arXiv subjects

John M. Doyle

Publications and source records attributed to John M. Doyle.

At least 19 recordsLinked to original sources

arXiv2026

Order of Magnitude Improved Optical Trapping of Molecules Through Transverse Cooling

We demonstrate a two-dimensional Sisyphus laser cooling method that increases the number of strontium monohydroxide (SrOH) molecules loaded into a magneto-optical trap by a factor of 12. Subsequent loading into an optical dipole trap (ODT) achieves $2.2 (3)\times10^4$ ultracold SrOH molecules with a peak density of $\sim2(1)\times10^{10}~\mathrm{cm^{-3}}$. The lifetime of molecules in the ODT is limited by two-body collisions characterized by a measured collision rate constant $β\sim 4\times10^{-10}~\mathrm{cm^3/s}$. The cooling method developed here is generally applicable to all known cases of direct molecular laser cooling, including symmetric and asymmetric top molecules. Increases in trapped molecule number will directly improve the search for ultralight dark matter, position polyatomic molecules as a platform for probing CP-violating new particles with masses $\gg$10 TeV, and facilitate a broad range of further research in quantum science.

physics.atom-ph↗

arXiv2026

High-fidelity entanglement of polar molecules by dynamic geometric control

In quantum information systems made of optical tweezer arrays of ultracold molecules, thermal motion of molecules degrades the coherence of their interactions, which limits entanglement fidelity and the concomitant scientific applicability of these systems. We show that by controlling the geometry of the dipolar interaction, even when a molecule occupies many motional states in the tweezer, coherence can be preserved. We characterize several geometries that suppress sensitivity to thermal fluctuations. We further use programmable, coherence-preserving motion of the molecules during entanglement to refocus dephasing from relative positional jitter of the tweezers, which is relevant even on the 10 nm scale. These methods yield substantially improved dipolar coherence and enable generation of two-molecule entanglement with a Bell state fidelity of $\mathcal{F}= 0.976^{+0.008}_{-0.011}$ in directly laser-cooled molecules.

physics.atom-ph↗

arXiv2026

Design and Performance of a Heated Gas Injector for Producing Cold Molecular Beams

We realize an injector device that supplies warm gas directly into a cryogenic environment. This injector has several advantageous features, including robustness, rigidity, simple installation, and excellent thermal isolation between a hot ($\sim$300 K) copper fill line and a cold ($<$3 K) cryogenic buffer gas cell. Less than 200 mW heat load on the cell is observed in realistic conditions of a molecular precision measurement experiment. A polyamide-imide (PAI) tube is the essential design feature. The fill line is epoxied to one end of the tube while the other end of the tube is connected to the cell via a slip-fit onto a brass nipple, realizing a complete vacuum-tight seal. PAI contracts on the brass nipple when cooled, forming a cryogenic leak-tight seal. The injector is easily (de-)mountable and rigid, with no significant displacement of the fill line relative to the cell observed during cooldown to 4 K. We characterize injector performance by flowing into the cell $\text{SF}_6$ through the hot fill line and cold $\text{He}$ buffer gas through a separate cryogenic fill line while laser ablating a barium-containing target. This produces cold BaF free radicals, detected using absorption spectroscopy. This injector design will be employed to laser cool radium-containing molecules, such as $\text{RaF}$ and $\text{RaOH}$, where leak-tight delivery of $\text{SF}_6$ and $\text{H}_2\text{O}$ reagents into a cryogenic buffer gas cell is required for scientific and safety reasons. These molecules are of particular interest for the study of symmetry-violating nuclear properties and searches for physics beyond the Standard Model.

physics.atom-ph↗

arXiv2026

Photon Cycling and Laser Cooling of an Asymmetric Top Molecule

We realize two-dimensional magnetically-assisted Sisyphus laser cooling of an asymmetric top molecule (ATM), calcium monoamide (CaNH$_2$). Vibrational state closure is achieved with $41.1 \pm 6.3$ photons scatters using optical pumping of the $X[3_1]$ state. Photon-cycling measurements show good agreement with branching ratios determined by dispersed fluorescence spectroscopy. Rotational closure is maintained by driving the $X[1_{11}] \to A [0_{00}]$ transition. The observed absence of additional state leakage channels broadens the scope of molecular laser cooling to include ATMs, which are the most general geometric class of molecules and possess the richest internal structure. Future applications of quantum controlled ATMs include new quantum information platforms and searches for physics beyond the Standard Model.

physics.atom-ph↗

arXiv2026

Parity-Doublet Coherence Times in Optically Trapped Polyatomic Molecules

Polyatomic molecules provide complex internal structures that are ideal for applications in quantum information science, quantum simulation, and precision searches for physics beyond the Standard Model. A key feature of polyatomic molecules is the presence of parity-doublet states. These structures, which generically arise from the rotational and vibrational degrees of freedom afforded by polyatomic molecules, are a powerful feature to pursue these diverse quantum science applications. Linear triatomic molecules contain $\ell$-type parity doublet states, which are predicted to exhibit robust coherence properties. We optically trap CaOH molecules, prepare them in $\ell$-type parity-doublet states, and realize a bare qubit coherence time of $T_2^* = 0.8(2)$ s. We suppress differential Stark shifts by employing molecular spectroscopy to cancel ambient electric fields, and characterize parity-dependent trap shifts, which are found to limit the coherence time. The parity-doublet coherence times achieved in this work are a defining milestone for the use of polyatomic molecules in quantum science.

physics.atom-ph↗

arXiv2026

A cryogenic buffer gas beam source with in-situ ablation target replacement

The design and performance of a cryogenic buffer gas beam (CBGB) source with a load-lock system is presented. The ACME III electron electric dipole moment (eEDM) search experiment uses this source to produce a beam of cold, slow thorium monoxide (ThO) molecules. A key feature of the apparatus is its capability to replace ablation targets without interrupting vacuum or cryogenic conditions, increasing the average signal in the eEDM search. The source produces approximately $1.3 \times 10^{11}$ ground-state ThO molecules per pulse, with a rotational temperature of $4.8$ K, molecular beam solid angle of $0.31$ sr, and forward velocity of $200$ m/s. These parameters match the performance of traditional sources that require time-consuming thermal cycles for target replacement. A long-term yield improvement of about 40% is achieved when the load-lock system is used to replace targets biweekly.

physics.atom-ph↗

arXiv2025

Hyperfine-Resolved Spectroscopy of Dysprosium Monoxide (DyO) for Precision Measurements of the Nuclear Schiff Moment

We perform laser spectroscopy of dysprosium monoxide (DyO) to determine the hyperfine structure of the ground X8 and excited [17.1]7 states in the $^{161}$Dy and $^{163}$Dy isotopologues. These dysprosium nuclei have non-zero nuclear spin and dynamical octupole deformation, which gives them high sensitivity to time-reversal-violating new physics via the nuclear Schiff moment (NSM). The DyO molecule was recently identified as being amenable to optical cycling -- the basis for many laser cooling and quantum control techniques -- which makes it a practical candidate for NSM searches. The measurements reported here are prerequisites to implementing optical cycling, designing precision measurement protocols, and benchmarking calculations of molecular sensitivity to symmetry-violating effects. The measured hyperfine parameters are interpreted using simple molecular orbital diagrams and show excellent agreement with relativistic quantum chemical calculations.

physics.atom-ph↗

arXiv2025

High-sensitivity molecular spectroscopy of SrOH using magneto-optical trapping

Polyatomic molecules are projected to be powerful tools in searches for physics beyond the Standard Model (BSM), including new CP-violating (CPV) interactions and ultralight dark matter (UDM) particles. Certain degrees of freedom present in polyatomic molecules enhance the sensitivity of these searches, as well as reject systematic errors, but necessitate extensive high-precision spectroscopy to identify pathways for optical cycling and quantum state readout. Here we show how a magneto-optical trap (MOT) can be used to locate weak optical transitions and identify rovibronic states for optical cycling and quantum control. We demonstrate this spectroscopic approach with strontium monohydroxide (SrOH), which is a candidate for both CPV and UDM searches. We identify two new repumping transitions in SrOH and implement them in a deeper optical cycle to achieve 32400(4700) trapped molecules, a 4.5-fold increase over the previous, shallower cycle. In addition, we determine the energy spacing between the $X^{2}Σ^{+}(200)$ and $X^{2}Σ^{+}(03^10)$ vibrational manifolds of SrOH, confirming the existence of numerous low-frequency rovibrational transitions that are sensitive to temporal variations of the proton-to-electron mass ratio, a predicted effect of the existence of UDM.

physics.atom-ph↗

arXiv2025

Optical Trapping of SrOH Molecules for Dark Matter and T-violation Searches

We report an optical dipole trap of strontium monohydroxide (SrOH) with 1400(300) trapped molecules. Through optical pumping, we access vibrational states that are proposed for improved probes of the electron's electric dipole moment (eEDM) and ultralight dark matter (UDM). For each of these states, the lifetime of trapped molecules is measured, and found to be consistent with spontaneous radiative decay and black-body excitation limits, making this platform viable for these eEDM and UDM searches.

physics.atom-ph↗

arXiv2025

Control of Dipolar Dynamics by Geometrical Programming

We propose and theoretically analyze methods for quantum many-body control through geometric reshaping of molecular tweezer arrays. Dynamic rearrangement during entanglement is readily available due to the extended coherence times of molecular rotational qubits. We show how motional dephasing can be suppressed and enhanced spin squeezing can be achieved in an actively rearranged short-range XY model. We also analyze in detail a specific static geometry that significantly suppresses decoherence. These general methods as applied to programmable quantum systems offer robust control modalities that are well suited to molecules.

quant-ph↗

arXiv2025

Quantum-State-Controlled Collisions of Ultracold Polyatomic Molecules

Collisions between ultracold calcium monohydroxide (CaOH) molecules are realized and studied. Inelastic collision rate constants are measured for CaOH prepared in ground and excited vibrational states, and the electric field dependence of these rates is measured for molecules in single quantum states of the parity-doubled bending mode. Theoretical calculations of collision rate coefficients are performed and found to agree with measured values. The lowest collisional loss rates are for states with repulsive long-range potentials that shield ultracold molecules from loss channels at short distance. These results unveil the collisional behavior of parity doublet molecules in the ultracold regime, and lay the foundation for future experiments to evaporatively cool polyatomic molecules to quantum degeneracy.

physics.atom-ph↗

arXiv2024

Conveyor-belt magneto-optical trapping of molecules

Laser cooling is used to produce ultracold atoms and molecules for quantum science and precision measurement applications. Molecules are more challenging to cool than atoms due to their vibrational and rotational internal degrees of freedom. Molecular rotations lead to the use of type-II transitions ($F \geq F'$) for magneto-optical trapping (MOT). When typical red detuned light frequencies are applied to these transitions, sub-Doppler heating is induced, resulting in higher temperatures and larger molecular cloud sizes than realized with the type-I MOTs most often used with atoms. To improve type-II MOTs, Jarvis et al. PRL 120, 083201 (2018) proposed a blue-detuned MOT to be applied after initial cooling and capture with a red-detuned MOT. This was successfully implemented (Burau et al. PRL 130, 193401 (2023), Jorapur et al. PRL 132, 163403 (2024), Li et al. PRL 132, 233402 (2024)), realizing colder and denser molecular samples. Very recently, Hallas et al. arXiv:2404.03636 (2024) demonstrated a blue-detuned MOT with a "1+2" configuration that resulted in even stronger compression of the molecular cloud. Here, we describe and characterize theoretically the conveyor-belt mechanism that underlies this observed enhanced compression. We perform numerical simulations of the conveyor-belt mechanism using both stochastic Schrödinger equation (SSE) and optical Bloch equation (OBE) approaches. We investigate the conveyor-belt MOT characteristics in relation to laser parameters, g-factors, and the structure of the molecular system.

physics.atom-ph↗

arXiv2024

A conveyor-belt magneto-optical trap of CaF

We report the experimental realization of a conveyor-belt magneto-optical trap for calcium monofluoride (CaF) molecules. The obtained highly-compressed cloud has a mean radius of 64(5) $μ$m and a peak number density of $3.6(5) \times 10^{10}$ cm$^{-3}$, a 600-fold increase over the conventional red-detuned MOTs of CaF, and the densest molecular MOT observed to date. Subsequent loading of these molecules into an optical dipole trap yields up to $2.6 \times 10^4$ trapped molecules at a temperature of 14(2) $μ$K with a peak phase-space density of $\sim 2.4 \times 10^{-6}$. This opens new possibilities for a range of applications utilizing high-density, optically trapped ultracold molecules.

physics.atom-ph↗

arXiv2024

Magneto-optical trapping of a heavy polyatomic molecule for precision measurement

We report a magneto-optical trap of strontium monohydroxide (SrOH) containing 2000(600) molecules at a temperature of 1.2(3) mK. The lifetime is 91(9) ms, which is limited by decay to optically unaddressed vibrational states. This provides the foundation for future sub-Doppler cooling and optical trapping of SrOH, a polyatomic molecule suited for precision searches for physics beyond the Standard Model including new CP violating particles and ultralight dark matter. We also identify important features in this system that guide cooling and trapping of complex and heavy polyatomic molecules into the ultracold regime.

physics.atom-ph↗

arXiv2024

Thermal Emission of Strontium in a Cryogenic Buffer Gas Beam Source

We demonstrate production of cold atomic strontium (Sr) and strontium-containing molecules (SrOH) in a cryogenic buffer gas beam source via direct heating of strontium oxide (SrO) with 30 mJ laser pulses several milliseconds long. $3.7(2)\times10^{14}$ Sr atoms are released, which represents a factor of 7 increase in atomic production per pulse compared to nanosecond-scale ablation laser pulses. A peak atomic density of $1.93(6) \times 10^{12}$ atoms/cm$^3$ is achieved, which corresponds to a factor of 2 increase relative to ablation. We further propose extensions of this method to other atomic and molecular species.

physics.atom-ph↗

arXiv2024

Relativistic Exact Two-Component Coupled-Cluster Study of Molecular Sensitivity Factors for Nuclear Schiff Moments

Relativistic exact two-component coupled-cluster calculations of molecular sensitivity factors for nuclear Schiff moments (NSMs) are reported. We focus on molecules containing heavy nuclei, especially octupole-deformed nuclei. Analytic relativistic coupled-cluster gradient techniques are used and serve as useful tools for identifying candidate molecules that sensitively probe for physics beyond the Standard Model in the hadronic sector. Notably, these tools enable straightforward ``black-box'' calculations. Two competing chemical mechanisms that contribute to the NSM are analyzed, illuminating the physics of ligand effects on NSM sensitivity factors.

physics.atom-ph↗

arXiv2024

Vibrational Branching Ratios for Laser-Cooling of Nonlinear Strontium-Containing Molecules

The vibrational branching ratios from the lowest excited electronic state for $\textrm{SrOCH}_3$, $\textrm{SrNH}_2$, and $\textrm{SrSH}$ are measured at the $< 0.1\%$ level. Spectra are obtained by driving the $\tilde{X} - \tilde{A}$ transitions and dispersing the fluorescence on a grating spectrometer. We also perform $\textit{ab initio}$ calculations for the energies of vibrational levels relevant for laser cooling, as well as branching ratios to support the interpretations of all molecular spectra. Symmetry group analysis is applied in conjunction with our data to study rotational closure in these molecules. These analyses indicate favorable prospects for laser cooling $\textrm{SrNH}_2$ and other similar alkaline-earth(-like) amides for future beyond the Standard Model physics searches using polyatomic molecules with long-lived parity doublets.

physics.atom-ph↗

arXiv2024

High Compression Blue-Detuned Magneto-Optical Trap of Polyatomic Molecules

We demonstrate a blue-detuned magneto-optical trap (MOT) of a polyatomic molecule, calcium monohydroxide (CaOH). We identify a novel MOT frequency configuration that produces high spatial compression of the molecular cloud. This high compression MOT achieves a cloud radius of $59(5)~μ\text{m}$ and a peak density of $8(2) \times 10^8~\text{cm}^{-3}$, the highest reported density for a molecular MOT to date. We compare our experimental studies of blue-detuned MOTs for CaOH and compare with Monte-Carlo simulations, finding good agreement.

physics.atom-ph↗