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arXiv:2002.11538 · Nature Communications

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

Baruch Margulis, Julia Narevicius, Edvardas Narevicius

Published Jul 16, 2020• 20 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1038/s41467-020-17393-0

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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.
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.
Rydberg atoms occupy a central role in quantum science; their loosely bound outer electron gives rise to properties that enable quantum information processing1 or the formation of exotic molecular bonds2. Beyond these roles, they have been proposed as a neutral platform for the observation of quantum effects in collisions and reactions of the ionic core with neutral particles3, 4, a long-standing goal of ion-based chemistry and physics. However, all of the experimental results so far could be explained using a classical description of the internuclear motion5. Here we demonstrate cold collisions inside a Rydberg helium atom, achieved by merging helium Rydberg and ground-state helium beams and imaging individual scattering events. We resolve the fully quantum-coherent motion and observe matter-wave diffraction and tunnelling-driven shape resonances down to collision energies of 90 mK. In the case of identical helium nuclei, we demonstrate a new regime of identical-particle Mott interference6, where quantum statistics begin to govern the total scattering cross section. For distinct isotopes, we show the breakdown of the Born-Oppenheimer approximation and benchmark parameter-free, state-of-the-art theory. We directly measure the helium isotope ionization-energy difference to be 15.0 +/- 0.1 K. Our experiments establish Rydberg atoms as a platform for the direct observation of quantum dynamics with a general class of ions, atoms and molecules.
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.
Penning ionization reactions in merged beams with precisely controlled collision energies have been shown to accurately probe quantum mechanical effects in reactive collisions. A complete microscopic understanding of the reaction is, however, faced with two major challenges-the highly excited character of the reaction's entrance channel and the limited precision of even the best state-of-the-art ab initio potential energy surfaces. Here, we suggest photoassociation spectroscopy as a tool to identify the character of orbiting resonances in the entrance channel and probe the ionization width as a function of interparticle separation. We introduce the basic concept, using the example of metastable helium and argon, and discuss the general conditions under which this type of spectroscopy will be successful.
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. 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.