arXiv subjects

John M. Doyle

Publications and source records attributed to John M. Doyle.

At least 55 records · Page 3Linked to original sources

arXiv2021

Magneto-Optical Trapping and Sub-Doppler Cooling of a Polyatomic Molecule

We report magneto-optical trapping (MOT) of a polyatomic molecule, calcium monohydroxide (CaOH). The MOT contains $2.0(5)\times 10^4$ CaOH molecules at a peak density of $3.0(8)\times10^{6}$ cm$^{-3}$. CaOH molecules are further sub-Doppler laser cooled in an optical molasses, to a temperature of 110(4) $μ$K. The temperatures and densities achieved here make CaOH a viable candidate for a wide variety of quantum science applications, including the creation of optical tweezer arrays of CaOH molecules. This work also suggests that laser cooling and magneto-optical trapping of many other polyatomic species will be both feasible and practical.

physics.atom-ph↗

arXiv2021

Establishing a nearly closed cycling transition in a polyatomic molecule

We study optical cycling in the polar free radical calcium monohydroxide (CaOH) and establish an experimental path towards scattering $\sim$$10^4$ photons. We report rovibronic branching ratio measurements with precision at the $\sim10^{-4}$ level and observe weak symmetry-forbidden decays to bending modes with non-zero vibrational angular momentum. Calculations are in excellent agreement with these measurements and predict additional decay pathways. Additionally, we perform high-resolution spectroscopy of the $\widetilde{\text{X}}\,^2Σ^+(12^00)$ and $\widetilde{\text{X}}\,^2Σ^+(12^20)$ hybrid vibrational states of CaOH. These advances establish a path towards radiative slowing, 3D magneto-optical trapping, and sub-Doppler cooling of CaOH.

physics.atom-ph↗

arXiv2021

Rotational Coherence Times of Polar Molecules in Optical Tweezers

Qubit coherence times are critical to the performance of any robust quantum computing platform. For quantum information processing using arrays of polar molecules, a key performance parameter is the molecular rotational coherence time. We report a 93(7) ms coherence time for rotational state qubits of laser cooled CaF molecules in optical tweezer traps, over an order of magnitude longer than previous systems. Inhomogeneous broadening due to the differential polarizability between the qubit states is suppressed by tuning the tweezer polarization and applied magnetic field to a "magic" angle. The coherence time is limited by the residual differential polarizability, implying improvement with further cooling. A single spin-echo pulse is able to extend the coherence time to nearly half a second. The measured coherence times demonstrate the potential of polar molecules as high fidelity qubits.

physics.atom-ph↗

arXiv2021

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.

physics.atom-ph↗

arXiv2021

Suppression of the optical crosstalk in a multi-channel silicon photomultiplier array

We propose and study a method of optical crosstalk suppression for silicon photomultipliers (SiPMs) using optical filters. We demonstrate that attaching absorptive visible bandpass filters to the SiPM can substantially reduce the optical crosstalk. Measurements suggest that the absorption of near infrared light is important to achieve this suppression. The proposed technique can be easily applied to suppress the optical crosstalk in SiPMs in cases where filtering near infrared light is compatible with the application.

physics.ins-det↗

arXiv2021

Observation of Microwave Shielding of Ultracold Molecules

Harnessing the potential wide-ranging quantum science applications of molecules will require control of their interactions. Here, we use microwave radiation to directly engineer and tune the interaction potentials between ultracold calcium monofluoride (CaF) molecules. By merging two optical tweezers, each containing a single molecule, we probe collisions in three dimensions. The correct combination of microwave frequency and power creates an effective repulsive shield, which suppresses the inelastic loss rate by a factor of six, in agreement with theoretical calculations. The demonstrated microwave shielding shows a general route to the creation of long-lived, dense samples of ultracold molecules and evaporative cooling.

physics.atom-ph↗

arXiv2021

Enhanced Sensitivity to Ultralight Bosonic Dark Matter in the Spectra of the Linear Radical SrOH

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 $μ\equiv m_{p}/m_{e}\approx1836$. 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 $\partial_{t}μ$, 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 ($\left|Q_μ\right|\approx10^{3}$), 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 $δμ/μ$ 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.

physics.atom-ph↗

arXiv2020

Observation and laser spectroscopy of ytterbium monomethoxide, YbOCH$_3$

We describe a laser spectroscopic study of ytterbium monomethoxide, YbOCH$_3$, a species of interest to searches for time-reversal symmetry violation using laser-cooled molecules. We report measurements of vibrational structure in the $\tilde{X}$ and $\tilde{A}$ states, vibrational branching ratios for several components of the $\tilde{A}$ state, and radiative lifetimes of low-lying electronic states. $\textit{Ab initio}$ calculations are used to aid the assignment of vibronic emission bands and provide insight into the electronic and vibrational structure. Our results demonstrate that rapid optical cycling is feasible for YbOCH$_3$, opening a path to orders-of-magnitude increased sensitivity in future measurements of P- and/or T-violating physics.

physics.atom-ph↗

arXiv2020

Direct Laser Cooling of a Symmetric Top Molecule

We report direct laser cooling of a symmetric top molecule, reducing the transverse temperature of a beam of calcium monomethoxide (CaOCH$_3$) to $1.8\pm0.7$ mK while addressing two distinct nuclear spin isomers. These results open a path to efficient production of ultracold chiral molecules and conclusively demonstrate that by using proper rovibronic optical transitions, both photon cycling and laser cooling of complex molecules can be as efficient as for much simpler linear species.

physics.atom-ph↗

arXiv2020

Observation of Collisions between Two Ultracold Ground-State CaF Molecules

We measure inelastic collisions between ultracold CaF molecules by combining two optical tweezers, each containing a single molecule. We observe collisions between $^2Σ$ CaF molecules in the absolute ground state $|X,v=0, N=0,F=0\rangle$, and in excited hyperfine and rotational states. In the absolute ground state, we find a two-body loss rate of $7(4) \times 10^{-11} \text{cm}^{3}/\text{s}$, which is below, but close to the predicted universal loss rate.

physics.atom-ph↗

arXiv2020

Molecular Asymmetry and Optical Cycling: Laser Cooling Asymmetric Top Molecules

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.

physics.atom-ph↗

arXiv2020

1D Magneto-Optical Trap of Polyatomic Molecules

We demonstrate a 1D magneto-optical trap of the polar free radical calcium monohydroxide (CaOH). A quasi-closed cycling transition is established to scatter $\sim 10^3$ 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 mK to 1.4 mK.

physics.atom-ph↗

arXiv2019

The metastable Q $^3Δ_2$ state of ThO: A new resource for the ACME electron EDM search

The best upper limit for the electron electric dipole moment was recently set by the ACME collaboration. This experiment measures an electron spin-precession in a cold beam of ThO molecules in their metastable $H~(^3Δ_1)$ state. Improvement in the statistical and systematic uncertainties is possible with more efficient use of molecules from the source and better magnetometry in the experiment, respectively. Here, we report measurements of several relevant properties of the long-lived $Q~(^3Δ_2)$ state of ThO, and show that this state is a very useful resource for both these purposes. The $Q$ state lifetime is long enough that its decay during the time of flight in the ACME beam experiment is negligible. The large electric dipole moment measured for the $Q$ state, giving rise to a large linear Stark shift, is ideal for an electrostatic lens that increases the fraction of molecules detected downstream. The measured magnetic moment of the $Q$ state is also large enough to be used as a sensitive co-magnetometer in ACME. Finally, we show that the $Q$ state has a large transition dipole moment to the $C~(^1Π_1)$ state, which allows for efficient population transfer between the ground state $X~(^1Σ^+)$ and the $Q$ state via $X-C-Q$ Stimulated Raman Adiabatic Passage (STIRAP). We demonstrate $90\,$% STIRAP transfer efficiency. In the course of these measurements, we also determine the magnetic moment of $C$ state, the $X\rightarrow C$ transition dipole moment, and branching ratios of decays from the $C$ state.

physics.atom-ph↗

arXiv2019

Laser-Cooled Polyatomic Molecules for Improved Electron Electric Dipole Moment Searches

Doppler and Sisyphus cooling of $^{174}$YbOH are achieved and studied. This polyatomic molecule has high sensitivity to physics beyond the Standard Model and represents a new class of species for future high-precision probes of new T-violating physics. The transverse temperature of the YbOH beam is reduced by nearly two orders of magnitude to $< 600 \, μ$K and the phase-space density is increased by a factor of $>6$ via Sisyphus cooling. We develop a full numerical model of the laser cooling of YbOH and find excellent agreement with the data. We project that laser cooling and magneto-optical trapping of long-lived samples of YbOH molecules are within reach and these will allow a high sensitivity probe of the electric dipole moment (EDM) of the electron. The approach demonstrated here is easily generalized to other isotopologues of YbOH that have enhanced sensitivity to other symmetry-violating electromagnetic moments.

physics.atom-ph↗

arXiv2019

A Scalable Quantum Computing Platform Using Symmetric-Top Molecules

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.

physics.atom-ph↗

arXiv2019

An Optical Tweezer Array of Ultracold Molecules

Arrays of single ultracold molecules promise to be a powerful platform for many applications ranging from quantum simulation to precision measurement. Here we report on the creation of an optical tweezer array of single ultracold CaF molecules. By utilizing light-induced collisions during the laser cooling process, we trap single molecules. The high densities attained inside the tweezer traps have also enabled us to observe in the absence of light molecule-molecule collisions of laser cooled molecules for the first time.

physics.atom-ph↗

arXiv2018

Determination of CaOH and CaOCH$_3$ vibrational branching ratios for direct laser cooling and trapping

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.

physics.atom-ph↗

arXiv2018

3-D 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 loaded is $\sim$1.5$\times10^4$ , with a temperature of 7(1)~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 3-D MOT of YO resolved here indicate that MOTs of more complex non-linear molecules should be feasible as well.

physics.atom-ph↗