High-Resolution Laser Spectroscopy of a Functionalized Aromatic Molecule.

We present a high-resolution laser spectroscopic study of the Ã2B2-X̃2A1 and B̃2B1-X̃2A1 transitions of calcium(I) phenoxide, CaOPh (CaOC6H5). The rotationally resolved band systems are analyzed using an effective Hamiltonian model and are accurately modeled as independent perpendicular (b- or c-type) transitions. The structure of calcium monophenoxide is compared to previously observed Ca-containing radicals, and implications for direct laser cooling are discussed. This work demonstrates that functionalization of aromatic molecules with optical cycling centers can preserve many of the properties needed for laser-based control.

Laser Spectroscopy of Aromatic Molecules with Optical Cycling Centers: Strontium(I) Phenoxides.

We report the production and spectroscopic characterization of strontium(I) phenoxide (SrOC6H5 or SrOPh) and variants featuring electron-withdrawing groups designed to suppress vibrational excitation during spontaneous emission from the electronically excited state. Optical cycling closure of these species, which is the decoupling of the vibrational state changes from spontaneous optical decay, is found by dispersed laser-induced fluorescence spectroscopy to be high, in accordance with theoretical predictions. A high-resolution, rotationally resolved laser excitation spectrum is recorded for SrOPh, allowing the estimation of spectroscopic constants and identification of candidate optical cycling transitions for future work. The results confirm the promise of strontium phenoxides for laser cooling and quantum state detection at the single-molecule level.

Functionalizing aromatic compounds with optical cycling centres.

Molecular design principles provide guidelines for augmenting a molecule with a smaller group of atoms to realize a desired property or function. We demonstrate that these concepts can be used to create an optical cycling centre, the Ca(I)-O unit, that can be attached to a number of aromatic ligands, enabling the scattering of many photons from the resulting molecules without changing the molecular vibrational state. Such capability plays a central role in quantum state preparation and measurement, as well as laser cooling and trapping, and is therefore a prerequisite for many quantum science and technology applications. We provide further molecular design principles that indicate the ability to optimize and expand this work to an even broader class of molecules. This represents a great step towards a quantum functional group, which may serve as a generic qubit moiety that can be attached to a wide range of molecular structures and surfaces.

Pathway toward Optical Cycling and Laser Cooling of Functionalized Arenes.

Rapid and repeated photon cycling has enabled precision metrology and the development of quantum information systems using atoms and simple molecules. Extending optical cycling to structurally complex molecules would provide new capabilities in these areas, as well as in ultracold chemistry. Increased molecular complexity, however, makes realizing closed optical transitions more difficult. Building on already established strong optical cycling of diatomic, linear triatomic, and symmetric top molecules, recent work has pointed the way to cycling of larger molecules, including phenoxides. The paradigm for these systems is an optical cycling center bonded to a molecular ligand. Theory has suggested that cycling may be extended to even larger ligands, like naphthalene, pyrene, and coronene. Herein, we study optical excitation and fluorescent vibrational branching of CaO-[Formula: see text], SrO-[Formula: see text], and CaO-[Formula: see text] and find only weak decay to excited vibrational states, indicating a promising path to full quantum control and laser cooling of large arene-based molecules.

Accurate prediction and measurement of vibronic branching ratios for laser cooling linear polyatomic molecules.

We report a generally applicable computational and experimental approach to determine vibronic branching ratios in linear polyatomic molecules to the 10-5 level, including for nominally symmetry-forbidden transitions. These methods are demonstrated in CaOH and YbOH, showing approximately two orders of magnitude improved sensitivity compared with the previous state of the art. Knowledge of branching ratios at this level is needed for the successful deep laser cooling of a broad range of molecular species.

Franck-Condon Tuning of Optical Cycling Centers by Organic Functionalization.

Laser induced electronic excitations that spontaneously emit photons and decay directly to the initial ground state ("optical cycling transitions") are used in quantum information and precision measurement for state initialization and readout. To extend this primarily atomic technique to large, organic compounds, we theoretically investigate optical cycling of alkaline earth phenoxides and their functionalized derivatives. We find that optical cycle leakage due to wave function mismatch is low in these species, and can be further suppressed by using chemical substitution to boost the electron-withdrawing strength of the aromatic molecular ligand through resonance and induction effects. This provides a straightforward way to use chemical functional groups to construct optical cycling moieties for laser cooling, state preparation, and quantum measurement.

Zeeman-Sisyphus Deceleration of Molecular Beams.

We present a robust, continuous molecular decelerator that employs high magnetic fields and few optical pumping steps. CaOH molecules are slowed, accumulating at low velocities in a range sufficient for loading both magnetic and magneto-optical traps. During the slowing, the molecules scatter only seven photons, removing around 8 K of energy. Because large energies can be removed with only a few spontaneous radiative decays, this method can in principle be applied to nearly any paramagnetic atomic or molecular species, opening a general path to trapping of complex molecules.

Direct laser cooling of a symmetric top molecule.

Ultracold polyatomic molecules have potentially wide-ranging applications in quantum simulation and computation, particle physics, and quantum chemistry. For atoms and small molecules, direct laser cooling has proven to be a powerful tool for quantum science in the ultracold regime. However, the feasibility of laser-cooling larger, nonlinear polyatomic molecules has remained unknown because of their complex structure. We laser-cooled the symmetric top molecule calcium monomethoxide (CaOCH3), reducing the temperature of ~104 molecules from 22 ± 1 millikelvin to 1.8 ± 0.7 millikelvin in one dimension and state-selectively cooling two nuclear spin isomers. These results demonstrate that the use of proper ro-vibronic transitions enables laser cooling of nonlinear molecules, thereby opening a path to efficient cooling of chiral molecules and, eventually, optical tweezer arrays of complex polyatomic species.

Assessment and mitigation of aerosol airborne SARS-CoV-2 transmission in laboratory and office environments.

Bioaerosols are known to be an important transmission pathway for SARS-CoV-2. We report a framework for estimating the risk of transmitting SARS-CoV-2 via aerosols in laboratory and office settings, based on an exponential dose-response model and analysis of air flow and purification in typical heating, ventilation, and air conditioning (HVAC) systems. High-circulation HVAC systems with high-efficiency particulate air (HEPA) filtration dramatically reduce exposure to the virus in indoor settings, and surgical masks or N95 respirators further reduce exposure. As an example of our risk assessment model, we consider the precautions needed for a typical experimental physical science group to maintain a low risk of transmission over six months of operation. We recommend that, for environments where fewer than five individuals significantly overlap, work spaces should remain vacant for between one (high-circulation HVAC with HEPA filtration) to six (low-circulation HVAC with no filtration) air exchange times before a new worker enters in order to maintain no more than 1% chance of infection over six months of operation in the workplace. Our model is readily applied to similar settings that are not explicitly given here. We also provide a framework for evaluating infection mitigation through ventilation in multiple occupancy spaces.

1D Magneto-Optical Trap of Polyatomic Molecules.

We demonstrate a 1D magneto-optical trap of the polar free radical calcium monohydroxide (CaOH). A quasiclosed cycling transition is established to scatter ∼10^{3} photons per molecule, predominantly limited by interaction time. This enables radiative laser cooling of CaOH while compressing the molecular beam, leading to a significant increase in on axis beam brightness and reduction in temperature from 8.4 to 1.4 mK.

Branching Ratios, Radiative Lifetimes, and Transition Dipole Moments for YbOH.

Medium resolution (Δν̃ ∼ 3 GHz) laser-induced fluorescence (LIF) excitation spectra of a rotationally cold sample of YbOH in the 17300-17950 cm-1 range have been recorded using two-dimensional (excitation and dispersed fluorescence) spectroscopy. High resolution (Δλ ∼ 0.65 nm) dispersed laser-induced fluorescence (DLIF) spectra and radiative decay curves of numerous bands detected in the medium resolution LIF excitation spectra were recorded. The vibronic energy levels of the X̃2Σ+ state were predicted using a discrete variable representation approach and compared with observations. The radiative decay curves were analyzed to produce fluorescence lifetimes. DLIF spectra resulting from high resolution (Δν̃ < 10 MHz) LIF excitation of individual low-rotational lines in the Ã2Π1/2(0,0,0)-X̃2Σ+(0,0,0), Ã2Π1/2(1,0,0)-X̃2Σ+(0,0,0), and [17.73]Ω = 0.5(0,0,0)-X̃2Σ+(0,0,0) bands were also recorded. The DLIF spectra were analyzed to determine branching ratios which were combined with radiative lifetimes to obtain transition dipole moments. The implications for laser cooling and trapping of YbOH are discussed.

3D Magneto-Optical Trap of Yttrium Monoxide.

We report three-dimensional trapping of an oxide molecule (YO), using a radio-frequency magneto-optical trap (MOT). The total number of molecules trapped is ∼1.5×10^{4}, with a temperature of 4.1(5) mK. This diversifies the frontier of molecules that are laser coolable and paves the way for the second-stage narrow-line cooling in this molecule to the microkelvin regime. Futhermore, the new challenges of creating a 3D MOT of YO resolved here indicate that MOTs of more complex nonlinear molecules should be feasible as well.

Λ-Enhanced Imaging of Molecules in an Optical Trap.

We report on nondestructive imaging of optically trapped calcium monofluoride molecules using in situ Λ-enhanced gray molasses cooling. 200 times more fluorescence is obtained compared to destructive on-resonance imaging, and the trapped molecules remain at a temperature of 20 µK. The achieved number of scattered photons makes possible nondestructive single-shot detection of single molecules with high fidelity.

Radio Frequency Magneto-Optical Trapping of CaF with High Density.

We demonstrate significantly improved magneto-optical trapping of molecules using a very slow cryogenic beam source and either rf modulated or dc magnetic fields. The rf magneto-optical trap (MOT) confines 1.0(3)×10^{5} CaF molecules at a density of 7(3)×10^{6} cm^{-3}, which is an order of magnitude greater than previous molecular MOTs. Near Doppler-limited temperatures of 340(20) µK are attained. The achieved density enables future work to directly load optical tweezers and create optical arrays for quantum simulation.

Sisyphus Laser Cooling of a Polyatomic Molecule.

We perform magnetically assisted Sisyphus laser cooling of the triatomic free radical strontium monohydroxide (SrOH). This is achieved with principal optical cycling in the rotationally closed P(N^{''}=1) branch of either the X[over ˜]^{2}Σ^{+}(000)↔A[over ˜]^{2}Π_{1/2}(000) or the X[over ˜]^{2}Σ^{+}(000)↔B[over ˜]^{2}Σ^{+}(000) vibronic transitions. Molecules lost into the excited vibrational states during the cooling process are repumped back through the B[over ˜](000) state for both the (100) level of the Sr-O stretching mode and the (02^{0}0) level of the bending mode. The transverse temperature of a SrOH molecular beam is reduced in one dimension by 2 orders of magnitude to ∼750 µK. This approach opens a path towards creating a variety of ultracold polyatomic molecules by means of direct laser cooling.