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Laser cooling of large, complex molecules is a long-standing goal, instrumental for enabling new quantum technology and precision measurements. A primary consideration for the feasibility of laser cooling, which determines the efficiency and technical requirements of the process, is the number of excited-state decay pathways leading to vibrational excitations. Therefore, the assessment of the laser-cooling potential of a molecule begins with estimate of the vibrational branching ratios of the first few electronic excited states theoretically to find the optimum cooling scheme. Such calculations, typically done within the Born-Oppenheimer and harmonic approximations, have suggested that one leading candidate for large, polyatomic molecule laser cooling, alkaline earth phenoxides, can most efficiently be laser cooled via the third electronically excited ( $\tilde{C}$) state. Here, we report the first detailed spectroscopic characterization of the $\tilde{C}$state in CaOPh and SrOPh. We find that nonadiabatic couplings between the $\tilde{A}, \tilde{B}$, and $\tilde{C}$states lead to substantial mixing, giving rise to vibronic states that enable additional decay pathways. Based on the intensity ratio of these extra decay channels, we estimate a nonadiabatic coupling strength of $\sim 0.1{\mathrm{cm}}^{-1}$. While this coupling strength is small, the large density of vibrational states available at photonic energy scales in a polyatomic molecule leads to significant mixing. Only the lowest excited state $\tilde{A}$is exempt from this coupling because it is highly separated from the ground state. Thus, this result is expected to be general for large molecules and implies that only the lowest electronic excited state should be considered when judging the suitability of a molecule for laser cooling. 

A near-minimal instance of optical cooling is experimentally presented, wherein the internal-state entropy of a single atom is reduced more than twofold by illuminating it with broadband, incoherent light. Since the rate of optical pumping by a thermal state increases monotonically with its temperature, the cooling power in this scenario increases with higher thermal occupation, an example of a phenomenon known as cooling by heating. In contrast to optical pumping using coherent, narrow-band laser light, here, we perform the same task with fiber-coupled, broadband sunlight, the brightest laboratory-accessible source of continuous blackbody radiation. 

Erasures, or errors with known locations, are a more favorable type of error for quantum error-correcting codes than Pauli errors. Converting physical noise into erasures can significantly improve the performance of quantum error correction. Here, we apply the idea of performing erasure conversion by encoding qubits into metastable atomic states, proposed by Wu, Kolkowitz, Puri, and Thompson [Nat. Comm. 13, 4657 (2022)], to trapped ions. We suggest an erasure-conversion scheme for metastable trapped-ion qubits and develop a detailed model of various types of errors. We then compare the logical performance of ground and metastable qubits on the surface code under various physical constraints and conclude that metastable qubits may outperform ground qubits when the achievable laser power is higher for metastable qubits. 

The energetic disorder induced by fluctuating liquid environments acts in opposition to the precise control required for coherence-based sensing. Overcoming fluctuations requires a protected quantum subspace that only weakly interacts with the local environment. We report a ytterbium complex that exhibited an ultranarrow absorption linewidth in solution at room temperature with a full width at half maximum of 0.625 milli–electron volts. Using spectral hole burning, we measured an even narrower linewidth of 410 pico–electron volts at 77 kelvin. Narrow linewidths allowed low-field magnetic circular dichroism at room temperature, used to sense Earth-scale magnetic fields. These results demonstrated that ligand protection in lanthanide complexes could substantially diminish electronic state fluctuations. We have termed this system an “atomlike molecular sensor” (ALMS) and proposed approaches to improve its performance.