We report on a novel bichromatic fluorescent imaging scheme for background-free detection of single CaF molecules trapped in an optical tweezer array. By collecting fluorescence on one optical transition while using another for laser cooling, we achieve an imaging fidelity of 97.7(2)% and a nondestructive detection fidelity of 95.5(6)%. Notably, these fidelities are achieved with a modest photon budget, suggesting that the method could be extended to more complex laser-coolable molecules with less favorable optical cycling properties. We also report on a framework and new methods to characterize various loss mechanisms that occur generally during fluorescent detection of trapped molecules, including two-photon decay and admixtures of higher excited states that are induced by the trapping light. In particular, we develop a novel method to dispersively measure transition matrix elements between electronically excited states. The method could also be used to measure arbitrarily small Franck-Condon factors between electronically excited states, which could significantly aid in ongoing efforts to laser cool complex polyatomic molecules.
We report on a novel bichromatic fluorescent imaging scheme for background-free detection of single CaF molecules trapped in an optical tweezer array. By collecting fluorescence on one optical transition while using another for laser cooling, we achieve an imaging fidelity of 97.7(2)% and a nondestructive detection fidelity of 95.5(6)%. Notably, these fidelities are achieved with a modest photon budget, suggesting that the method could be extended to more complex laser-coolable molecules with less favorable optical cycling properties. We also report on a framework and new methods to characterize various loss mechanisms that occur generally during fluorescent detection of trapped molecules, including two-photon decay and admixtures of higher excited states that are induced by the trapping light. In particular, we develop a novel method to dispersively measure transition matrix elements between electronically excited states. The method could also be used to measure arbitrarily small Franck-Condon factors between electronically excited states, which could significantly aid in ongoing efforts to laser cool complex polyatomic molecules.
Scalable atom-based quantum platforms for simulation, computing, and metrology require fast high-fidelity, low-loss imaging of individual atoms. Standard fluorescence detection methods rely on continuous cooling, limiting the detection range to one atom and imposing long imaging times that constrain the experimental cycle and midcircuit conditional operations. Here, we demonstrate fast and low-loss single-atom imaging in optical tweezers without active cooling, enabled by the favorable properties of ytterbium. Collecting fluorescence over microsecond timescales, we reach single-atom discrimination fidelities above 99.9% and single-shot survival probabilities above 99.5%. Through interleaved recooling pulses, as short as a few hundred microseconds for atoms in magic traps, we perform tens of consecutive detections with constant atom-retention probability per image-an essential step toward fast atom reuse in tweezer-based processors and clocks. Our scheme does not induce parity projection in multiply occupied traps, enabling number-resolved single-shot detection of several atoms per site. This allows us to study the near-deterministic preparation of single atoms in tweezers driven by blue-detuned light-assisted collisions. Moreover, the near-diffraction-limited spatial resolution of our low-loss imaging enables number-resolved microscopy in dense arrays, opening the way to direct site-occupancy readout in optical lattices for density fluctuation and correlation measurements in quantum simulators.
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.
Optical tweezer arrays of neutral atoms have emerged as a versatile and powerful platform for quantum simulation and quantum information processing. In this thesis, I present the realization of an experimental platform for quantum simulation based on individually trapped strontium atoms in optical tweezer arrays. The experiment combines precise laser cooling, optical control, and high-resolution imaging to enable the manipulation and high fidelity detection of single atoms. I developed and optimized a two-stage three-dimensional magneto-optical trap (3D-MOT) that produces cold and dense samples of strontium atoms from a thermal beam. In the f irst stage, atoms are captured and precooled using the dipole-allowed 1S0 → 1P1 transition at 461nm (which has a linewidth of !=2ω ↑ 32MHz). The second stage employs the 1S0 → 3P1 narrow intercombination transition at 689nm (with a linewidth of !=2ω ↑7.5kHz) to further cool and compress the atomic cloud. By optimizing the trapping parameters, I achieved clouds with temperatures around 5μK and densities above 1010cm→3, providing ideal initial conditions for e!cient loading into optical tweezers. A 3↑3 array of 360μK deep optical tweezers is generated by spatially modulating an 813.4nm laser beam using two crossed acousto-optic deflectors. The deflected beams are relayed and focused into the science chamber using a high–numericalaperture objective, which simultaneously serves as the collection optics for atomic f luorescence. The fluorescence light emitted by the atoms is imaged onto a scientific qCMOS camera, enabling site-resolved detection of individual atoms. I implemented and optimized the in-trap cooling dynamics to prevent atom loss during imaging and to minimize residual thermal motion. In addition, by precisely tuning lightassisted collisions, multiple atoms occupancies are removed from the traps and a single-atom regime is reached in the array, with a filling fraction of about 50%. I have demonstrated a single-atom detection fidelity of 99,986(1)% and a survival probability of 97(2)% between subsequent image acquisition, comparable to other current state-of-the-art experiments. To characterize the platform, I carried out release-and-recapture experiments, from which it is possible to measure a temperature for the individually trapped atoms of 12.95(5)μK. These results demonstrate the successful implementation of a robust and high-fidelity platform for optical trapping and imaging of single strontium atoms. The apparatus provides the foundation for future quantum simulation experiments with alkalineearth atoms excited to the Rydberg state, o"ering precise control over individual particles and the ability to scale towards larger, programmable atomic arrays.
We demonstrate the lossless state-selective detection of a single rubidium 87 atom trapped in an optical tweezer. This detection is analogous to the one used on trapped ions. After preparation in either a dark or a bright state, we probe the atom internal state by sending laser light that couples an excited state to the bright state only. The laser-induced fluorescence is collected by a high numerical aperture lens. The single-shot fidelity of the detection is 98.6±0.2% and is presently limited by the dark count noise of the detector. The simplicity of this method opens new perspectives in view of applications to quantum manipulations of neutral atoms.
A barrier to realizing the potential of molecules for quantum information science applications is a lack of high-fidelity, single-molecule imaging techniques. Here, we present and theoretically analyze a general scheme for dispersive imaging of electronic ground-state molecules. Our technique relies on the intrinsic anisotropy of excited molecular rotational states to generate optical birefringence, which can be detected through polarization rotation of an off-resonant probe laser beam. Using 23Na87Rb and 87Rb133Cs as examples, we construct a formalism for choosing the molecular state to be imaged and the excited electronic states involved in off-resonant coupling. Our proposal establishes the relevant parameters for achieving degree-level polarization rotations for bulk molecular gases, thus enabling high-fidelity nondestructive imaging. We additionally outline requirements for the high-fidelity imaging of individually trapped molecules.
Ultracold polar molecules provide a powerful platform for quantum science because they combine long-lived rotational states, rich internal structure, and strong electric dipole-dipole interactions. Optical tweezer arrays provide a pristine way of controlling these molecules at single-particle level, in which molecules can be individually trapped, rearranged into programmable geometries, coherently manipulated by optical and microwave fields, and entangled through their native dipolar interactions. This dissertation describes the development of geometric control as a resource for improving interaction coherence and high fidelity of quantum entanglement between directly laser-cooled calcium monofluoride (CaF) molecules in optical tweezers. A central challenge in molecular tweezer systems is that dipolar interactions are intrinsically sensitive to the relative position of the molecules. Thermal motion in the traps, especially along the weakly confined axial direction, causes molecules to sample a distribution of intermolecular separations, degrading dipolar coherence and limiting entanglement fidelity. We show in this work that the interaction itself can be made robust by controlling its geometry. The experimental work begins with improvements to the production and optical trapping of dense CaF samples. We realize a blue-detuned ``conveyor-belt" magneto-optical trap (MOT) that compresses laser-cooled CaF to a mean cloud radius of 64(5)μm and a peak density of 3.6(5)×1010cm−3, a 600-fold density increase over conventional red-detuned CaF MOTs. Loading from this compressed source into an optical dipole trap yields up to 2.6×104 trapped molecules at 14(2)μK, with a peak phase-space density of approximately 2.4×10−6. This high-density source improves the transfer of laser-cooled molecules into conservative optical traps and provides the starting point for loading and manipulating single molecules in a hybrid SLM-AOD optical tweezer array. Using this platform, we prepare CaF molecules in selected rotational and hyperfine states to encode a rotational qubiyt. We show how to preserve the single-qubit coherence with a combination of techniques, including ``magic" polarization condition and microwave dynamical decoupling, as well as reduce motional quantum state of the trapped molecule with Raman sideband cooling. We then characterize coherent dipolar spin exchange between pairs of molecules and identify thermal motion and relative trap-center offsets as dominant sources of interaction dephasing. To suppress these effects, we engineer the three-dimensional interaction geometry between two individually trapped molecules. More specifically, we show that one can tune the \textit{static} geometric of the dipolar interaction to configurations where sensitivity to thermal fluctuations is strongly reduced while retaining a finite interaction strength. Furthermore, we show that a molecule can be moved during the interaction while preserving the coherence of ongoing entangling operations. We leverage programmable molecular motion to refocus dephasing arising from relative positional jitter of the optical tweezers. Combining static geometric insensitivity, programmable molecular motion, and partial Raman sideband cooling, we generate two-molecule entanglement with a Bell-state fidelity of F=0.976−0.011+0.008 in directly laser-cooled molecules. Crucially, the high-fidelity molecular entanglement here is performed without ground-state preparation. Rather than relying on stringent cooling or species-specific trapping conditions, as in prior work, the methods demonstrated here are instead based on dynamic and static geometric control of interacting molecules and are therefore broadly applicable across molecular platforms. These results extend moving optical tweezers beyond assembly and rearrangement, opening routes to robust two-qubit gates, many-body dynamics, and dynamically programmable networks of interaction.