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.
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.
Molecules, with their rich spectrum of internal states as well as strong and tunable dipolar interactions, are promising candidates for a broad range of experiments including quantum information, quantum chemistry, precision measurement and probing physics beyond the Standard Model, and quantum simulation of interacting many-body systems. At the same time, the complexity that made them attractive also poses a significant challenge to achieve a high level of quantum control that is required in many of their potential applications. Multiple approaches are being pursued for full quantum control of molecules including association of atomic gases and direct cooling of molecules, yet it remains challenging to control molecules at single particle level due to the difficulty in tuning the atom-atom interaction and laser cooling of molecules. In this thesis, we achieved full control on a single weakly bound ground state molecule created by coherent optical association from single atoms. We first discuss the trapping and imaging of the atoms in the optical tweezer and the cooling into a single quantum state in order to achieve the quantum control of atoms. Combining this control with the resolution and flexibility of tweezers. we developed a versatile platform to study interactions between single atoms and properties of single molecules, using precise optical spectroscopy on pairs of atoms in the tweezer. Based on these studies, we proposed a promising pathway for coherent all-optical creation of molecules and experimentally demonstrated full control on the molecule including all degrees of freedom.
Ultracold polar molecules possess a manifold of long-lived molecular rotational states, which can be coherently controlled using microwave fields and entangled by the long-range dipole-dipole interactions between molecules. The ability to control these features at the individual molecule level provides a rich toolbox with which to engineer quantum simulations of exotic materials or build a molecular quantum computer. Until recently, this level of single molecule control has eluded researchers due to the challenges inherent in taming the complex internal structure of molecules. In this thesis, we demonstrate full control over the internal quantum states and coherent interactions of individual NaCs molecules in optical tweezers. This platform is based on coherent assembly of ultracold Na and Cs atoms trapped and cooled in separate arrays, before being magnetoassociated at a Feshbach resonance to form weakly-bound molecules. Using high-resolution spectroscopy of electronically excited molecular states, we identify an efficient two-photon pathway to the rovibrational ground state of NaCs that we use to prepare an array of ground state molecules in tweezers. We demonstrate a "magic ellipticity'' technique to eliminate differential light shifts between two molecular rotational states and achieve coherence times of up to 250(40) ms for a superposition of those states. We then show that we can rearrange molecules in an array to eliminate defects and perform single-shot readout of multiple rotational states using controlled molecule dissociation and imaging of constituent atoms at high magnetic field. Finally, we coherently control the dipole-dipole interactions between two molecules, producing a Bell state with a fidelity of 94(3) % and demonstrating a universal entangling iSWAP gate for qubits encoded in molecular hyperfine states.
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.
The ability to control particles in the quantum regime at the individual particle level is a challenge at the frontier of quantum science and engineering. Of the many quantum objects developed in pursuit of this goal, ultracold molecules host rich internal states and unique inter-particle interactions that could lend themselves useful to a broad range of applications including quantum computing and simulation, precision measurements and quantum chemistry. In this thesis we present a bottom-up approach to creating single molecules in individual optical tweezers. In particular, single atoms of two different species are first trapped and cooled in individual optical tweezers then brought together to form a single molecule coherently. Using this approach, we have successfully created an array of fully quantum-state-controlled polar molecules. The quantum state – including both internal and external states – of the resulting molecules are known to us, and is the first time single neutral molecules have been under full quantum state control. This platform offers exciting new opportunities to harness the rich properties of molecules in many quantum science applications.
The realization of rovibrationally stable dense samples of ultracold diatomic molecules remains one of the main stepping stones to achieve the next slate of major goals in the field of atomic and molecular physics. Though obtaining diatomic alkali molecules was seen as a logical next step following the optical cooling of atoms, many of the possible applications currently under investigation extend beyond atomic and molecular physics. For example, spectroscopy of ultracold molecules can help in testing extensions of the Standard Model via the search for a permanent electric dipole moment of the electron (1; 2), or the energy difference between enantiomers of chiral molecules (3). Various molecular transitions can be utilized to track the time dependence of fundamental constants, including the fine structure constant and the proton to electron mass ratio (4). They also open the way for cold and ultracold chemistry, where the interacting species and products are in a coherent quantum superposition state (5) and reactions can happen via quantum tunneling. Dipolar ultracold quantum gases promise to show a plethora of new phenomena due to anisotropic long-range dipole-dipole interactions (6). Dipolar molecules in optical lattices can be employed as a quantum simulator of condensed matter systems, and they are predicted to demonstrate new quantum phases such as a dipolar crystal, supersolid, checkerboard and collapse phases (7; 8). Ultracold polar molecules also represent an attractive platform for quantum computation (9). They offer a variety of long-lived states for qubit encoding, including rotational, spin and hyperfine (if electronic and nuclear spins are non-zero), Λ and Ω-doublet states (10) and scalability to a large number of qubits. Polar molecules can be easily controlled by DC electric and magnetic fields, as well as bymicrowave and optical fields, allowing the design of various traps (11; 12). The main appeal of polar molecules for quantum information processing, however, comes from their permanent electric dipole moment, permitting them to interact via a long-range dipole-dipole interaction. The dipole-dipole interaction offers a tool to construct two-qubit gates, required for universal quantum computation (9; 13). Ultracold molecules in their ground vibrational state v = 0 (and even in specific rotational, hyperfine or Zeeman states) are required formany of these applications since they have a large permanent electric dipole moment and are stable with respect to collisions and spontaneous emission. Currently translationally ultracold (100 nK 1 mK) molecules are produced by magneto(14) and photo-association (15) techniques. In a typical photoassociation scheme, 3
Chemical reactions typically proceed via stochastic encounters between reactants. Going beyond this paradigm, we combined exactly two atoms in a single, controlled reaction. The experimental apparatus traps two individual laser-cooled atoms [one sodium (Na) and one cesium (Cs)] in separate optical tweezers and then merges them into one optical dipole trap. Subsequently, photoassociation forms an excited-state NaCs molecule. The discovery of previously unseen resonances near the molecular dissociation threshold and measurement of collision rates are enabled by the tightly trapped ultracold sample of atoms. As laser-cooling and trapping capabilities are extended to more elements, the technique will enable the study of more diverse, and eventually more complex, molecules in an isolated environment, as well as synthesis of designer molecules for qubits.