arXiv subjects

Christian Hallas

Publications and source records attributed to Christian Hallas.

17 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

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↗

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

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↗

arXiv2023

An optical tweezer array of ultracold polyatomic molecules

Polyatomic molecules have rich structural features that make them uniquely suited to applications in quantum information science, quantum simulation, ultracold chemistry, and searches for physics beyond the Standard Model. However, a key challenge is fully controlling both the internal quantum state and the motional degrees of freedom of the molecules. Here, we demonstrate the creation of an optical tweezer array of individual polyatomic molecules, CaOH, with quantum control of their internal quantum state. The complex quantum structure of CaOH results in a non-trivial dependence of the molecules' behavior on the tweezer light wavelength. We control this interaction and directly and nondestructively image individual molecules in the tweezer array with >90% fidelity. The molecules are manipulated at the single internal quantum state level, thus demonstrating coherent state control in a tweezer array. The platform demonstrated here will enable a variety of experiments using individual polyatomic molecules with arbitrary spatial arrangement.

physics.atom-ph↗

arXiv2023

Blackbody thermalization and vibrational lifetimes of trapped polyatomic molecules

We study the internal state dynamics of optically trapped polyatomic molecules subject to room temperature blackbody radiation. Using rate equations that account for radiative decay and blackbody excitation between rovibrational levels of the electronic ground state, we model the microscopic behavior of the molecules' thermalization with their environment. As an application of the model, we describe in detail the procedure used to determine the blackbody and radiative lifetimes of low-lying vibrational states in ultracold CaOH molecules, the values of which were reported in previous work [Hallas et al., arXiv:2208.13762]. Ab initio calculations are performed and are found to agree with the measured values. Vibrational state lifetimes for several other laser-coolable molecules, including SrOH and YbOH, are also calculated.

physics.atom-ph↗

arXiv2023

Direct Laser Cooling of Polyatomic Molecules

Over the past decade, tremendous progress has been made to extend the tools of laser cooling and trapping to molecules. Those same tools have recently been applied to polyatomic molecules (molecules containing three or more atoms). In this review, we discuss the scientific drive to bring larger molecules to ultralow temperatures, the features of molecular structure that provide the most promising molecules for this pursuit, and some technical aspects of how lasers can be used to control the motion and quantum states of polyatomic molecules. We also present opportunities for and challenges to the use of polyatomic molecules for science and technology.

physics.atom-ph↗

arXiv2023

Quantum Control of Trapped Polyatomic Molecules for eEDM Searches

Ultracold polyatomic molecules are promising candidates for experiments in quantum science, quantum sensing, ultracold chemistry, and precision measurements of physics beyond the Standard Model. A key, yet unrealized, requirement of these experiments is the ability to achieve full quantum control over the complex internal structure of the molecules. Here, we establish coherent control of individual quantum states in a polyatomic molecule, calcium monohydroxide (CaOH), and use these techniques to demonstrate a method for searching for the electron electric dipole moment (eEDM). Optically trapped, ultracold CaOH molecules are prepared in a single quantum state, polarized in an electric field, and coherently transferred into an eEDM sensitive state where an electron spin precession measurement is performed. To extend the coherence time of the measurement, we utilize eEDM sensitive states with tunable, near-zero magnetic field sensitivity. The spin precession coherence time is limited by AC Stark shifts and uncontrolled magnetic fields. These results establish a path for eEDM searches with trapped polyatomic molecules, towards orders-of-magnitude improved experimental sensitivity to time-reversal-violating physics.

physics.atom-ph↗

arXiv2022

Optical Trapping of a Polyatomic Molecule in an $\ell$-Type Parity Doublet State

We report optical trapping of a polyatomic molecule, calcium monohydroxide (CaOH). CaOH molecules from a magneto-optical trap are sub-Doppler laser cooled to $20(3)~μ\text{K}$ in free space and loaded into an optical dipole trap. We attain an in-trap molecule number density of $3(1) \times 10^9~\text{cm}^{-3}$ at a temperature of $57(8)~μ$K. Trapped CaOH molecules are optically pumped into an excited vibrational bending mode, whose $\ell$-type parity doublet structure is a potential resource for a wide range of proposed quantum science applications with polyatomic molecules. We measure the spontaneous, radiative lifetime of this bending mode state to be $\sim$$0.7~\text{s}$.

physics.atom-ph↗

arXiv2022

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 7 photons, removing around 8 K of energy. Because large energies can be removed with only a few spontaneous radiative decays, this method can be applied to nearly any paramagnetic atomic or molecular species, opening a general path to trapping of complex molecules.

physics.atom-ph↗

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↗

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

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↗

arXiv2016

Direct Time-domain Observation of Conformational Relaxation in Gas-phase Cold Collisions

Cooling molecules in the gas phase is important for precision spectroscopy, cold molecule physics, and physical chemistry. Measurements of conformational relaxation cross sections shed important light on potential energy surfaces and energy flow within a molecule. However, gas-phase conformational cooling has not been previously observed directly. In this work, we directly observe conformational dynamics of 1,2-propanediol in cold (6K) collisions with atomic helium using microwave spectroscopy and buffer-gas cooling. Precise knowledge and control of the collisional environment in the buffer-gas allows us to measure the absolute collision cross-section for conformational relaxation. Several conformers of 1,2-propanediol are investigated and found to have relaxation cross-sections with He ranging from $σ=4.7(3.0)\times10^{-18}\:\mathrm{cm}^{2}$ to $σ>5\times10^{-16}\:\mathrm{cm}^{2}$. Our method is applicable to a broad class of molecules and could be used to provide information about the potential energy surfaces of previously uninvestigated molecules.

physics.chem-ph↗