss rate coefficient although sticky three-body collisions are assumed to occur. This behavior demands further investigations regarding different hyperfine collisional chan-nels and magnetic field regions.
The thesis reports transferring the ultracold RbCs molecules to the absolute ground state and a trapping light that eliminates the differential AC Stark shift. We build a laser system to perform Stimulated Raman Adiabatic Passage (STIRAP) for the molecules trapped in tweezers, which transfer the molecules from the weakly- bounded state to the absolute ground state. We use the offset cavity stabilisation technique to stabilise the laser frequencies to a passive cavity to narrow the laser linewidths while keeping the laser frequency tunable. We then align the beams to the molecules. We demonstrate a “magic” laser frequency to eliminate the differential AC Stark shift of the rotational states in the ground vibrational state of RbCs molecule and to increase the rotational coherence time of multiple states. We study the AC Stark effect caused by the trapping light. We calculate the polarisabilities of the rotational states near a narrow electronic from X ^1Σ^+ state to b^3Π_0 state and found at certain laser frequency the polarisabilities become the same. We measure the transition frequencies to different vibrational states in the excited electronic state experimentally. We perform microwave spectroscopy to measure the light shift and show that the shift vanishes at the magic frequency. We confirmed the coherence in 1 ms timescale by measuring the Ramsey fringe contrast.
The production of a quantum gas with strong long - range dipolar interactions is a major scientific goal in the research field of ultracold gases. In their ro - vibrational ground state Li -K dimers possess a large permanent dipole moment, which could possibly be exploited for the realization of such a quantum gas. A production of these molecules can be achieved by the association of Li and K at a Feshbach resonance, followed by a coherent state transfer. In this thesis, detailed theoretical an experimental preparations to achieve state transfer by means of Stimulated Raman Adiabatic Passage (STIRAP) are described. The theoretical preparations focus on the selection of an electronically excited molecular state that is suitable for STIRAP transfer. In this context, molecular transition dipole moments for both transitions involved in STIRAP transfer are predicted for the first time. This is achieved by the calculation of Franck -Condon factors and a determination of the state in which the 6Li - 40K Feshbach molecules are produced. The calculations show that state transfer by use of a single STIRAP sequence is experimentally very well feasible. Further, the optical wavelengths that are needed to address the selected states are calculated. The high accuracy of the data will allow to carry out the molecular spectroscopy in a fast and efficient manner. Further, only a comparatively narrow wavelength tuneability of the spectroscopy lasers is needed. The most suitable Feshbach resonance for the production of 6Li - 40K molecules at experimentally manageable magnetic field strengths is occurring at 155G. Experimentally, this resonance is investigated by means of cross - dimensional relaxation. The application of the technique at various magnetic field strengths in the vicinity of the 155G Feshbach resonance allows a determination of the resonance position and width with so far unreached precision. This reveals the production of molecules on the atomic side of the resonance, thereby establishing the first observation of a many body effect in the crossover regime of a narrow Feshbach resonance. Further, mass dependent factors, with which the equilibration of an induced anisotropic temperature of the trapped particle samples can be described, are experimentally determined for the first time. The type of resonance as well as the measured molecular lifetimes are found to be very well suited for STIRAP transfer. A Raman laser system is designed based on the transition wavelengths and durations of state transfer which are predicted. As the wavelengths of the Raman lasers differ widely but coherence of the light fields is needed, the technical realization of a laser system is challenging. As a part of the laser system, the construction and characterization of a reference optical resonator are presented. Laser frequency stabilization with a linewidth of approximately 500Hz and an Allan deviation below 10−12 for timespans up to several ten seconds are demonstrated. Further, the stabilization of a frequency comb to this reference laser is demonstrated. For the laser spectroscopy of electronically excited Li -K states an interferometric laser frequency stabilization will be used. The device is a commercial design, for which a calibration procedure that enhances the precision by several orders of magnitude is worked out within this thesis. The calibration scheme includes the precise measurement of the stabilization’s wavelength dependent frequency deviations by means of a frequency comb. By the implementation of several calibration steps a remaining frequency deviation of less than 5.7MHz (rms 1.6MHz) in the whole relevant wavelength range 750 - 795 nm is achieved. Only the exceptional precision of the fully calibrated device permits the usage for the Li -K spectroscopy, while the demonstrated wide tuning capability facilitates the completion of the latter in a fast and convenient manner.