Preparation and coherent manipulation of pure quantum states of a single molecular ion

Abstract

Laser cooling and trapping of atoms and atomic ions has led to numerous advances including the observation of exotic phases of matter, development of exquisite sensors and state-of-the-art atomic clocks. The same level of control in molecules could also lead to profound developments such as controlled chemical reactions and sensitive probes of fundamental theories, but the vibrational and rotational degrees of freedom in molecules pose a formidable challenge for controlling their quantum mechanical states. Here, we use quantum-logic spectroscopy (QLS) for preparation and nondestructive detection of quantum mechanical states in molecular ions. We develop a general technique to enable optical pumping and preparation of the molecule into a pure initial state. This allows for the observation of high-resolution spectra in a single ion (here CaH+) and coherent phenomena such as Rabi flopping and Ramsey fringes. The protocol requires a single, far-off resonant laser, which is not specific to the molecule, so that many other molecular ions, including polyatomic species, could be treated with the same methods in the same apparatus by changing the molecular source. Combined with long interrogation times afforded by ion traps, a broad range of molecular ions could be studied with unprecedented control and precision, representing a critical step towards proposed applications, such as precision molecular spectroscopy, stringent tests of fundamental physics, quantum computing, and precision control of molecular dynamics.

arXiv comment38 pages in preprint format, 9 figures, 3 tables; added references

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• Rotational spectrum of molecular ion NH^+ as a probe for alpha- and m_e/m_p-variation
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Cited by in corpus (102)

• Search for New Physics with Atoms and Molecules
• Trapped-Ion Quantum Computing: Progress and Challenges
• Quantum control of molecular rotation
• Highly charged ions: optical clocks and applications in fundamental physics
• 3-D Magneto-Optical Trap of Yttrium Monoxide
• Microscopic control and detection of ultracold strontium in optical-tweezer arrays
• High-fidelity laser-free universal control of two trapped ion qubits
• Robust encoding of a qubit in a molecule
• Coherent laser spectroscopy of highly charged ions using quantum logic
• Assembly of a rovibrational ground state molecule in an optical tweezer
• Observation of Collisions between Two Ultracold Ground-State CaF Molecules
• Quantum entanglement between an atom and a molecule
• Rotational Coherence Times of Polar Molecules in Optical Tweezers
• Molecular lattice clock with long vibrational coherence
• Quantum non-demolition state detection and spectroscopy of single trapped molecules
• Principles of enantio-selective excitation in three-wave mixing spectroscopy of chiral molecules
• Opportunities for Fundamental Physics Research with Radioactive Molecules
• Precision frequency-comb terahertz spectroscopy on pure quantum states of a single molecular ion
• Forming a single molecule by magnetoassociation in an optical tweezer
• Rotational spectroscopy of cold, trapped molecular ions in the Lamb-Dicke regime
• Dipolar quantum logic for freely-rotating trapped molecular ions
• Measuring the stability of fundamental constants with a network of clocks
• Quantum tomography of electrical currents
• Probing Fundamental Symmetries of Deformed Nuclei in Symmetric Top Molecules
• Detection of the $5p-4f$ orbital crossing and its optical clock transition in Pr${}^{9+}$
• Optical Traps for sympathetic Cooling of Ions with ultracold neutral Atoms
• Benchmarking a high-fidelity mixed-species entangling gate
• Quantum control of molecules for fundamental physics
• CPT tests with the antihydrogen molecular ion
• Cold trapped molecular ions and hybrid platforms for ions and neutral particles
• Observation of Chemical Reactions between a Trapped Ion and Ultracold Feshbach Dimers
• Enriching the quantum toolbox of ultracold molecules with Rydberg atoms
• Dipole-phonon quantum logic with trapped polar molecular ions
• Direct frequency-comb-driven Raman transitions in the terahertz range
• Experimental and theoretical investigation of a multi-mode cooling scheme using multiple EIT resonances
• Laser Cooling of Radium Ions
• Cooling of a Zero-Nuclear-Spin Molecular Ion to a Selected Rotational State
• A Method for Preparation and Readout of Polyatomic Molecules in Single Quantum States
• Algorithmic Ground-state Cooling of Weakly-Coupled Oscillators using Quantum Logic
• Enantiomer superpositions from matter-wave interference of chiral molecules
• Identification of molecular quantum states using phase-sensitive forces
• Two-photon vibrational transitions in ${\mathrm{O}}_2^{+}$ as probes of variation of the proton-to-electron mass ratio
• Controlling the nature of a charged impurity in a bath of Feshbach dimers
• Mass-selective removal of ions from Paul traps using parametric excitation
• From megahertz to terahertz qubits encoded in molecular ions: theoretical analysis of dipole-forbidden spectroscopic transitions in N${}_2^{+}$
• Coherent coupling and non-destructive measurement of trapped-ion mechanical oscillators
• State-selective coherent motional excitation as a new approach for the manipulation, spectroscopy and state-to-state chemistry of single molecular ions
• Æ codes
• Rotational spectroscopy of a single molecular ion at sub part-per-trillion resolution
• Quantum logic inspired techniques for spacetime-symmetry tests with (anti-)protons
• State resolved investigation of Förster resonant energy transfer in collisions between polar molecules and Rydberg atoms
• A hybrid ion-atom trap with integrated high resolution mass spectrometer
• Trapping and Ground-State Cooling of a Single H${}_2^{+}$
• Optical Pumping of TeH+: Implications for the Search for Varying mp/me
• Prospects for Polar Molecular Ion Optical Probe of Varying Proton-Electron Mass Ratio
• Frequency measurement of the ${}^1{\mathrm{S}}_0,F=5/2\leftrightarrow {}^3{\mathrm{P}}_1,F=7/2$ transition of ${}^{27}$Al${}^{+}$ via quantum logic spectroscopy with ${}^{40}$Ca${}^{+}$
• Higher-order corrections to spin-orbit and spin-spin tensor interactions in hydrogen molecular ions: theory and application to H${}_2^{+}$
• Ultracold ion-atom experiments: cooling, chemistry, and quantum effects
• Atomically-precise engineering of spin-orbit polarons in a kagome magnetic Weyl semimetal
• Laserless quantum gates for electric dipoles in thermal motion
• Quantum state tracking and control of a single molecular ion in a thermal environment
• Coherent Control of Trapped Ion Qubits with Localized Electric Fields
• Combining experiments and relativistic theory for establishing accurate radiative quantities in atoms: the lifetime of the ${}^2$P${}_{3/2}$ state in ${}^{40}$Ca${}^{+}$
• Observation of Microwave Shielding of Ultracold Molecules
• Prospects of nuclear-coupled-dark-matter detection via correlation spectroscopy of I${}_2^{+}$ and Ca${}^{+}$
• A room-temperature ion trapping apparatus with hydrogen partial pressure below $10^{-11}$ mBar
• Strategies for implementing quantum error correction in molecular rotation
• Indirect Cooling of Weakly Coupled Trapped-Ion Mechanical Oscillators
• Prospect for precision quantum logic spectroscopy of vibrational overtone transitions in molecular oxygen ions
• Reassigning the CaH${}^{+}$ 1${}^1\Sigma \to$ 2${}^1\Sigma$ vibronic transition with CaD${}^{+}$
• Quantum control of a single ${\mathrm{H}}_2^{+}$ molecular ion
• Quantum logic spectroscopy with ions in thermal motion
• Photodissociation spectra of single trapped CaOH+ molecular ions
• Studying fundamental physics using quantum enabled technologies with trapped molecular ions
• Dynamics of translational and rotational thermalization of AlF molecules via collisions with cryogenic helium
• Unresolved sideband photon recoil spectroscopy of molecular ions
• Protocol for Optically Pumping AlH${}^{+}$ to a Pure Quantum State
• Photon Recoil Spectroscopy: Systematic Shifts and Nonclassical Enhancements
• State Selective Preparation and Nondestructive Detection of Trapped ${\mathrm{O}}_2^{+}$
• Wavelength modulation laser spectroscopy of N${}_2$O at 17 $\mu$m
• Ultrafast infrared spectroscopy with single molecular ions
• Measurement-based ground state cooling of a trapped ion oscillator
• Adiabatically controlled motional states of a ground-state cooled CaO${}^{+}$ and Ca${}^{+}$ trapped ion chain
• Quantum logic control of a transition metal ion
• Experimental Demonstration of Swift Analytical Universal Control over Nearby Transitions
• Features of Molecular Structure Beneficial for Optical Pumping
• Spectroscopy of electric dipole and quadrupole transitions in ${}^{224}$Ra${}^{+}$
• Precise Determination of Excited State Rotational Constants and Black-Body Thermometry in Coulomb Crystals of Ca${}^{+}$ and CaH${}^{+}$
• Quantum Logic Spectroscopy of an Electron and Positron for Precise Tests of the Standard Model
• High-fidelity quantum state control of a polar molecular ion in a cryogenic environment
• Coulomb crystallization of xenon highly charged ions in a laser-cooled Ca+ matrix
• Laser Cooling and Hyperfine Measurements of Radium-225 Ions
• High-accuracy multi-ion spectroscopy with mixed-species Coulomb crystals
• Landé $g$ factor measurement of ${}^{48}$Ti${}^{+}$ using simultaneous co-magnetometry and quantum logic spectroscopy
• Radioactive Molecules as Laboratories of Fundamental Physics
• High-Resolution Spectroscopy of ${}^{173}$Yb${}^{+}$ Ions
• Molecular Quantum Control Algorithm Design by Reinforcement Learning
• Electric field dissociation of weakly bound molecular ions
• Rotational excitation in sympathetic cooling of diatomic molecular ions by laser-cooled atomic ions
• Diffraction of diatomic molecular beams: a model with applications to Talbot-Lau interferometry
• Optimal Displacement Sensing with Spin-Dependent Squeezed States
• Charge Exchange Dynamics in Cold Collisions of ${}^{40}$CaH${}^{+}$ and ${}^{39}$K