Molecular Asymmetry and Optical Cycling: Laser Cooling Asymmetric Top Molecules

Abstract

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.

arXiv comment22 pages, 7 figures

References in corpus (77)

• Search for New Physics with Atoms and Molecules
• Quantum computation with trapped polar molecules
• Cold and Ultracold Molecules: Science, Technology, and Applications
• A toolbox for lattice spin models with polar molecules
• Order of Magnitude Smaller Limit on the Electric Dipole Moment of the Electron
• Laser cooling of a diatomic molecule
• Magneto-optical trapping of a diatomic molecule
• A precision measurement of the electron's electric dipole moment using trapped molecular ions
• The Buffer Gas Beam: An Intense, Cold, and Slow Source for Atoms and Molecules
• Molecules cooled below the Doppler limit
• Tunable Superfluidity and Quantum Magnetism with Ultracold Polar Molecules
• Schemes for robust quantum computation with polar molecules
• Precision Measurement of Time-Reversal Symmetry Violation with Laser-Cooled Polyatomic Molecules
• Sisyphus Laser Cooling of a Polyatomic Molecule
• Radio Frequency Magneto-Optical Trapping of CaF with High Density
• 3-D Magneto-Optical Trap of Yttrium Monoxide
• Cold polar molecules in 2D traps: Tailoring interactions with external fields for novel quantum phases
• Ultracold molecules for measuring the electron's electric dipole moment
• Direct observation of bimolecular reactions of ultracold KRb molecules
• Dipolar Exchange Quantum Logic Gate with Polar Molecules
• Radiative force from optical cycling on a diatomic molecule
• Magneto-Optical Trap for Polar Molecules
• Sub-millikelvin dipolar molecules in a radio-frequency magneto-optical trap
• Laser radiation pressure slowing of a molecular beam
• Magic state distillation in all prime dimensions using quantum Reed-Muller codes
• Optoelectrical cooling of polar molecules to sub-millikelvin temperatures
• Robust encoding of a qubit in a molecule
• Ultracold polar molecules as qudits
• Laser-Cooled Polyatomic Molecules for Improved Electron Electric Dipole Moment Searches
• Enantiomer-Specific State Transfer of Chiral Molecules
• Polyatomic candidates for cooling of molecules with lasers from simple theoretical concepts
• Ultracold molecules for quantum simulation: rotational coherences in CaF and RbCs
• $\Lambda$-Enhanced Imaging of Molecules in an Optical Trap
• Rotational state microwave mixing for laser cooling of complex diatomic molecules
• 1D Magneto-Optical Trap of Polyatomic Molecules
• Laser cooling of molecules
• A Scalable Quantum Computing Platform Using Symmetric-Top Molecules
• Perspective: Tipping the scales - search for drifting constants from molecular spectra
• Magneto-optical trapping forces for atoms and molecules with complex level structures
• Deep laser cooling and efficient magnetic compression of molecules
• Laser-coolable polyatomic molecules with heavy nuclei
• An intense, cold, velocity-controlled molecular beam by frequency-chirped laser slowing
• Characteristics of a magneto-optical trap of molecules
• Molecular assembly of ground state cooled single atoms
• On the Prospects for Laser Cooling of TlF
• Field-free Three-Dimensional Orientation of Asymmetric-Top Molecules
• Realizing unconventional quantum magnetism with symmetric top molecules
• Improved magneto-optical trapping of a diatomic molecule
• Dipolar quantum logic for freely-rotating trapped molecular ions
• Magnetic Trapping of Molecules via Optical Loading and Magnetic Slowing
• Towards low overhead magic state distillation
• Spectroscopic characterization of aluminum monofluoride with relevance to laser cooling and trapping
• Electric Dipole Moments in Natural Supersymmetry
• Enhanced Yield from a Cryogenic Buffer Gas Beam Source via Excited State Chemistry
• Ultracold hydrogen and deuterium production via Doppler-cooled Feshbach molecules
• Determination of CaOH and CaOCH${}_3$ vibrational branching ratios for direct laser cooling and trapping
• Simulating quantum magnets with symmetric top molecules
• Coherent Bichromatic Force Deflection of Molecules
• Microwave and submillimeter molecular transitions and their dependence on fundamental constants
• Prospects for laser cooling of polyatomic molecules with increasing complexity
• A new experiment to test parity symmetry in cold chiral molecules using vibrational spectroscopy
• Enhanced nuclear Schiff moment and time reversal violation in 229Th-containing molecules
• Hypermetallic Polar Molecules for Precision Measurements
• Enhanced sensitivity of the electron electric dipole moment from YbOH: The role of theory
• High-precision spectroscopy of ultracold molecules in an optical lattice
• Photodissociation of CS from Excited Rovibrational Levels
• Radiation Pressure Force from Optical Cycling on a Polyatomic Molecule
• Radiative Branching Ratios for Excited States of ${}^{174}$YbF: Application to Laser Cooling
• STIRAP preparation of a coherent superposition of ThO $H^3{\Delta }_1$ states for an improved electron EDM measurement
• A Method for Preparation and Readout of Polyatomic Molecules in Single Quantum States
• Deflection of a Molecular Beam Using the Bichromatic Stimulated Force
• Emulating optical cycling centers in polyatomic molecules
• Fluorescence branching ratios and magnetic tuning of the visible spectrum of SrOH
• Statistical sensitivity of phase measurements via laser-induced fluorescence with optical cycling detection
• Suppressed spontaneous emission for coherent momentum transfer
• Methyl mercaptan (CH3SH) as a probe for $\mu$ variation
• Prospects for high-resolution microwave spectroscopy of methanol in a Stark-deflected molecular beam

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• Robust encoding of a qubit in a molecule
• Polyatomic Molecules as Quantum Sensors for Fundamental Physics
• Laser cooled molecules
• Probing Fundamental Symmetries of Deformed Nuclei in Symmetric Top Molecules
• Quantum Control of Trapped Polyatomic Molecules for eEDM Searches
• Optical cycling, radiative deflection and laser cooling of barium monohydride (BaH)
• Quantum control of molecules for fundamental physics
• Accurate prediction and measurement of vibronic branching ratios for laser cooling linear polyatomic molecules
• Franck-Condon tuning of optical cycling centers by organic functionalization
• Establishing a nearly closed cycling transition in a polyatomic molecule
• Observation and laser spectroscopy of ytterbium monomethoxide, YbOCH${}_3$
• Optical Trapping of a Polyatomic Molecule in an $\ell$-Type Parity Doublet State
• Molecular Laser-Cooling in a Dynamically Tunable Repulsive Optical Trap
• Enantiomer superpositions from matter-wave interference of chiral molecules
• Towards improved loading, cooling, and trapping of molecules in magneto-optical traps
• Enantio-conversion of chiral mixtures via optical pumping
• Entanglement-Assisted Quantum Chiral Spectroscopy
• Observation of photoassociation resonances in ultracold atom-molecule collisions
• Large molasses-like cooling forces for molecules using polychromatic optical fields: A theoretical description
• Bichromatic Imaging of Single Molecules in an Optical Tweezer Array
• Quantum-Enhanced Metrology for Molecular Symmetry Violation using Decoherence-Free Subspaces
• Intensity-borrowing mechanisms pertinent to laser cooling of linear polyatomic molecules
• Blackbody thermalization and vibrational lifetimes of trapped polyatomic molecules
• Single-shot Non-destructive Quantum Sensing for Gaseous Samples with Hundreds of Chiral Molecules
• Four-body singlet potential energy surface for reactions of calcium monofluoride
• Precisely Spun Super Rotors
• Laser spectroscopy of aromatic molecules with optical cycling centers: strontium (I) phenoxides
• Enantio-detection via cavity-assisted three-photon processes
• Fully saturated hydrocarbons as hosts of optical cycling centers
• Vibrational Branching Ratios for Laser-Cooling of Nonlinear Strontium-Containing Molecules
• Quantum phases of bosonic chiral molecules in helicity lattices
• Slow molecular beams from a cryogenic buffer gas source
• Zeeman-Sisyphus Deceleration for Heavy Molecules with Perturbed Excited-State Structure
• Dynamics of translational and rotational thermalization of AlF molecules via collisions with cryogenic helium
• Cold CH radicals for laser cooling and trapping
• Rotational properties of two interacting cold polar molecules: linear, symmetric, and asymmetric tops
• Features of Molecular Structure Beneficial for Optical Pumping
• Vibronic coupling limits the use of high-lying electronic states in complex molecules for laser cooling
• Purcell modified Doppler cooling of quantum emitters inside optical cavities
• Strong parity-violation effects induced by large-amplitude motions: A quantum-dynamics study of substituted chiral methanols
• Non-resonant cavity for intensity buildup of multiple lasers
• Molecular Quantum Control Algorithm Design by Reinforcement Learning