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

Abstract

State-of-the-art ab initio techniques have been applied to compute the potential energy curves for the electronic states in the A^1Σ_u^+, c^3Π_u, and a^3Σ_u^+ manifold of the strontium dimer, the spin-orbit and nonadiabatic coupling matrix elements between the states in the manifold, and the electric transition dipole moment from the ground X^1Σ_g^+ to the nonrelativistic and relativistic states in the A+c+a manifold. The potential energy curves and transition moments were obtained with the linear response (equation of motion) coupled cluster method limited to single, double, and linear triple excitations for the potentials and limited to single and double excitations for the transition moments. The spin-orbit and nonadiabatic coupling matrix elements were computed with the multireference configuration interaction method limited to single and double excitations. Our results for the nonrelativistic and relativistic (spin-orbit coupled) potentials deviate substantially from recent ab initio calculations. The potential energy curve for the spectroscopically active (1)0_u^+ state is in quantitative agreement with the empirical potential fitted to high-resolution Fourier transform spectra [A. Stein, H. Knoeckel, and E. Tiemann, Eur. Phys. J. D 64, 227 (2011)]. The computed ab initio points were fitted to physically sound analytical expressions, and used in converged coupled channel calculations of the rovibrational energy levels in the A+c+a manifold and line strengths for the A^1Σ_u^+ <-- X^1Σ_g^+ transitions. Positions and lifetimes of quasi-bound Feshbach resonances lying above the ^1S + ^3P_1 dissociation limit were also obtained. Our results reproduce (semi)quantitatively the experimental data observed thus far. Predictions for on-going and future experiments are also reported.

Final version, accepted for publication in Journal of Chemical Physics

References in corpus (9)

• Precision Test of Mass Ratio Variations with Lattice-Confined Ultracold Molecules
• Bose-Einstein condensation of alkaline earth atoms: ${}^{40}${Ca}
• Bose-Einstein Condensation of an Ytterbium Isotope
• Narrow Line Photoassociation in an Optical Lattice
• Two-photon photoassociative spectroscopy of ultracold 88-Sr
• Sympathetic cooling of the Ba${}^{+}$ ion by collisions with ultracold Rb atoms: theoretical prospects
• Prospects for application of ultracold Sr${}_2$ molecules in precision measurements
• Formation of deeply bound ultracold Sr_2 molecules by photoassociation near the ^1S + ^3P_1 intercombination line
• Engineering an all-optical route to ultracold molecules in their vibronic ground state

Cited by in corpus (19)

• Creation of ultracold Sr2 molecules in the electronic ground state
• Cold interactions between an Yb${}^{+}$ ion and a Li atom: Prospects for sympathetic cooling, radiative association, and Feshbach resonances
• Mass scaling and non-adiabatic effects in photoassociation spectroscopy of ultracold strontium atoms
• A terahertz vibrational molecular clock with systematic uncertainty at the $10^{-14}$ level
• Diatomic molecules of alkali-metal and alkaline-earth-metal atoms: interaction potentials, dipole moments, and polarizabilities
• Enhancing photoassociation rates by non-resonant light control of shape resonances
• Ultracold ${}^{88}{\mathrm{Sr}}_2$ molecules in the absolute ground state
• Ab initio properties of the ground-state polar and paramagnetic europium-alkali-metal-atom and europium-alkaline-earth-metal-atom molecules
• Transition strength measurements to guide magic wavelength selection in optically trapped molecules
• Analytical two-center integrals over Slater geminal functions
• Optical Feshbach resonances and ground state molecule production in the RbHg system
• Relativistic calculations of $C_6$ and $C_8$ coefficients for strontium dimers
• Asymptotic model for shape resonance control of diatomics by intense non-resonant light
• Control of Ultracold Photodissociation with Magnetic Fields
• Transition moments between excited electronic states from the Hermitian formulation of the coupled cluster quadratic response function
• Searching for New Fundamental Interactions via Isotopic Shifts in Molecular Lattice Clocks
• Excited electronic states of Sr${}_2$: ab initio predictions and experimental observation of the $2^1{\Sigma }_u^{+}$ state
• Spin-orbit coupling matrix elements from the explicitly connected expressions of the response functions within the coupled-cluster theory
• Ab initio study of the reactivity of ultracold RbSr$+$RbSr collisions