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Evidence for association of triatomic molecule in ultracold $^{23}$Na$^{40}$K and $^{40}$K mixture

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 Added by Bo Zhao
 Publication date 2021
  fields Physics
and research's language is English




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Ultracold assembly of diatomic molecules has enabled great advances in controlled chemistry, ultracold chemical physics, and quantum simulation with molecules. Extending the ultracold association to triatomic molecules will offer many new research opportunities and challenges in these fields. A possible approach is to form triatomic molecules in the ultracold atom and diatomic molecule mixture by employing the Feshbach resonance between them. Although the ultracold atom-diatomic-molecule Feshbach resonances have been observed recently, utilizing these resonances to form triatomic molecules remains challenging. Here we report on the evidence of the association of triatomic molecules near the Feshbach resonances between $^{23}$Na$^{40}$K molecules in the rovibrational ground state and $^{40}$K atoms. We apply a radio-frequency pulse to drive the free-bound transition and monitor the loss of $^{23}$Na$^{40}$K molecules. The association of triatomic molecules manifests itself as an additional loss feature in the radio-frequency spectra, which can be distinguished from the atomic loss feature.The binding energy of triatomic molecule is estimated from the measurement. Our work is helpful to understand the complex ultracold atom-molecule Feshbach resonance and may open up an avenue towards the preparation and control of ultracold triatomic molecules.



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We present measurements of more than 80 magnetic Feshbach resonances in collisions of ultracold $^{23}$Na$^{40}$K with $^{40}$K. We assign quantum numbers to a group of low-field resonances and show that they are due to long-range states of the triatomic complex in which the quantum numbers of the separated atom and molecule are approximately preserved. The resonant states are not members of chaotic bath of short-range states. Similar resonances are expected to be a common feature of alkali-metal diatom + atom systems.
We demonstrate coherent microwave control of rotational and hyperfine states of trapped, ultracold, and chemically stable $^{23}$Na$^{40}$K molecules. Starting with all molecules in the absolute rovibrational and hyperfine ground state, we study rotational transitions in combined magnetic and electric fields and explain the rich hyperfine structure. Following the transfer of the entire molecular ensemble into a single hyperfine level of the first rotationally excited state, $J{=}1$, we observe collisional lifetimes of more than $3, rm s$, comparable to those in the rovibrational ground state, $J{=}0$. Long-lived ensembles and full quantum state control are prerequisites for the use of ultracold molecules in quantum simulation, precision measurements and quantum information processing.
Coherence, the stability of the relative phase between quantum states, lies at the heart of quantum mechanics. Applications such as precision measurement, interferometry, and quantum computation are enabled by physical systems that have quantum states with robust coherence. With the creation of molecular ensembles at sub-$mu$K temperatures, diatomic molecules have become a novel system under full quantum control. Here, we report on the observation of stable coherence between a pair of nuclear spin states of ultracold fermionic NaK molecules in the singlet rovibrational ground state. Employing microwave fields, we perform Ramsey spectroscopy and observe coherence times on the scale of one second. This work opens the door for the exploration of single molecules as a versatile quantum memory. Switchable long-range interactions between dipolar molecules can further enable two-qubit gates, allowing quantum storage and processing in the same physical system. Within the observed coherence time, $10^4$ one- and two-qubit gate operations will be feasible.
Stimulated Raman adiabatic passage (STIRAP) allows to efficiently transferring the populations between two discrete quantum states and has been used to prepare molecules in their rovibrational ground state. In realistic molecules, a well-resolved intermediate state is usually selected to implement the resonant STIRAP. Due to the complex molecular level structures, the detuned STIRAP always coexists with the resonant STIRAP and may cause unexpected interference phenomenon. However, it is generally accepted that the detuned STIRAP can be neglected if compared with the resonant STIRAP. Here we report on the first observation of interference between the resonant and detuned STIRAP in the adiabatic creation of $^{23}$Na$^{40}$K ground-state molecules. The interference is identified by observing that the number of Feshbach molecules after a round-trip STIRAP oscillates as a function of the hold time, with a visibility of about 90%. This occurs even if the intermediate excited states are well resolved, and the single-photon detuning of the detuned STIRAP is about one order of magnitude larger than the linewidth of the excited state and the Rabi frequencies of the STIRAP lasers. Moreover, the observed interference indicates that if more than one hyperfine level of the ground state is populated, the STIRAP prepares a coherent superposition state among them, but not an incoherent mixed state. Further, the purity of the hyperfine levels of the created ground state can be quantitatively determined by the visibility of the oscillation.
We demonstrate a versatile, rotational-state dependent trapping scheme for the ground and first excited rotational states of $^{23}$Na$^{40}$K molecules. Close to the rotational manifold of a narrow electronic transition, we determine tune-out frequencies where the polarizability of one state vanishes while the other remains finite, and a magic frequency where both states experience equal polarizability. The proximity of these frequencies of only 10 GHz allows for dynamic switching between different trap configurations in a single experiment, while still maintaining sufficiently low scattering rates.
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