The pairInteraction toolkit for modeling Rydberg physics in alkali and alkaline-earth-like atoms
Johannes Mögerle, Frederic Hummel, Alicia Keil, T. Legrand, Eduard J. Braun, Henri Menke, Jonathan King, Beatriz Olmos, Sebastian Hofferberth, Hans Peter Büchler, Sebastian Weber
Rydberg atoms provide a powerful platform for exploring strongly interacting quantum systems, both in free space and in structured electromagnetic environments, with growing applications in quantum technology. Accurately modeling their single-atom properties and mutual interactions is essential for interpreting experiments and designing new architectures. We present a unified theoretical framework for Rydberg atoms and their interactions based on multi-channel quantum defect theory (MQDT) and static electromagnetic Green’s tensors. MQDT provides a precise description of Rydberg states of divalent atoms such as strontium and ytterbium, while the Green’s tensor formalism provides a general and flexible approach for calculating interactions between two Rydberg atoms in arbitrary geometries, including modifications induced by nearby surfaces. We implement this framework in an updated version of the open-source toolkit PairInteraction [Weber et al., J. Phys. B 50 (2017)]. The implementation leverages high-performance libraries and achieves speedups of one order of magnitude for pair-potential calculations compared to prior software. We demonstrate the capabilities of the toolkit through example applications to divalent atoms and show excellent agreement with experimental data for an exemplary Stark map of Yb. The modular software architecture enables the community to extend it further.
Rydberg atoms provide a powerful platform for exploring strongly interacting quantum systems, both in free space and in structured electromagnetic environments, with growing applications in quantum technology. Accurately modeling their single-atom properties and mutual interactions is essential for interpreting experiments and designing new architectures. We present a unified theoretical framework for Rydberg atoms and their interactions based on multi-channel quantum defect theory (MQDT) and static electromagnetic Green’s tensors. MQDT provides a precise description of Rydberg states of divalent atoms such as strontium and ytterbium, while the Green’s tensor formalism provides a general and flexible approach for calculating interactions between two Rydberg atoms in arbitrary geometries, including modifications induced by nearby surfaces. We implement this framework in an updated version of the open-source toolkit PairInteraction [Weber et al., J. Phys. B 50 (2017)]. The implementation leverages high-performance libraries and achieves speedups of one order of magnitude for pair-potential calculations compared to prior software. We demonstrate the capabilities of the toolkit through example applications to divalent atoms and show excellent agreement with experimental data for an exemplary Stark map of Yb. The modular software architecture enables the community to extend it further.
Rydberg atoms provide a powerful platform for exploring strongly interacting quantum systems, both in free space and in structured electromagnetic environments, with growing applications in quantum technology. Accurately modeling their single-atom properties and mutual interactions is essential for interpreting experiments and designing new architectures. We present a unified theoretical framework for Rydberg atoms and their interactions based on multi-channel quantum defect theory (MQDT) and static electromagnetic Green's tensors. MQDT provides a precise description of Rydberg states of divalent atoms such as strontium and ytterbium, while the Green's tensor formalism provides a general and flexible approach for calculating interactions between two Rydberg atoms in arbitrary geometries, including modifications induced by nearby surfaces. We implement this framework in an updated version of the open-source toolkit PairInteraction [Weber et al., J.~Phys.~B~50 (2017)]. The implementation leverages high-performance libraries and achieves speedups of one order of magnitude for pair-potential calculations compared to prior software. We demonstrate the capabilities of the toolkit through example applications to divalent atoms and show excellent agreement with experimental data for an exemplary Stark map of 174Yb. The modular software architecture enables the community to extend it further.
Highly excited Rydberg states and their interactions play an important role in quantum computing and simulation. These properties can be predicted accurately for alkali atoms with simple Rydberg level structures. However, an extension of these methods to more complex atoms such as alkaline-earth atoms has not been demonstrated or experimentally validated. Here, we present multichannel quantum defect models for highly excited Yb 174 and Yb 171 Rydberg states with L ≤ 2 . The models are developed using a combination of existing literature data and new, high-precision laser and microwave spectroscopy in an atomic beam, and validated by detailed comparison with experimentally measured Stark shifts and magnetic moments. We then use these models to compute interaction potentials between two Yb atoms, and find excellent agreement with direct measurements in an optical tweezer array. From the computed interaction potential, we identify an anomalous Förster resonance that likely degraded the fidelity of previous entangling gates in Yb 171 using F = 3 / 2 Rydberg states. We then identify a more suitable F = 1 / 2 state, and achieve a state-of-the-art controlled- gate fidelity of F = 0.994 ( 1 ) , with the remaining error fully explained by known sources. This work establishes a solid foundation for the continued development of quantum computing, simulation, and entanglement-enhanced metrology with Yb neutral atom arrays.
Quantum information processing with neutral atoms relies on Rydberg excitation for entanglement generation. While the use of heavy divalent or open-shell elements, such as strontium or ytterbium, has benefits due to their optically active core and a variety of possible qubit encodings, their Rydberg structure is generally complex. For some isotopes in particular, hyperfine interactions are relevant even for highly excited electronic states. We employ multichannel quantum defect theory to infer the Rydberg structure of isotopes with nonzero nuclear spin and perform nonperturbative Rydberg-pair interaction calculations. We find that due to the high level density and sensitivities to external fields, experimental parameters must be precisely controlled. Specifically in Sr 87 , we study an intrinsic Förster resonance, unique to divalent atoms with hyperfine-split thresholds, which simultaneously provides line stability with respect to external field fluctuations and enhanced long-range interactions. Additionally, we provide parameters for pair states that can be effectively described by single-channel Rydberg series. The explored pair states provide exciting opportunities for applications in the blockade regime, as well as for more exotic long-range interactions such as largely flat, distance-independent potentials. Published by the American Physical Society 2024
Divalent atoms have emerged as powerful alternatives to alkalis in ultracold atom platforms, offering unique advantages arising from their two-electron structure. Among these species, ytterbium (Yb) is especially promising, yet its anionic properties and its Rydberg spectrum remain comparatively unexplored. In this work, we perform a first and comprehensive experimental and theoretical investigation of ultralong-range Rydberg molecules (ULRMs) of 174Yb in 6sns1S0 Rydberg states across nearly two decades in principal quantum number n and three orders of magnitude in molecular binding energy. Using the Coulomb Green's function formalism, we compute Born-Oppenheimer molecular potentials describing the Rydberg atom in the presence of a ground-state perturber and achieve quantitative agreement with high-resolution molecular spectra. This enables the extraction of low-energy electron-Yb scattering phase shifts, including the zero-energy s-wave scattering length and the positions of two spin-orbit split p-wave shape resonances. Our results provide strong evidence that the Yb− anion exists only as a metastable resonance.% We additionally show the sensitivity of ULRM spectra to the atomic quantum defects, using this to determine the quantum defect of the 6s23f1F3 state. Together, these findings establish Yb ULRMs as a powerful probe of electron-Yb interactions and lay essential groundwork for future Rydberg experiments with divalent atoms.
We present calculations of long-range interactions in Rydberg atoms, with a focus on the dipole-dipole interactions of strontium Rydberg states. The growing use of Rydberg states in the field of cold atoms necessitates a more detailed understanding of the effects of dipole-dipole interactions, which are currently being investigated in a number of research groups worldwide. Calculations of long-range interactions in Rydberg states of caesium, cal- cium, rubidium, strontium and ytterbium are presented. By taking the one active electron approximation we develop consistent models of these long- range interactions, and construct a survey of the Rydberg state dipole-dipole interactions and quadrupole-quadrupole interactions. We compare the inter- actions between series and between atoms, highlighting the importance of certain series for applications suggested in previous works. In order to include two-electron effects in the description of dipole-dipole interactions in divalent atoms, we use multichannel quantum defect theory (MQDT) to develop models of the Rydberg series of strontium. We use an empirical reactance matrix formalism, where the reactance matrix is fitted to reproduce experimentally measured values of the bound state energy levels. Models are found for all series of strontium with L ≤ 3. We extend the MQDT formalism to the description of the natural radiative lifetimes of strontium, where the perturbers are found to have a large quenching effect on these lifetimes. By incorporating the MQDT description of the Rydberg states of strontium into the calculation of dipole-dipole interactions, we find a spin-forbidden two-atom resonance in the 3D2 states of strontium. We consider a one- dimensional lattice of strontium atoms, and find that the internal dynamics of the Rydberg atoms demonstrates spin transport for large lattice spacings and a separation of the spin and total angular momentum dynamics for small lattice spacings. Spin-angular momentum separation (analogous to spin-charge separation in condensed matter) in strontium Rydberg atoms may have uses in the investigation of one-dimensional Fermi gases and their description using Luttinger liquid theory.
Abstract Using the reactance matrix approach, we systematically develop new multichannel quantum defect theory (MQDT) models for the singlet and triplet S, P, D and F states of strontium below the first ionization limit, based on improved energy level measurements. The new models reveal additional insights into the character of doubly excited perturber states, and the improved energy level measurements for certain series allow fine structure to be resolved for those series’ perturbers. Comparison between the predictions of the new models and those of previous empirical and ab initio studies reveals good agreement with most series; however, some discrepancies are highlighted. Using the MQDT wave functions derived from our models we calculate other observables such as Landé -factors and radiative lifetimes. The analysis reveals the impact of perturbers on the Rydberg state properties of divalent atoms, highlighting the importance of including two-electron effects in the calculations of these properties. The work enables future investigations of properties such as Stark maps and long-range interactions of Rydberg states of strontium.