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arXiv:2506.12329 · Nature Communications

Multi-state detection and spatial addressing in a microscope for ultracold molecules

Jonathan M. Mortlock, Adarsh P. Raghuram, Benjamin Maddox, Philip D. Gregory, Simon L. Cornish

Published Dec 9, 2025• 2 citations
arXivHTMLPDF

Abstract

Abstract Precise measurement of the particle number, spatial distribution and internal state is fundamental to all proposed experiments with ultracold molecules both in bulk gases and optical lattices. Here, we demonstrate in-situ detection of individual molecules in a bulk sample of 87 Rb 133 Cs molecules. Extending techniques from atomic quantum gas microscopy, we pin the molecules in a deep two-dimensional optical lattice and, following dissociation, collect fluorescence from the constituent atoms using a high-numerical-aperture objective. This enables detection of individual molecules up to the resolution of the sub-micron lattice spacing. Our approach provides direct access to the density distribution of small samples of molecules, allowing us to obtain precise measurements of density-dependent collisional losses. Further, by mapping two internal states of the molecule to different atomic species, we demonstrate simultaneous detection of the position and rotational state of individual molecules. Finally, we implement local addressing of the sample using a focused beam to induce a spatially-dependent light shift on the rotational transitions of the molecules.

DOI
10.1038/s41467-025-67212-7

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•Jan 1, 2011•11 citations
Abstract Precise measurement of the particle number, spatial distribution and internal state is fundamental to all proposed experiments with ultracold molecules both in bulk gases and optical lattices. Here, we demonstrate in-situ detection of individual molecules in a bulk sample of 87 Rb 133 Cs molecules. Extending techniques from atomic quantum gas microscopy, we pin the molecules in a deep two-dimensional optical lattice and, following dissociation, collect fluorescence from the constituent atoms using a high-numerical-aperture objective. This enables detection of individual molecules up to the resolution of the sub-micron lattice spacing. Our approach provides direct access to the density distribution of small samples of molecules, allowing us to obtain precise measurements of density-dependent collisional losses. Further, by mapping two internal states of the molecule to different atomic species, we demonstrate simultaneous detection of the position and rotational state of individual molecules. Finally, we implement local addressing of the sample using a focused beam to induce a spatially-dependent light shift on the rotational transitions of the molecules.
Our knowledge on ultracold quantum gases is strongly influenced by our ability to probe these objects. In situ imaging combined with single atom sensitivity is an especially appealing scenario as it can provide direct information on the structure and the correlations of such systems. For a precise characterization a high spatial resolution is mandatory. In particular, the perspective to study quantum gases in optical lattices makes a resolution well below one micrometer highly desirable. Here, we report on a novel microscopy technique which is based on scanning electron microscopy and allows for the detection of single atoms inside a quantum gas with a spatial resolution of better than 150 nm. Imaging a Bose-Einstein condensate in a one-dimensional optical lattice with 600 nm period we demonstrate single site addressability in a sub-um optical lattice. The technique offers exciting possibilities for the preparation, manipulation and analysis of quantum gases.
Abstract Imaging is central to gaining microscopic insight into physical systems, and new microscopy methods have always led to the discovery of new phenomena and a deeper understanding of them. Ultracold atoms in optical lattices provide a quantum simulation platform, featuring a variety of advanced detection tools including direct optical imaging while pinning the atoms in the lattice1,2. However, this approach suffers from the diffraction limit, high optical density and small depth of focus, limiting it to two-dimensional (2D) systems. Here we introduce an imaging approach where matter wave optics magnifies the density distribution before optical imaging, allowing 2D sub-lattice-spacing resolution in three-dimensional (3D) systems. By combining the site-resolved imaging with magnetic resonance techniques for local addressing of individual lattice sites, we demonstrate full accessibility to 2D local information and manipulation in 3D systems. We employ the high-resolution images for precision thermodynamics of Bose–Einstein condensates in optical lattices as well as studies of thermalization dynamics driven by thermal hopping. The sub-lattice resolution is demonstrated via quench dynamics within the lattice sites. The method opens the path for spatially resolved studies of new quantum many-body regimes, including exotic lattice geometries or sub-wavelength lattices3–6, and paves the way for single-atom-resolved imaging of atomic species, where efficient laser cooling or deep optical traps are not available, but which substantially enrich the toolbox of quantum simulation of many-body systems.
We demonstrate a method to determine the position of single atoms in a three-dimensional optical lattice. Atoms are sparsely loaded from a far-off-resonant optical tweezer into a few vertical planes of a cubic optical lattice positioned near a high-resolution microscope objective. In a single realization of the experiment, we pin the atoms in deep lattices and then acquire multiple fluorescence images with single-site resolution. The objective is translated between images, bringing different vertical planes of the lattice into focus. The applicability of our method is assessed using simulated fluorescence images where the atomic filling fraction in the lattice is varied. This opens up the possibility of extending the domain of quantum simulation using quantum gas microscopes from two to three dimensions.
Quantum gas microscopy provides single-shot access to many-body configurations, yet has so far relied on pinning atoms to a discrete lattice during fluorescence readout. Here, we realize ultrafast atom-resolved fluorescence microscopy of an ultracold 162^{162}162Dy gas directly in free space, with all external confinement removed during imaging. Exploiting the large mass and broad optical transition of dysprosium together with a high numerical aperture in-vacuum objective, we detect single atoms within 4 μs4\,μ\mathrm{s}4μs while maintaining an effective point-spread function with a full width at half maximum of 254.8(3) nm254.8(3)\,\mathrm{nm}254.8(3)nm. We achieve a single-atom conditional classification fidelity of 99.72(3)%99.72(3)\%99.72(3)% for identified fluorescence candidates. We use the measured single-atom response to construct a statistical configuration-inference model that recovers atomic positions and multiplicities, coming from overlapping atoms, directly from single fluorescence snapshots. We further benchmark our reconstruction algorithm through end-to-end Monte Carlo simulations with known ground-truth atomic configurations, obtaining a reconstruction fidelity of 98.7%98.7\%98.7%. Our approach, applicable to a wide variety of atomic species, extends quantum gas microscopy beyond predefined detection lattices, enabling atom-resolved measurements of counting statistics and higher-order spatial correlations directly on the intrinsic length scales of continuum many-body systems.
We propose a new technique for the detection of single atoms in ultracold quantum gases. The technique is based on scanning electron microscopy and employs the electron impact ionization of trapped atoms with a focused electron probe. Subsequent detection of the resulting ions allows for the reconstruction of the atom's position. This technique is expected to achieve a much better spatial resolution compared to any optical detection method. In combination with the sensitivity to single atoms, it makes new in situ measurements of atomic correlations possible. The detection principle is also well suited for the addressing of individual sites in optical lattices.
This thesis reports on new experimental techniques for the study of strongly correlated states of ultracold atoms in optical lattices. We used a high numerical aperture imaging system to probe 87Rb atoms in a two-dimensional lattice with single-site resolution. Fluorescence imaging allows to detect single atoms with a large signal to noise ratio and to reconstruct the atom distribution on the lattice. We applied this new technique to a two-dimensional Mott insulator and directly observed number squeezing and the emerging shell structure. A comparison of the radial density and variance distributions to theory provides a precise in situ temperature and entropy measurement from single images. We find entropies around the critical value for quantum magnetism. In a second series of experiments, we demonstrated two-dimensional single-site spin control in the optical lattice. The differential light shift of a tightly focused laser beam shifts selected atoms into resonance with a microwave field driving a spin flip. In this way, we reach sub-diffraction limited spatial resolution well below the lattice spacing. Starting from a Mott insulator with unity filling we were able to create arbitrary spin patterns. We used this ability to prepare atom distributions to study one-dimensional single-particle tunneling dynamics in a lattice. By discriminating the dynamics of the ground state and of the first excited band, we find that our addressing scheme leaves most atoms in the vibrational ground state. Moreover, we studied coherent light scattering from the atoms in the optical lattice and found diffraction maxima in the far-field. We showed that an antiferromagnetic order leads to additional diffraction peaks which can be used to detect this order also when single-site resolution is not available. The new techniques described in this thesis open the path to a wide range of novel applications from quantum dynamics of spin impurities, entropy transport, implementation of novel cooling schemes, and engineering of quantum many-body phases to quantum information processing.