Photodissociation of ultracold diatomic strontium molecules with quantum state control

Abstract

Chemical reactions at ultracold temperatures are expected to be dominated by quantum mechanical effects. Although progress towards ultracold chemistry has been made through atomic photoassociation, Feshbach resonances and bimolecular collisions, these approaches have been limited by imperfect quantum state selectivity. In particular, attaining complete control of the ground or excited continuum quantum states has remained a challenge. Here we achieve this control using photodissociation, an approach that encodes a wealth of information in the angular distribution of outgoing fragments. By photodissociating ultracold 88Sr2 molecules with full control of the low-energy continuum, we access the quantum regime of ultracold chemistry, observing resonant and nonresonant barrier tunneling, matter-wave interference of reaction products and forbidden reaction pathways. Our results illustrate the failure of the traditional quasiclassical model of photodissociation and instead are accurately described by a quantum mechanical model. The experimental ability to produce well-defined quantum continuum states at low energies will enable high-precision studies of long-range molecular potentials for which accurate quantum chemistry models are unavailable, and may serve as a source of entangled states and coherent matter waves for a wide range of experiments in quantum optics.

References in corpus (21)

• Feshbach Resonances in Ultracold Gases
• Quantum-State Controlled Chemical Reactions of Ultracold KRb Molecules
• Spectroscopic observation of SU(N)-symmetric interactions in Sr orbital magnetism
• Precise determination of ${}^6$Li cold collision parameters by radio-frequency spectroscopy on weakly bound molecules
• Manipulation of Molecules with Electromagnetic Fields
• Strong saturation absorption imaging of dense clouds of ultracold atoms
• Bounds on fifth forces from precision measurements on molecules
• Precise study of asymptotic physics with subradiant ultracold molecules
• Einstein-Podolsky-Rosen correlations via dissociation of a molecular Bose-Einstein condensate
• Optical Production of Stable Ultracold ${}^{88}$Sr${}_2$ Molecules
• `Stückelberg interferometry' with ultracold molecules
• Rovibrational dynamics of the strontium molecule in the A^1Σ_u^+, c^3Π_u, and a^3Σ_u^+ manifold from state-of-the-art ab initio calculations
• Ultracold hydrogen and deuterium production via Doppler-cooled Feshbach molecules
• Complete photoionization experiments via ultra-fast coherent control with polarization-multiplexing
• Mass scaling and non-adiabatic effects in photoassociation spectroscopy of ultracold strontium atoms
• High-precision spectroscopy of ultracold molecules in an optical lattice
• Feshbach Spectroscopy of a Shape Resonance
• Nonadiabatic Effects in Ultracold Molecules via Anomalous Linear and Quadratic Zeeman Shifts
• Enhancing photoassociation rates by non-resonant light control of shape resonances
• Metastable Feshbach Molecules in High Rotational States
• Control of Optical Transitions with Magnetic Fields in Weakly Bound Molecules

Cited by in corpus (39)

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• Optical cycling, radiative deflection and laser cooling of barium monohydride (BaH)
• Observation of Rydberg-atom macrodimers: micrometer-sized diatomic molecules
• High-resolution optical spectroscopy with a buffer-gas-cooled beam of BaH molecules
• Ultracold field-linked tetratomic molecules
• Diatomic molecules of alkali-metal and alkaline-earth-metal atoms: interaction potentials, dipole moments, and polarizabilities
• Second-Scale Coherence Measured at the Quantum Projection Noise Limit with Hundreds of Molecular Ions
• In-situ Imaging of a Single-Atom Wave Packet in Continuous Space
• Steering ultracold reactions through long-lived transient intermediates
• Coherent Manipulation of Orbital Feshbach Molecules of Two-Electron Atoms
• Probing ultracold chemistry using ion spectrometry
• Molecular Frame Photoelectron Angular Distributions in Polyatomic Molecules from Lab Frame Coherent Rotational Wavepacket Evolution
• Mapping partial wave dynamics in scattering resonances by rotational de-excitation collisions
• Two interacting ultracold molecules in a one-dimensional harmonic trap
• Atom-Number Enhancement by Shielding Atoms from Losses in Strontium Magneto-Optical Traps
• Microscopic electronic structure tomography of Rydberg macrodimers
• Optical Feshbach resonances and ground state molecule production in the RbHg system
• Transition strength measurements to guide magic wavelength selection in optically trapped molecules
• Calculation of Araki-Sucher correction for many-electron systems
• Crossover from the Ultracold to the Quasiclassical Regime in State-Selected Photodissociation
• Rydberg Macrodimers: Diatomic molecules on the micrometer scale
• Control of Ultracold Photodissociation with Magnetic Fields
• Photodissociation of long-range Rydberg molecules
• Combining Slater-type orbitals and effective core potentials
• Van der Waals molecules consisting of a zinc or cadmium atom interacting with an alkali-metal or alkaline-earth-metal atom
• Chemical reactions of ultracold alkaline-earth-metal diatomic molecules
• Experimental and Theoretical Investigation of the Crossover from the Ultracold to the Quasiclassical Regime of Photodissociation
• Transition moments between excited electronic states from the Hermitian formulation of the coupled cluster quadratic response function
• Probing the limits of optical cycling in a predissociative diatomic molecule
• High-intensity two-frequency photoassociation spectroscopy of a weakly bound molecular state: theory and experiment
• Excited electronic states of Sr${}_2$: ab initio predictions and experimental observation of the $2^1{\Sigma }_u^{+}$ state
• Ab initio electronic structure of the Sr${}_2^{+}$ molecular ion
• High-Efficiency Quantum-State Detection of ThF${}^{+}$ with Resonance-Enhanced Multiphoton Asymmetric Dissociation
• Magneto-Optical Trapping of a Metal Hydride Molecule
• Chemistry in a Cryogenic Buffer Gas Cell
• Optimization of the Femtosecond Laser Impulse for Excitation and the Spin-Orbit Mediated Dissociation in the NaRb Dimer