We demonstrate full quantum state control of two species of single atoms using optical tweezers and assemble the atoms into a molecule.Our demonstration includes 3D ground-state cooling of a single atom (Cs) in an optical tweezer, transport by several microns with minimal heating, and merging with a single Na atom.Subsequently, both atoms occupy the simultaneous motional ground state with 61(4)% probability.This realizes a sample of exactly two cotrapped atoms near the phase-space-density limit of one, and allows for efficient stimulated-Raman transfer of a pair of atoms into a molecular bound state of the triplet electronic ground potential a 3 Σ þ .The results are key steps toward coherent creation of single ultracold molecules for future exploration of quantum simulation and quantum information processing.
We demonstrate full quantum state control of two species of single atoms using optical tweezers and assemble the atoms into a molecule.Our demonstration includes 3D ground-state cooling of a single atom (Cs) in an optical tweezer, transport by several microns with minimal heating, and merging with a single Na atom.Subsequently, both atoms occupy the simultaneous motional ground state with 61(4)% probability.This realizes a sample of exactly two cotrapped atoms near the phase-space-density limit of one, and allows for efficient stimulated-Raman transfer of a pair of atoms into a molecular bound state of the triplet electronic ground potential a 3 Σ þ .The results are key steps toward coherent creation of single ultracold molecules for future exploration of quantum simulation and quantum information processing.
Recent theoretical and experimental advances have led to better understanding and control of simple molecules, bringing them to the forefront of quantum science. Diatomic polar molecules, with their vibrational and rotational degrees of freedom and electric dipole moment, are excellent candidates for a scalable qubit, probes of beyond-Standard Model physics, and quantum simulation of topological and chiral many-body systems. These applications call for high-phase space density (PSD) of molecules in a single quantum state. To date, the highest molecular PSD is achieved by coherently associating degenerate quantum gases of atoms into molecules. However, this requires fine-tuning of experimental parameters to maximize spatial overlap of the atomic density distributions while minimizing three-body recombination of the atoms.\nIn this thesis, we propose a bottom-up solution to gain single particle control of ultracold molecules for the first time. We use optical tweezers to deterministically assemble a single NaCs molecule in a single quantum state from a pair of Na and Cs atoms. Added benefits of using optical tweezers include: tight confinement of isolated atoms enabling cooling of Na and Cs to their quantum ground state of motion in less than 100~ms, and dynamic reconfigurability of optical tweezer arrays which will allow scaling up to defect-free arrays of single molecules. In the process, we realize a conceptually simple platform for studying atomic collisions and molecular spectra which derives its strength from the ability to gather "before" and "after" images of single atoms.
Chemical reactions can be surprisingly efficient at ultracold temperatures ( < 1mK) due to the wave nature of atoms and molecules. The study of reactions in the ultracold regime is a new research frontier enabled by cooling and trapping techniques developed in atomic and molecular physics. In addition, ultracold molecular gases that offer diverse molecular internal states and large electric dipolar interactions are sought after for studies of strongly interacting many-body quantum physics. Here we propose a new approach for producing ultracold molecules in the absolute internal and motional quantum ground state, where single molecules are assembled one by one from individual atoms. The scheme involves laser cooling, optical trapping, Raman sideband cooling, and coherent molecular state transfer. As a crucial initial step, we demonstrate quantum control of constituent atoms, including 3D ground-state cooling of a single Cs atom, in a simple apparatus. As laser technology advances to shorter wavelengths, additional atoms will be amenable to laser-cooling, allowing more diverse, and eventually more complex, molecules to be assembled with full quantum control.
Abstract We report simultaneous Raman sideband cooling of a single 87Rb atom and a single 133Cs atom held in separate optical tweezers at 814 nm and 938 nm, respectively. Starting from outside the Lamb-Dicke regime, after 45 ms of cooling we measure probabilities to occupy the three-dimensional motional ground state of 0.8 6 − 0.04 + 0.03 for Rb and 0.9 5 − 0.04 + 0.03 for Cs. Our setup overlaps the Raman laser beams used to cool Rb and Cs, reducing hardware requirements by sharing equipment along the same beam path. The cooling protocol is scalable, and we demonstrate cooling of single Rb atoms in an array of four tweezers. After motional ground-state cooling, a 938 nm tweezer is translated to overlap with a 814 nm tweezer so that a single Rb and a single Cs atom can be transferred into a common 1064 nm trap. By minimising the heating during the merging and transfer, we prepare the atoms in the relative motional ground state with an efficiency of 0.8 1 − 0.08 + 0.08 . This is a crucial step towards the formation of single RbCs molecules confined in optical tweezer arrays.
Ultracold molecules are attractive candidates for various applications including ultracold chemistry, quantum information processing, quantum simulation and searches for physics beyond the standard model. Combined with optical tweezer techniques, an optical tweezer array of ultracold polar molecules holds promise for versatile quantum applications. Their long-lived molecular rotational states form robust qubits, while the long-range dipolar interaction between molecules provides quantum entanglement. In this thesis, we build a new generation experiment of optical tweezer array of ultracold CaF molecules. We optically transport the laser cooled and optically trapped molecules into a science glass cell using a hybrid method, where high numerical aperture optical access allows for tighter optical tweezers. In an array of these tight optical tweezers, we demonstrate dipolar spin-exchange interactions between single CaF molecules for the first time. We realize the spin-21 quantum XY model by encoding an effective spin-21 system into the rotational states of the molecules, and use it to generate a Bell state through an iSWAP operation. Conditioned on the verified existence of molecules in both tweezers at the end of the measurement, we obtain a Bell state fidelity of 0.89(6). Employing interleaved tweezer arrays, we demonstrate single site molecular addressability. To further improve the platform, cooling of the molecules to near the motional ground state is crucial for reducing various dephasings. We demonstrate Raman sideband cooling (RSC) of CaF molecules in optical tweezers to near their 3-D motional ground state, with a 3-D motional ground state probability of 54±18% of the molecules that survive the RSC. This paves the way to increase molecular coherence times in optical tweezers for robust quantum information processing and simulation applications in the near future.
We report coherent association of atoms into a single weakly bound NaCs molecule in an optical tweezer through an optical Raman transition.The Raman technique uses a deeply bound electronic excited intermediate state to achieve a large transition dipole moment while reducing photon scattering.Starting from two atoms in their relative motional ground state, we achieve an optical transfer efficiency of 69%.The molecules have a binding energy of 770.2 MHz at 8.83(2) G.This technique does not rely on Feshbach resonances or narrow excited-state lines and may allow a wide range of molecular species to be assembled atom by atom.
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.