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Microscopic electronic structure tomography of Rydberg macrodimers

163   0   0.0 ( 0 )
 Added by Simon Hollerith
 Publication date 2020
  fields Physics
and research's language is English




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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 almost all of these challenges and enables unique access to the molecular frame. Here, we demonstrate the power of this approach and present first photoassociation studies for different molecular symmetries 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 characteristic dependencies allow for an electronic structure tomography of the molecular state. We additionally observe an orientation-dependent Zeeman shift and reveal a significant influence on it caused by the hyperfine interaction of the macrodimer state. Finally, we demonstrate controlled engineering of the electrostatic binding potential by opening a gap in the energetic vicinity of two crossing pair potentials.



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A microscopic understanding of molecules is essential for many fields of natural sciences but their tiny size hinders direct optical access to their constituents. Rydberg macrodimers - bound states of two highly-excited Rydberg atoms - feature bond lengths easily exceeding optical wavelengths. Here we report on the direct microscopic observation and detailed characterization of such macrodimers in a gas of ultracold atoms in an optical lattice. The size 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 resolve more than 50 vibrational resonances. Using our spatially resolved detection, we observe the macrodimers by correlated atom loss and demonstrate control of the molecular alignment by the choice of the vibrational state. Our results allow for precision testing of Rydberg interaction potentials and establish quantum gas microscopy as a powerful new tool for quantum chemistry.
Interaction between Rydberg atoms can significantly modify Rydberg excitation dynamics. Under a resonant driving field the Rydberg-Rydberg interaction in high-lying states can induce shifts in the atomic resonance such that a secondary Rydberg excitation becomes unlikely leading to the Rydberg blockade effect. In a related effect, off-resonant coupling of light to Rydberg states of atoms contributes to the Rydberg anti-blockade effect where the Rydberg interaction creates a resonant condition that promotes a secondary excitation in a Rydberg atomic gas. Here, we study the light-matter interaction and dynamics of off-resonant two-photon excitations and include two- and three-atom Rydberg interactions and their effect on excited state dynamics in an ensemble of cold atoms. In an experimentally-motivated regime, we find the optimal physical parameters such as Rabi frequencies, two-photon detuning, and pump duration to achieve significant enhancement in the probability of generating doubly-excited collective atomic states. This results in large auto-correlation values due to the Rydberg anti-blockade effect and makes this system a potential candidate for a high-purity two-photon Fock state source.
We have performed two-photon excitation via the 6P3/2 state to n=50-80 S or D Rydberg state in Bose-Einstein condensates of rubidium atoms. The Rydberg excitation was performed in a quartz cell, where electric fields generated by plates external to the cell created electric charges on the cell walls. Avoiding accumulation of the charges and realizing good control over the applied electric field was obtained when the fields were applied only for a short time, typically a few microseconds. Rydberg excitations of the Bose-Einstein condensates loaded into quasi one-dimensional traps and in optical lattices have been investigated. The results for condensates expanded to different sizes in the one-dimensional trap agree well with the intuitive picture of a chain of Rydberg excitations controlled by the dipole-dipole interaction. The optical lattice applied along the one-dimensional geometry produces localized, collective Rydberg excitations controlled by the nearest-neighbour blockade.
We report on the direct measurement in real space of the effect of the van der Waals forces between individual Rydberg atoms on their external degrees of freedom. Clusters of Rydberg atoms with inter-particle distances of around 5 {mu}m are created by first generating a small number of seed excitations in a magneto-optical trap, followed by off-resonant excitation that leads to a chain of facilitated excitation events. After a variable expansion time the Rydberg atoms are field ionized, and from the arrival time distributions the size of the Rydberg cluster after expansion is calculated. Our experimental results agree well with a numerical simulation of the van der Waals explosion.
163 - Peter Schauss 2017
Finite-range interacting spin models are the simplest models to study the effect of beyond nearest-neighbour interactions and access new effects caused by the range of the interactions. Recent experiments have reached the regime of dominant interactions in Ising quantum magnets via optical coupling of trapped neutral atoms to Rydberg states. This approach allows for the tunability of all relevant terms in an Ising Hamiltonian with $1/r^6$ interactions in a transverse and longitudinal field. This review summarizes the recent progress of these implementations in Rydberg lattices with site-resolved detection. The strong correlations in this quantum Ising model have been observed in several experiments up to the point of crystallization. In systems with a diameter small compared to the Rydberg blockade radius, the number of excitations is maximally one in the so-called superatom regime.
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