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arXiv:2401.05129 · PRX Quantum

Rydberg Molecules Bound by Strong Light Fields

Simon Hollerith, Valentin Walther, Kritsana Srakaew, David Wei, Daniel Adler, Suchita Agrawal, Pascal Weckesser, Immanuel Bloch, Johannes Zeiher

Published Aug 16, 2024• 7 citations
arXivHTMLPDF

Abstract

The coupling of an isolated quantum state to a continuum is typically associated with decoherence and decreased lifetime. For coupling rates larger than the bandwidth of the associated continuum, decoherence can be mitigated, and new stable eigenstates emerge. Here, we laser-couple diatomic molecules of highly excited Rydberg atoms, so-called Rydberg macrodimers, to a continuum of free motional states. Enabled by their small vibrational eigenfrequencies, we achieve the regime of strong continuum couplings and observe the appearance of new resonances. We explain the observed spectroscopic features as molecular states emerging in the presence of the light field using a Fano model. For atoms arranged on a lattice, we predict the strong continuum coupling to even stabilize triatomic molecules and find the first signatures of these by observing three-atom loss correlations using quantum gas microscopy. Our results present a mechanism to control decoherence and bind polyatomic molecules using strong light-matter interactions. Published by the American Physical Society 2024

DOI
10.1103/prxquantum.5.030335

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•Jan 1, 2014•0 citations
The coupling of an isolated quantum state to a continuum is typically associated with decoherence and decreased lifetime. For coupling rates larger than the bandwidth of the associated continuum, decoherence can be mitigated, and new stable eigenstates emerge. Here, we laser-couple diatomic molecules of highly excited Rydberg atoms, so-called Rydberg macrodimers, to a continuum of free motional states. Enabled by their small vibrational eigenfrequencies, we achieve the regime of strong continuum couplings and observe the appearance of new resonances. We explain the observed spectroscopic features as molecular states emerging in the presence of the light field using a Fano model. For atoms arranged on a lattice, we predict the strong continuum coupling to even stabilize triatomic molecules and find the first signatures of these by observing three-atom loss correlations using quantum gas microscopy. Our results present a mechanism to control decoherence and bind polyatomic molecules using strong light-matter interactions. Published by the American Physical Society 2024
Controlling molecular binding at the level of single atoms is one of the holy grails of quantum chemistry. Rydberg macrodimers─bound states between highly excited Rydberg atoms─provide a novel perspective in this direction. Resulting from binding potentials formed by the strong, long-range interactions of Rydberg states, Rydberg macrodimers feature bond lengths in the micrometer regime, exceeding those of conventional molecules by orders of magnitude. Using single-atom control in quantum gas microscopes, the unique properties of these exotic states can be studied with unprecedented control, including the response to magnetic fields or the polarization of light in their photoassociation. The high accuracy achieved in spectroscopic studies of macrodimers makes them an ideal testbed to benchmark Rydberg interactions, with direct relevance to quantum computing and information protocols where these are employed. This review provides a historic overview and summarizes the recent findings in the field of Rydberg macrodimers. Furthermore, it presents new data on interactions between macrodimers, leading to a phenomenon analogous to Rydberg blockade at the level of molecules, opening the path toward studying many-body systems of ultralong-range Rydberg molecules.
The subnanoscale size of typical diatomic molecules hinders direct optical access to their constituents. Rydberg macrodimers-bound states of two highly excited Rydberg atoms-feature interatomic distances easily exceeding optical wavelengths. We report the direct microscopic observation and detailed characterization of such molecules in a gas of ultracold rubidium atoms in an optical lattice. The bond length of about 0.7 micrometers, comparable to the size of small bacteria, matches the diagonal distance of the lattice. By exciting pairs in the initial two-dimensional atom array, we resolved more than 50 vibrational resonances. Using our spatially resolved detection, we observed the macrodimers by correlated atom loss and demonstrated control of the molecular alignment by the choice of the vibrational state. Our results allow for rigorous testing of Rydberg interaction potentials and highlight the potential of quantum gas microscopy for molecular physics.
Precise control and study of molecules is challenging due to the variety of internal degrees of freedom and local coordinates that are typically not controlled in an experiment.Employing quantum gas microscopy to position and resolve the atoms in Rydberg macrodimer states solves most of these challenges and enables unique access to the molecular frame.Here, we demonstrate this approach and present photoassociation studies in which the molecular orientation relative to an applied magnetic field, the polarization of the excitation light, and the initial atomic state are fully controlled.The observed dependencies allow for an electronic structure tomography of the molecular state.We additionally observe an orientation-dependent Zeeman shift, and we reveal a significant influence on it caused by the hyperfine interaction of the macrodimer state.Finally, we demonstrate control over the electrostatic binding potential by engineering a gap between two crossing pair potentials.Our results establish macrodimers as the most sensitive tool to benchmark Rydberg interaction potentials, and they open new perspectives for improving Rydberg dressing schemes.
Long-range metastable molecules consisting of two cesium atoms in high Rydberg states have been observed in an ultracold gas. A sequential three-photon two-color photoassociation scheme is employed to form these molecules in states, which correlate to np(n+1)s dissociation asymptotes. Spectral signatures of bound molecular states are clearly resolved at the positions of avoided crossings between long-range van der Waals potential curves. The experimental results are in agreement with simulations based on a detailed model of the long-range multipole-multipole interactions of Rydberg-atom pair states. We show that a full model is required to accurately predict the occurrence of bound Rydberg macrodimers. The macrodimers are distinguished from repulsive molecular states by their behavior with respect to spontaneous ionization and possible decay channels are discussed.
We present a theoretical study of interactions between Rydberg macrodimers, molecular bound states of Rydberg atoms, and the largest known neutral homonuclear diatomic molecules. Accounting for the large number of molecular interaction channels from four interacting Rydberg atoms, we show that macrodimer-macrodimer interactions are anisotropic and similar in strength and range to atomic-state Rydberg interactions. Our analysis reveals the presence of two-atom, three-atom, and four-atom contributions in the bimolecular system, and elucidates how these interactions are rooted in the underlying atomic Rydberg-state couplings. Our calculations of the excitation blockade between macrodimers are in reasonable agreement with experimentally observed signals, and pave the way for the exploration of optically controlled collective quantum dynamics in molecular systems.
This thesis investigates new phenomena that arise when light is strongly coupled to an interacting atomic gas. For this, a new apparatus has been built which allows to create ultracold and dense atomic samples and to detect individual atoms in high-lying atomic states, so-called Rydberg atoms. Strong light-matter coupling is achieved using the collective coupling of the atomic cloud to the light field under conditions of electromagnetically induced transparency (EIT). In experiments on EIT involving non-interacting Rydberg states, we characterize the light-matter coupling and demonstrate the first combined optical and matter based probing of EIT. By coupling to strongly-interacting Rydberg states, we investigate the effect of interactions which we observe as a strong nonlinear optical \nresponse of the atomic gas as well as in the emergence of strong correlations between the hybrid quasiparticles associated with the strong light-matter coupling. We employ the nonlinear response of the atomic cloud to image Rydberg atoms immersed in the atomic cloud. In a theoretical proposal, we show that this novel imaging technique allows to investigate many-body Rydberg states with single particle sensitivity. Using the proposed imaging method, we demonstrate imaging of small numbers of Rydberg atoms with high time-resolution in single shot experiments. In experiments exploiting the dipolar exchange interaction between Rydberg atoms, we employ the new imaging technique to follow dipole-mediated transport of Rydberg excitations through the cloud. The transport dynamics is determined by the continuous spatial projection of the electronic quantum state under observation and features an emergent spatial scale of micrometer size induced by Rydberg-Rydberg interactions.