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Tomography of Feshbach Resonance States

Baruch Margulis, Karl P. Horn, Daniel M. Reich, Meenu Upadhyay, Nitzan Kahn, Arthur Christianen, Ad van der Avoird, Gerrit C. Groenenboom, Markus Meuwly, Christiane P. Koch, Edvardas Narevicius

Published Jan 1, 2023• 0 citations
Publisher

Abstract

Feshbach resonances are fundamental to interparticle interactions and become particularly important in cold collisions with atoms, ions, and molecules. Here we present the detection of Feshbach resonances in a benchmark system for strongly interacting and highly anisotropic collisions -- molecular hydrogen ions colliding with noble gas atoms. The collisions are launched by cold Penning ionization exclusively populating Feshbach resonances that span both short- and long-range parts of the interaction potential. We resolved all final molecular channels in a tomographic manner using ion-electron coincidence detection and demonstrated the non-statistical nature of the final state distribution. By performing quantum scattering calculations on ab initio potential energy surfaces, we show that the isolation of the Feshbach resonance pathways reveals their distinctive fingerprints in the collision outcome.

DOI
10.17169/refubium-42276

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Feshbach resonances are fundamental to interparticle interactions and become particularly important in cold collisions with atoms, ions, and molecules. Here we present the detection of Feshbach resonances in a benchmark system for strongly interacting and highly anisotropic collisions -- molecular hydrogen ions colliding with noble gas atoms. The collisions are launched by cold Penning ionization exclusively populating Feshbach resonances that span both short- and long-range parts of the interaction potential. We resolved all final molecular channels in a tomographic manner using ion-electron coincidence detection. We demonstrate the non-statistical nature of the final state distribution. By performing quantum scattering calculations on ab initio potential energy surfaces, we show that the isolation of the Feshbach resonance pathways reveals their distinctive fingerprints in the collision outcome.

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Direct observation of a Feshbach resonance by coincidence detection of ions and electrons in Penning ionization collisions

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Abstract Observation of molecular dynamics with quantum state resolution is one of the major challenges in chemical physics. Complete characterization of collision dynamics leads to the microscopic understanding and unraveling of different quantum phenomena such as scattering resonances. Here we present an experimental approach for observing molecular dynamics involving neutral particles and ions that is capable of providing state-to-state mapping of the dynamics. We use Penning ionization reaction between argon and metastable helium to generate argon ion and ground state helium atom pairs at separation of several angstroms. The energy of an ejected electron carries the information about the initial electronic state of an ion. The coincidence detection of ionic products provides a state resolved description of the post-ionization ion-neutral dynamics. We demonstrate that correlation between the electron and ion energy spectra enables us to directly observe the spin-orbit excited Feshbach resonance state of HeAr+. We measure the lifetime of the quasi-bound HeAr+A2 state and discuss possible applications of our method.

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Universal relations between Feshbach resonances and molecules

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The susceptibility of ultracold gases to precise manipulation via external fields makes them ideal systems to study fundamental quantum mechanical phenomena. Various regimes, which are not possible to reach in condensed matter or nuclear physics, can be probed with these quantum gases. Especially the tunability of the interactions and confining potentials make that these ultracold gases offer unique possibilities to explore and study universal behavior. The tunability of the dominant two-body interactions in dilute ultracold atomic gases stems from the presence of Feshbach resonances. Via these resonances pairs of ultracold atoms can be associated to form ultracold molecules. In fact, measurements of Feshbach resonance positions can be used to reveal part of the underlying molecular structure. Vica versa, accurate molecular Born-Oppenheimer potentials can be used as input for full numerical coupled-channels calculations to reliably predict Feshbach resonances. For most of the heteronuclear mixtures currently studied however, the relevant molecular potentials are not accurate enough. As the coupled-channels method is often too elaborate and too time consuming to be used to fit the measured data to enable the construction of more accurate potentials, a need for accurate models which complement this established method is created. In this thesis we have developed a simplified model for resonant scattering of two ultracold atoms which fulfills this need. The asymptotic bound-state model (ABM) is a hierarchical model which can be systematically increased in complexity and accuracy. In its most simple form, the ABM only needs two parameters to predict the position and strength of Feshbach resonances: Two binding energies corresponding to the least bound state of the two molecular potentials involved. We demonstrate that this model, although it is solely based on bound states, can incorporate threshold effects. Additionally, the model can be extended to include: Multiple vibrational levels, overlapping resonances, and magnetic dipole-dipole interactions. This versatile model allows for a description of Feshbach resonances in a large variety of systems without accurate knowledge of the relevant molecular Born-Oppenheimer potentials. Being computationally light, the ABM can be used to analyze measurements of Feshbach resonances and hereby expose the basic underlying molecular structure. Additionally, the ABM is well suited to map out all available Feshbach resonances in a system. This ability is particularly useful when an optimal resonance is required for a certain experiment. For the 6Li-40K mixture we have utilized this ability to experimentally observe a strong Feshbach resonance which offers promising perspectives to reach the strongly interacting universal regime in a mass-imbalanced Fermi gas. By analyzing the various inelastic decay processes and the accuracy of the ab initio Born-Oppenheimer potentials, we predict a strong resonance in a mixture of metastable bosonic and fermionic helium atoms. For the homonuclear (bosonic as well as fermionic) helium gas we do not find strong resonances. For an ultracold gas of 40K atoms, an elaborate combined theoretical and experimental effort is presented to map out the Feshbach resonance structure. On the experimental side we observed 36 Feshbach resonances, 31 of which where observed for the first time. These observations are in excellent agreement with coupled-channels calculations which use unmodified Born-Oppenheimer potentials as input. On the theoretical side, we present a comparison between different simplified models of resonance scattering and the full numerical coupled-channels calculations. We have developed the resonant state model (RSM) to describe the resonant scattering of two ultracold atoms. This model is founded on resonant states, the natural (eigen) frequencies of the two-body system, and their non-trivial properties. Threshold effects are implicitly build into the RSM. The RSM can describe the effect of the continuum of scattering states, states which are neglected in the ABM, on the position and strength of a Feshbach resonance by only a few resonant states. Especially when a low-energy resonance is embedded in the continuum of scattering states, the effect of these states on the Feshbach resonance cannot be neglected. The RSM can be viewed as the natural generalization of the ABM. As the RSM can be based on just a few resonant states, it retains the computational simplicity of the ABM. Using the tunability of two-body interactions induced by a Feshbach resonance, we describe a crossover for a rotating Fermi gas between two strongly-correlated many-body states. We demonstrate that the correlation induced long-range interaction will shift the crossover with respect to the non-rotating case.

•Jan 1, 2011•1 citation
Feshbach resonances are fundamental to interparticle interactions and become particularly important in cold collisions with atoms, ions, and molecules. Here we present the detection of Feshbach resonances in a benchmark system for strongly interacting and highly anisotropic collisions -- molecular hydrogen ions colliding with noble gas atoms. The collisions are launched by cold Penning ionization exclusively populating Feshbach resonances that span both short- and long-range parts of the interaction potential. We resolved all final molecular channels in a tomographic manner using ion-electron coincidence detection and demonstrated the non-statistical nature of the final state distribution. By performing quantum scattering calculations on ab initio potential energy surfaces, we show that the isolation of the Feshbach resonance pathways reveals their distinctive fingerprints in the collision outcome.
Feshbach resonances are fundamental to interparticle interactions and become particularly important in cold collisions with atoms, ions, and molecules. Here we present the detection of Feshbach resonances in a benchmark system for strongly interacting and highly anisotropic collisions -- molecular hydrogen ions colliding with noble gas atoms. The collisions are launched by cold Penning ionization exclusively populating Feshbach resonances that span both short- and long-range parts of the interaction potential. We resolved all final molecular channels in a tomographic manner using ion-electron coincidence detection. We demonstrate the non-statistical nature of the final state distribution. By performing quantum scattering calculations on ab initio potential energy surfaces, we show that the isolation of the Feshbach resonance pathways reveals their distinctive fingerprints in the collision outcome.
Feshbach resonances are fundamental to interparticle interactions and become particularly important in cold collisions with atoms, ions, and molecules. In this work, we present the detection of Feshbach resonances in a benchmark system for strongly interacting and highly anisotropic collisions: molecular hydrogen ions colliding with noble gas atoms. The collisions are launched by cold Penning ionization, which exclusively populates Feshbach resonances that span both short- and long-range parts of the interaction potential. We resolved all final molecular channels in a tomographic manner using ion-electron coincidence detection. We demonstrate the nonstatistical nature of the final-state distribution. By performing quantum scattering calculations on ab initio potential energy surfaces, we show that the isolation of the Feshbach resonance pathways reveals their distinctive fingerprints in the collision outcome.
High Resolution Image Download MS PowerPoint Slide High-quality potential energy surfaces (PESs) are prerequisites for quantitative atomistic simulations with both quantum and classical dynamics approaches. The ultimate test for the validity of a PES entails comparisons with judiciously chosen experimental observables. Here we ask whether cold collision measurements are sufficiently informative to validate and distinguish between high-level, state-of-the art PESs for the strongly interacting Ne–H 2 + system. We show that measurement of the final state distributions for a process that involves several metastable intermediate states is sufficient to identify the PES that captures the long-range interactions properly. Furthermore, we show that a modest increase in the experimental energy resolution will allow for resolving individual Feshbach resonances and enable a quantitative probe of the interactions in the short and intermediate ranges.
Abstract Observation of molecular dynamics with quantum state resolution is one of the major challenges in chemical physics. Complete characterization of collision dynamics leads to the microscopic understanding and unraveling of different quantum phenomena such as scattering resonances. Here we present an experimental approach for observing molecular dynamics involving neutral particles and ions that is capable of providing state-to-state mapping of the dynamics. We use Penning ionization reaction between argon and metastable helium to generate argon ion and ground state helium atom pairs at separation of several angstroms. The energy of an ejected electron carries the information about the initial electronic state of an ion. The coincidence detection of ionic products provides a state resolved description of the post-ionization ion-neutral dynamics. We demonstrate that correlation between the electron and ion energy spectra enables us to directly observe the spin-orbit excited Feshbach resonance state of HeAr+. We measure the lifetime of the quasi-bound HeAr+ A2 state and discuss possible applications of our method.
Abstract Observation of molecular dynamics with quantum state resolution is one of the major challenges in chemical physics. Complete characterization of collision dynamics leads to the microscopic understanding and unraveling of different quantum phenomena such as scattering resonances. Here we present an experimental approach for observing molecular dynamics involving neutral particles and ions that is capable of providing state-to-state mapping of the dynamics. We use Penning ionization reaction between argon and metastable helium to generate argon ion and ground state helium atom pairs at separation of several angstroms. The energy of an ejected electron carries the information about the initial electronic state of an ion. The coincidence detection of ionic products provides a state resolved description of the post-ionization ion-neutral dynamics. We demonstrate that correlation between the electron and ion energy spectra enables us to directly observe the spin-orbit excited Feshbach resonance state of HeAr+. We measure the lifetime of the quasi-bound HeAr+A2 state and discuss possible applications of our method.
The susceptibility of ultracold gases to precise manipulation via external fields makes them ideal systems to study fundamental quantum mechanical phenomena. Various regimes, which are not possible to reach in condensed matter or nuclear physics, can be probed with these quantum gases. Especially the tunability of the interactions and confining potentials make that these ultracold gases offer unique possibilities to explore and study universal behavior. The tunability of the dominant two-body interactions in dilute ultracold atomic gases stems from the presence of Feshbach resonances. Via these resonances pairs of ultracold atoms can be associated to form ultracold molecules. In fact, measurements of Feshbach resonance positions can be used to reveal part of the underlying molecular structure. Vica versa, accurate molecular Born-Oppenheimer potentials can be used as input for full numerical coupled-channels calculations to reliably predict Feshbach resonances. For most of the heteronuclear mixtures currently studied however, the relevant molecular potentials are not accurate enough. As the coupled-channels method is often too elaborate and too time consuming to be used to fit the measured data to enable the construction of more accurate potentials, a need for accurate models which complement this established method is created. In this thesis we have developed a simplified model for resonant scattering of two ultracold atoms which fulfills this need. The asymptotic bound-state model (ABM) is a hierarchical model which can be systematically increased in complexity and accuracy. In its most simple form, the ABM only needs two parameters to predict the position and strength of Feshbach resonances: Two binding energies corresponding to the least bound state of the two molecular potentials involved. We demonstrate that this model, although it is solely based on bound states, can incorporate threshold effects. Additionally, the model can be extended to include: Multiple vibrational levels, overlapping resonances, and magnetic dipole-dipole interactions. This versatile model allows for a description of Feshbach resonances in a large variety of systems without accurate knowledge of the relevant molecular Born-Oppenheimer potentials. Being computationally light, the ABM can be used to analyze measurements of Feshbach resonances and hereby expose the basic underlying molecular structure. Additionally, the ABM is well suited to map out all available Feshbach resonances in a system. This ability is particularly useful when an optimal resonance is required for a certain experiment. For the 6Li-40K mixture we have utilized this ability to experimentally observe a strong Feshbach resonance which offers promising perspectives to reach the strongly interacting universal regime in a mass-imbalanced Fermi gas. By analyzing the various inelastic decay processes and the accuracy of the ab initio Born-Oppenheimer potentials, we predict a strong resonance in a mixture of metastable bosonic and fermionic helium atoms. For the homonuclear (bosonic as well as fermionic) helium gas we do not find strong resonances. For an ultracold gas of 40K atoms, an elaborate combined theoretical and experimental effort is presented to map out the Feshbach resonance structure. On the experimental side we observed 36 Feshbach resonances, 31 of which where observed for the first time. These observations are in excellent agreement with coupled-channels calculations which use unmodified Born-Oppenheimer potentials as input. On the theoretical side, we present a comparison between different simplified models of resonance scattering and the full numerical coupled-channels calculations. We have developed the resonant state model (RSM) to describe the resonant scattering of two ultracold atoms. This model is founded on resonant states, the natural (eigen) frequencies of the two-body system, and their non-trivial properties. Threshold effects are implicitly build into the RSM. The RSM can describe the effect of the continuum of scattering states, states which are neglected in the ABM, on the position and strength of a Feshbach resonance by only a few resonant states. Especially when a low-energy resonance is embedded in the continuum of scattering states, the effect of these states on the Feshbach resonance cannot be neglected. The RSM can be viewed as the natural generalization of the ABM. As the RSM can be based on just a few resonant states, it retains the computational simplicity of the ABM. Using the tunability of two-body interactions induced by a Feshbach resonance, we describe a crossover for a rotating Fermi gas between two strongly-correlated many-body states. We demonstrate that the correlation induced long-range interaction will shift the crossover with respect to the non-rotating case.