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Recent theoretical investigations have indicated that rapid optical cycling should be feasible in complex polyatomic molecules with diverse constituents, geometries and symmetries. However, as a composite molecular mass grows, so does the required number of photon scattering events necessary to decelerate and confine molecular beams using laser light. Utilizing coherent momentum exchange between light fields and molecules can suppress spontaneous emission and significantly reduce experimental complexity for slowing and trapping. Working with BaH as a test species, we have identified a robust, experimentally viable configuration to achieve large molasses-like cooling forces for molecules using polychromatic optical fields addressing both $X-A$ and $X-B$ electronic transitions, simultaneously. Using numerical solutions of the time-dependent density matrix as well as Monte Carlo simulations, we demonstrate that creation of Suppressed Emission Rate (SupER) molasses with large capture velocities ($\sim 40$ m/s) is generically feasible for polyatomic molecules of increasing complexity that have an optical cycling center. Proposed SupER molasses are anticipated to not only extend quantum control to novel molecular species with abundant vibrational decay channels, but also significantly increase trapped densities for previously laser-cooled diatomic and triatomic species.

We present the first experimental demonstration of radiation pressure force deflection and direct laser cooling for barium monohydride (BaH) molecules resulting from multiple photon scattering. Despite a small recoil velocity (2.7 mm/s) and a long excited state lifetime (137 ns), we use 1060 nm laser light exciting the $X\rightarrow A$ electronic transition of BaH to deflect a cryogenic buffer-gas beam and reduce its transverse velocity spread. Multiple experimental methods are employed to characterize the optical cycling dynamics and benchmark theoretical estimates based on rate equation models as well as solutions of the Lindblad master equation for the complete multilevel system. Broader implications for laser cooling and magneto-optical trapping of heavy-metal-containing molecules with narrow transition linewidths are presented. Our results pave the way for producing a new class of ultracold molecules -- alkaline earth monohydrides -- via direct laser cooling and trapping, opening the door to realizing a new method for delivering ultracold hydrogen atoms (Lane 2015 \textit{Phys. Rev. A} 92, 022511).

We present a practical roadmap to achieve optical cycling and laser cooling of asymmetric top molecules (ATMs). Our theoretical analysis describes how reduced molecular symmetry, as compared to diatomic and symmetric non-linear molecules, plays a role in photon scattering. We present methods to circumvent limitations on rapid photon cycling in these systems. We calculate vibrational branching ratios for a diverse set of asymmetric top molecules and find that many species within a broad class of molecules can be effectively cooled with a manageable number of lasers. We also describe methods to achieve rotationally closed optical cycles in ATMs. Despite significant structural complexity, laser cooling can be made effective using extensions of the current techniques used for linear molecules. Potential scientific impacts of laser-cooled ATMs span frontiers in controlled chemistry, quantum simulation, and searches for physics beyond the Standard Model., Comment: 22 pages, 7 figures

We propose a new scalable platform for quantum computing (QC) -- an array of optically trapped symmetric-top molecules (STMs) of the alkaline earth monomethoxide (MOCH$_3$) family. Individual STMs form qubits, and the system is readily scalable to 100 to 1000 qubits.STM qubits have desirable features for quantum computing compared to atoms and diatomic molecules. The additional rotational degree of freedom about the symmetric top axis gives rise to closely-spaced opposite parity $K$-doublets that allow full alignment at low electric fields, and the hyperfine structure naturally provides magnetically insensitive states with switchable electric dipole moments. These features lead to much reduced requirements for electric field control, provide minimal sensitivity to environmental perturbations, and allow for 2-qubit interactions that can be switched on at will. We examine in detail the internal structure of STMs relevant to our proposed platform, taking into account the full effective molecular Hamiltonian including hyperfine interactions, and identify useable STM qubit states. We then examine the effects of the electric dipolar interaction in STMs, which not only guide the designing of high-fidelity gates, but also elucidate the nature of dipolar spin-exchange in STMs. Under realistic experimental parameters, we estimate that the proposed QC platform could yield gate errors at the $10^{-3}$ level, approaching that required for fault-tolerant quantum computing.

Alkaline earth monoalkoxide free radicals (MORs) have molecular properties conducive to direct laser cooling to sub-millikelvin temperatures. Using dispersed laser induced fluorescence (DLIF) measurements from a pulsed supersonic molecular beam source we determine vibrational branching ratios and Franck-Condon factors for the MORs CaOH and CaOCH$_{3}$. With narrow linewidth continuous-wave dye laser excitation, we precisely measure fluorescence branching for both $\tilde{X}-\tilde{A}$ and $\tilde{X}-\tilde{B}$ electronic systems in each molecule. Weak symmetry-forbidden decays to excited bending states with non-zero vibrational angular momentum are observed. Normal mode theoretical analysis combined with ab initio structural calculations are performed and compared to experimental results. Our measurements and analysis pave the way for direct laser cooling of these (and other) complex nonlinear polyatomic molecules. We also describe a possible approach to laser cooling and trapping of molecules with fewer symmetries like chiral species., Comment: to be submitted to New Journal of Physics

Coupling between Standard Model particles and theoretically well-motivated ultralight dark matter (UDM) candidates can lead to time variation of fundamental constants including the proton-to-electron mass ratio $\mu\equiv m_{p}/m_{e}\approx1836$. The presence of nearly-degenerate vibrational energy levels of different character in polyatomic molecules can result in significantly enhanced relative energy shifts in molecular spectra originating from $\partial_{t}\mu$, relaxing experimental complexity required for high-sensitivity measurements. We analyze the amplification of UDM effects in the spectrum of laser-cooled strontium monohydroxide (SrOH). SrOH is the first and, so far, the only polyatomic molecule to be directly laser cooled to sub-millikelvin temperatures, opening the possibility of long experimental coherence times. Because of the high enhancement factors ($\left|Q_{\mu}\right|\approx10^{3}$), measurements of the $\tilde{X}\left(200\right)\leftrightarrow\tilde{X}\left(03^{1}0\right)$ rovibrational transitions of SrOH in the microwave regime can result in $\sim10^{-17}$ fractional uncertainty in $\delta\mu/\mu$ with one day of integration. Furthermore, ultracold SrOH provides a promising platform for suppressing systematic errors. More complex SrOR radicals with additional vibrational modes arising from larger ligands R could lead to even greater enhancement factors., Comment: significantly revised version of the original submission

The magnetic tuning of the low rotational levels in the Xsigma+(0,0,0), Api(0,0,0), and Bsigma+ (0,0,0) electronic states of strontium hydroxide, SrOH, have been experimentally investigated using high resolution optical Zeeman spectroscopy of a cold molecular beam sample. The observed Zeeman shifts and splittings are successfully modeled using a traditional effective Hamiltonian approach to account for the interaction between the Api and Bsigma+ states. The determined magnetic g-factors for the Xsigma+, Api , and Bsigma+ states are compared to those predicted by perturbation theory. The dispersed fluorescence resulting from laser excitation of rotationally resolved branch features of the Bsigma+ (0,0,0)

We demonstrate the coherent optical bichromatic force on a molecule, the polar free radical strontium monohydroxide (SrOH). A dual-frequency retro-reflected laser beam addressing the $\tilde{X}^2\Sigma^+\leftrightarrow\tilde{A}^2\Pi_{1/2}$ electronic transition coherently imparts momentum onto a cryogenic beam of SrOH. This directional photon exchange creates a bichromatic force that transversely deflects the molecules. By adjusting the relative phase between the forward and counter propagating laser beams we reverse the direction of the applied force. A momentum transfer of $70\hbar k$ is achieved with minimal loss of molecules to dark states. Modeling of the bichromatic force is performed via direct numerical solution of the time-dependent density matrix and is compared with experimental observations. Our results open the door to further coherent manipulation of molecular motion, including the efficient optical deceleration of diatomic and polyatomic molecules with complex level structures.

Precision searches for time-reversal symmetry violating interactions in polar molecules are extremely sensitive probes of high energy physics beyond the Standard Model. To extend the reach of these probes into the PeV regime, long coherence times and large count rates are necessary. Recent advances in laser cooling of polar molecules offer one important tool -- optical trapping. However, the types of molecules that have been laser-cooled so far do not have the highly desirable combination of features for new physics searches, such as the ability to fully polarize and the existence of internal co-magnetometer states. We show that by utilizing the internal degrees of freedom present only in molecules with at least three atoms, these features can be attained simultaneously with molecules that have simple structure and are amenable to laser cooling and trapping.

We recently set a new limit on the electric dipole moment of the electron (eEDM) (J. Baron et al., ACME collaboration, Science 343 (2014), 269-272), which represented an order-of-magnitude improvement on the previous limit and placed more stringent constraints on many CP-violating extensions to the Standard Model. In this paper we discuss the measurement in detail. The experimental method and associated apparatus are described, together with the techniques used to isolate the eEDM signal. In particular, we detail the way experimental switches were used to suppress effects that can mimic the signal of interest. The methods used to search for systematic errors, and models explaining observed systematic errors, are also described. We briefly discuss possible improvements to the experiment., Comment: 81 pages, 37 figures, submitted to NJP

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 $P\left(N"=1\right)$ branch of either the $\tilde{X}^{2}\Sigma^{+}\left(000\right)\leftrightarrow\tilde{A}^{2}\Pi_{1/2}\left(000\right)$ or the $\tilde{X}^{2}\Sigma^{+}\left(000\right)\leftrightarrow\tilde{B}^{2}\Sigma^{+}\left(000\right)$ vibronic transitions. Molecules lost into the excited vibrational states during the cooling process are repumped back through the $\tilde{B}\left(000\right)$ state for both the $\left(100\right)$ level of the Sr-O stretching mode and the $\left(02^{0}0\right)$ level of the bending mode. The transverse temperature of a SrOH molecular beam is reduced in one dimension by two orders of magnitude to $\sim700\ {\rm \mu K}$. This approach opens a path towards creating a variety of ultracold polyatomic molecules, including much larger ones, by means of direct laser cooling.

We demonstrate multiple photon cycling and radiative force deflection on the triatomic free radical strontium monohydroxide (SrOH). Optical cycling is achieved on SrOH in a cryogenic buffer-gas beam by employing the rotationally closed $P\left(N''=1\right)$ branch of the vibronic transition $\tilde{X}^{2}\Sigma^{+}\left(000\right)\leftrightarrow\tilde{A}^{2}\Pi_{1/2}\left(000\right)$. A single repumping laser excites the Sr-O stretching vibrational mode, and photon cycling of the molecule deflects the SrOH beam by an angle of $0.2^{\circ}$ via scattering of $\sim100$ photons per molecule. This approach can be used for direct laser cooling of SrOH and more complex, isoelectronic species.

The Standard Model (SM) of particle physics fails to explain dark matter and why matter survived annihilation with antimatter following the Big Bang. Extensions to the SM, such as weak-scale Supersymmetry, may explain one or both of these phenomena by positing the existence of new particles and interactions that are asymmetric under time-reversal (T). These theories nearly always predict a small, yet potentially measurable ($10^{-27}$-$10^{-30}$ $e$ cm) electron electric dipole moment (EDM, $d_e$), which is an asymmetric charge distribution along the spin ($\vec{S}$). The EDM is also asymmetric under T. Using the polar molecule thorium monoxide (ThO), we measure $d_e = (-2.1 \pm 3.7_\mathrm{stat} \pm 2.5_\mathrm{syst})\times 10^{-29}$ $e$ cm. This corresponds to an upper limit of $|d_e| < 8.7\times 10^{-29}$ $e$ cm with 90 percent confidence, an order of magnitude improvement in sensitivity compared to the previous best limits. Our result constrains T-violating physics at the TeV energy scale.

Calcium monofluoride (CaF) is magnetically slowed and trapped using optical pumping. Starting from a collisionally cooled slow beam, CaF with an initial velocity of ~ 30 m/s is slowed via magnetic forces as it enters a 800 mK deep magnetic trap. Employing two-stage optical pumping, CaF is irreversibly loaded into the trap via two scattered photons. We observe a trap lifetime exceeding 500 ms, limited by background collisions. This method paves the way for cooling and magnetic trapping of chemically diverse molecules without closed cycling transitions.