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 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.
Fully internal and motional state controlled and individually manipulable polar molecules are desirable for many quantum science applications leveraging the rich state space and intrinsic interactions of molecules. While prior efforts at assembling molecules from their constituent atoms individually trapped in optical tweezers achieved such a goal for exactly one molecule, here we extend the technique to an array of five molecules, unlocking the ability to study molecular interactions. We detail the technical challenges and solutions inherent in scaling this system up. With parallel preparation and control of multiple molecules in hand, this platform now serves as a starting point to harness the vast resources and long-range dipolar interactions of molecules.
Abstract Fully internal and motional state controlled and individually manipulable polar molecules are desirable for many quantum science applications leveraging the rich state space and intrinsic interactions of molecules. While prior efforts at assembling molecules from their constituent atoms individually trapped in optical tweezers achieved such a goal for exactly one molecule (Zhang J T et al 2020 Phys. Rev. Lett. 124 253401; Cairncross W B et al 2021 Phys. Rev. Lett. 126 123402; He X et al 2020 Science 370 331–5), here we extend the technique to an array of five molecules, unlocking the ability to study molecular interactions. We detail the technical challenges and solutions inherent in scaling this system up. With parallel preparation and control of multiple molecules in hand, this platform now serves as a starting point to harness the vast resources and long-range dipolar interactions of molecules.
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.
Control over the quantum states of individual molecules is crucial in the quest to harness their rich internal structure and dipolar interactions for applications in quantum science. In this paper, we develop a toolbox of techniques for the control and readout of individually trapped polar molecules in an array of optical tweezers. Starting with arrays of up to eight Rb and eight Cs atoms, we assemble arrays of RbCs molecules in their rovibrational and hyperfine ground state with an overall efficiency of 48(2)%. We demonstrate global microwave control of multiple rotational states of the molecules and use an auxiliary tweezer array to implement site-resolved addressing and state control. We show how the rotational state of the molecule can be mapped onto the position of Rb atoms and use this capability to readout multiple rotational states in a single experimental run. Further, using a scheme for the midsequence detection of molecule formation errors, we perform rearrangement of assembled molecules to prepare small defect-free arrays. Finally, we discuss a feasible route to scaling to larger arrays of molecules. Published by the American Physical Society 2024
Potential wide-ranging scientific applications, spanning fundamental physics to quantum engineering, has led to significant efforts in controlling molecules at the quantum level. The rich internal structure of molecules, that gives rise to these desirable properties also complicates the task of controlling such species. Over the past decade, our ability to produce, control, and detect molecules has advanced tremendously with direct laser-cooling and magneto-optical trapping of diatomic molecules realized by several groups around the world. In this thesis, we describe the creation of the first RF MOT of CaF, which at the time of the writing of this thesis, remains the largest and densest molecular MOT. New laser cooling techniques for molecules are demonstrated, allowing laser cooling of molecules to 4 uK, 50 times colder than the Doppler limit. Optical trapping of these molecules is also achieved, which, in combination with in-trap laser cooling increased the density of trapped molecules by five orders of magnitude compared to the density in the MOT. We developed methods to cool and detect single molecules with high fidelity, which aided us in the creation of an optical tweezer array of single, ultracold CaF molecules. The densities of molecules (10^12 cm^-3) attained inside the tweezer traps also enabled us to observe both light-assisted and ground state collisions of laser cooled molecules, for the first time. The phase space density within the merged tweezers reached 5x10^-4, 10 orders of magnitude larger than the initial MOT. We implemented internal quantum state control of the molecules and dynamical control of the tweezers to build a platform for exploring state-selective ultracold quantum chemistry.
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.