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Physical Review A

Forming ultracold YbAg molecules via photoassociation predicted from ab initio calculations

Xiang Yuan, Yong Liu

Published Dec 17, 2024• 1 citation
Publisher

Abstract

This paper discusses the formation of ultracold YbAg molecules via photoassociation, following the proposal of using YbAg as a promising molecular candidate for electron electric dipole moment experiments [M. Verma et al. Phys. Rev. Lett. 125, 153201 (2020)]. Our study utilizes high-level ab initio calculations, encompassing both multireference configuration interaction, relativistic Fock-space coupled cluster, and Kramers-restricted configuration interaction methods, to investigate the electronic structures including potential energy curves, spectroscopic constant, vibrational energy levels, and associated transition dipole moment and Franck-Condon factors for 28 electronic states. By choosing (5)($\mathrm{\ensuremath{\Omega}}=3/2$) as the intermediate state, we discuss the feasibility of forming ultracold YbAg molecules through stimulated Raman adiabatic passage method.

DOI
10.1103/physreva.110.062813

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This paper discusses the formation of ultracold YbAg molecules via photoassociation, following the proposal of using YbAg as a promising molecular candidate for electron electric dipole moment experiments [M. Verma et al. Phys. Rev. Lett. 125, 153201 (2020)]. Our study utilizes high-level ab initio calculations, encompassing both multireference configuration interaction, relativistic Fock-space coupled cluster, and Kramers-restricted configuration interaction methods, to investigate the electronic structures including potential energy curves, spectroscopic constant, vibrational energy levels, and associated transition dipole moment and Franck-Condon factors for 28 electronic states. By choosing (5)(\ensuremathΩ=3/2\mathrm{\ensuremath{\Omega}}=3/2\ensuremathΩ=3/2) as the intermediate state, we discuss the feasibility of forming ultracold YbAg molecules through stimulated Raman adiabatic passage method.
State-of-the-art ab initio techniques have been applied to compute the potential energy curves for the SrYb molecule in the Born-Oppenheimer approximation for the electronic ground state and the first fifteen excited singlet and triplet states. All the excited state potential energy curves were computed using the equation of motion approach within the coupled-cluster singles and doubles framework and large basis-sets, while the ground state potential was computed using the coupled cluster method with single, double, and noniterative triple excitations. The leading long-range coefficients describing the dispersion interactions at large interatomic distances are also reported. The electric transition dipole moments have been obtained as the first residue of the polarization propagator computed with the linear response coupled-cluster method restricted to single and double excitations. Spin-orbit coupling matrix elements have been evaluated using the multireference configuration interaction method restricted to single and double excitations with a large active space. The electronic structure data were employed to investigate the possibility of forming deeply bound ultracold SrYb molecules in an optical lattice in a photoassociation experiment using continuous-wave lasers. Photoassociation near the intercombination line transition of atomic strontium into the vibrational levels of the strongly spin-orbit mixed b(3)Σ(+), a(3)Π, A(1)Π, and C(1)Π states with subsequent efficient stabilization into the v'' = 1 vibrational level of the electronic ground state is proposed. Ground state SrYb molecules can be accumulated by making use of collisional decay from v'' = 1 to v'' = 0. Alternatively, photoassociation and stabilization to v'' = 0 can proceed via stimulated Raman adiabatic passage provided that the trapping frequency of the optical lattice is large enough and phase coherence between the pulses can be maintained over at least tens of microseconds.
Abstract Ultracold YbAg molecules have been recently proposed as promising candidates for electron electric dipole moment searches Verma et al (2020 Phys. Rev. Lett. 125 153201). Here, we calculate potential energy curves, permanent electric dipole and quadrupole moments, and static electric dipole polarizabilities for the YbCu, YbAg, and YbAu molecules in their ground electronic states. We use the coupled cluster method restricted to single, double, and noniterative triple excitations with large Gaussian basis sets, while the scalar relativistic effects are included within the small-core energy-consistent pseudopotentials. We find that the studied molecules are relatively strongly bound with the well depths of 5708 cm −1 , 5253 cm −1 , and 13349 cm −1 and equilibrium distances of 5.50 bohr, 5.79 bohr, and 5.55 bohr for YbCu, YbAg, and YbAu, respectively. They have large permanent electric dipole moments of 3.2 D , 3.3 D , and 5.3 D at equilibrium distances, respectively. We also calculate equilibrium geometries and energies of corresponding trimers. The studied molecules are chemically reactive unless they are segregated in an optical lattice or shielded with external fields. The investigated molecules may find application in ultracold controlled chemistry, dipolar many-body physics, or precision measurement experiments.
We recently reported the formation of ultracold LiCs molecules in the rovibrational ground state X1sigma+, v" = 0,J" = 0 (J. Deiglmayr et al., Phys. Rev. Lett., 2008, 101, 133004). Here we discuss details of the experimental setup and present a thorough analysis of the photoassociation step including the photoassociation line shape. We predict the distribution of produced ground state molecules using accurate potential energy curves combined with an ab initio dipole transition moment and compare this prediction with experimental ionization spectra. Additionally we improve the value of the dissociation energy for the X1sigma+ state by high resolution spectroscopy of the vibrational ground state.
Ultracold paramagnetic and polar diatomic molecules are among the promising systems for quantum simulation of lattice-spin models. Unfortunately, their experimental observation is still challenging. Based on our recent ab initio calculations, we analyze the feasibility of all-optical schemes for the formation of ultracold 87Rb84Sr^{87}\mathrm{Rb}^{84}\mathrm{Sr}87Rb84Sr bosonic molecules. A first possibility is photoassociation followed by spontaneous emission. The photoassociation rate coefficients toward electronic states converging to the 87Rb(5s2S1/2)+84Sr(5s5p3P0,1,2^{87}\mathrm{Rb}(5s\phantom{\rule{0.16em}{0ex}}^{2}S_{1/2})+^{84}\mathrm{Sr}(5s5p\phantom{\rule{0.16em}{0ex}}^{3}P_{0,1,2}87Rb(5s2S1/2​)+84Sr(5s5p3P0,1,2​) asymptotes are particularly small for vibrational levels close to the asymptote. The creation of molecules would be more interesting by using deeply bound levels which preferentially relax to the ${v}^{\ensuremath{'}\ensuremath{'}}=0$ level of the ground state. On the other hand, the photoassociation rate coefficients toward electronic states correlated to the Rb(5p2P1/2,3/2)+Sr(5s21S0\mathrm{Rb}(5p\phantom{\rule{0.16em}{0ex}}^{2}P_{1/2,3/2})+\mathrm{Sr}(5{s}^{2}\phantom{\rule{0.16em}{0ex}}^{1}S_{0}Rb(5p2P1/2,3/2​)+Sr(5s21S0​) are significant for levels close to the asymptote. The spontaneous emission thus creates weakly bound molecules in a single vibrational level. A second option relies on stimulated Raman adiabatic passage implemented in a tight optical trap. It efficiently creates weakly bound ground-state molecules in a well-defined level, thus providing a promising alternative to magnetic Feshbach resonances for further population transfer toward the absolute ground state of the RbSr molecule.
We present high-level four-component coupled cluster and multireference configuration interaction calculations of potential energy curves, dipole moment, Franck-Condon factors and spectroscopic constants of the newly formed RbYb molecule. From finite-field calculations we obtain an electric dipole moment for RbYb of almost 1 D. In combination with its magnetic dipole moment this makes RbYb an excellent candidate for trapping and for studying dipolar interaction in the ultracold regime. Significant Franck-Condon factors are found between the rovibronic ground state and the lowest rovibrational levels of the first excited 2Sigma1/2+ state but also between a broad range of rovibrational levels of the 2Pi1/2 and 2Pi3/2 states. This allows for several two-step approaches to reach the rovibronic ground state after initial photoassociation.
Abstract Molecular ions formed in cold hybrid ion-atom experiments may find interesting applications ranging from precision measurements to controlled chemical reactions. Here, we investigate electronic structure of the Sr2 + molecular ion, which may be produced by photoassociation of laser-cooled Sr+ ions immersed into an ultracold gas of Sr atoms or by ionization of ultracold Sr2 molecules. Using ab initio electronic structure methods, such as the coupled cluster and configuration interaction ones with small-core relativistic energy-consistent pseudopotentials and large Gaussian basis sets, we calculate potential energy curves for the ground and 41 excited electronic states, and electric dipole transition moments between them. We show that alkaline-earth molecular ions despite of their apparently simple structure with three valence electrons only are challenging for state-of-the-art quantum chemistry methods due to their multireference nature and high density of states. Finally, we calculate and analyze Franck-Condon factors governing the photoionization of ground-state Sr2 molecules into 2Σu + and 2Σg + states of Sr2 + molecular ions. The present results may be useful for studying and guiding formation and spectroscopy of cold Sr2 + molecular ions.