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arXiv:1803.04159 · Physical Review Letters

Ultracold Rare-Earth Magnetic Atoms with an Electric Dipole Moment

Maxence Lepers, Hui Li, Jean-François Wyart, Goulven Quéméner, Olivier Dulieu

Published Aug 8, 2018• 15 citations
arXivHTMLPDF

Abstract

We propose a new method to produce an electric and magnetic dipolar gas of ultracold dysprosium atoms. The pair of nearly degenerate energy levels of opposite parity, at 17513.33 cm^{-1} with electronic angular momentum J=10, and at 17514.50 cm^{-1} with J=9, can be mixed with an external electric field, thus inducing an electric dipole moment in the laboratory frame. For field amplitudes relevant to current-day experiments, i.e., an electric field of 5 kV/cm, we predict a large magnetic dipole moment up to 13 Bohr magnetons, and sizeable electric dipole moment up to 0.22 D. When a magnetic field is present, we show that the induced electric dipole moment is strongly dependent on the angle between the fields. The lifetime of the field-mixed levels is found in the millisecond range, thus allowing for suitable experimental detection and manipulation.

DOI
10.1103/physrevlett.121.063201

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We propose a new method to produce an electric and magnetic dipolar gas of ultracold dysprosium atoms. The pair of nearly degenerate energy levels of opposite parity, at 17513.33 cm^{-1} with electronic angular momentum J=10, and at 17514.50 cm^{-1} with J=9, can be mixed with an external electric field, thus inducing an electric dipole moment in the laboratory frame. For field amplitudes relevant to current-day experiments, i.e., an electric field of 5 kV/cm, we predict a large magnetic dipole moment up to 13 Bohr magnetons, and sizeable electric dipole moment up to 0.22 D. When a magnetic field is present, we show that the induced electric dipole moment is strongly dependent on the angle between the fields. The lifetime of the field-mixed levels is found in the millisecond range, thus allowing for suitable experimental detection and manipulation.
We experimentally show that an electric dipole moment of more than 1 Debye can be induced in the dysprosium (Dy) atom, in a long-lived state that is about 17 513 cm − 1 above the ground state. This metastable state is part of a strongly coupled opposite-parity doublet. Using optically detected microwave spectroscopy in an atomic beam, we determine the approximately 1.12 cm − 1 doublet spacing for the five stable bosonic isotopes of Dy with kilohertz-level accuracy. From the shift of the microwave transition frequency in low electric fields (below 150 V/cm) and from optical spectra in high electric fields (up to 150 kV/cm), a reduced transition dipole moment of 7.65 ± 0.05 Debye between the doublet states is extracted. In high electric fields the doublet interacts with a third state at 17 727 cm − 1 that connects to the ground state via an electric-dipole transition. The three-state Stark interaction enables preparation of Dy atoms in the metastable state via single-photon excitation from the ground state. Our work experimentally validates predicted characteristics of the opposite-parity doublet and provides an effective route to the first doubly polar quantum gas of atoms.
Doubly polar molecules, possessing an electric dipole moment and a magnetic dipole moment, can strongly couple to both an external electric field and a magnetic field, providing unique opportunities to exert full control of the system quantum state at ultracold temperatures. We propose a method for creating a purely long-range doubly polar homonuclear molecule from a pair of strongly magnetic lanthanide atoms, one atom being in its ground level and the other in a superposition of quasidegenerate opposite-parity excited levels [Phys. Rev. Lett. 121, 063201 (2018)]. The electric dipole moment is induced by coupling the excited levels with an external electric field. We derive the general expression of the long-range, Stark, and Zeeman interaction energies in the properly symmetrized and fully-coupled basis describing the diatomic complex. Taking the example of holmium, our calculations predict a few shallow long-range wells in the potential energy curves that support vibrational levels accessible by direct photoassociation from pairs of ground-level atoms.
We report on the creation of bosonic NaCs molecules in their absolute rovibrational ground state via stimulated Raman adiabatic passage. We create ultracold gases with up to 22 000 dipolar NaCs molecules at a temperature of 300(50) nK and a peak density of 1.0(4)×10^{12} cm^{-3}. We demonstrate comprehensive quantum state control by preparing the molecules in a specific electronic, vibrational, rotational, and hyperfine state. We measure the ground state ac polarizability at 1064 nm along with the two-body loss rate, which we find to be universal. Employing the tunability and strength of the permanent electric dipole moment of NaCs, we induce dipole moments of up to 2.6 D at a dc electric field of 2.1(2) kV/cm and demonstrate strong microwave coupling between the two lowest rotational states with a Rabi frequency of 2π×45 MHz. A large electric dipole moment, accessible at relatively small electric fields, makes ultracold gases of NaCs molecules well suited for the exploration of strongly interacting phases of dipolar quantum matter.
In this thesis, I present the study of the laser trapping and cooling of a Dysprosium atomic gas. This latter belong to the lanthanide family, it exhibits a large angular momentum in its electronic ground state, making it a suitable candidate for investigating dipolar quantum gases. These systems present a major interest as they can lead to the observation of novel quantum phenomena thanks to the anisotropic and long-range character of the interaction between magnetic dipoles. Moreover, Dysprosium has a rich electronic structure offering the possibility to implement strong light-spin coupling with a reduced heating with respect to alkali species, which paves the way toward the realization of synthetic gauge fields.In this work, I present the experimental investigation of different interaction mechanisms occurring in an ultracold gas of Dysprosium, ranging from light-assisted collisions to dipolar relaxation and evaporative cooling. I expose also the experimental realization of an effective magnetic field, using spin-dependent light-shift, allowing optical control over atomic interactions by means of Feshbach resonances.
The nature of the interaction between ultracold atoms with a large orbital and spin angular momentum has attracted considerable attention. It was suggested that such interactions can lead to the realization of exotic states of highly correlated matter. Here, we report on a theoretical study of the competing anisotropic dispersion, magnetic dipole-dipole, and electric quadrupole-quadrupole forces between two dysprosium atoms. Each dysprosium atom has an orbital angular momentum of L = 6 and a magnetic moment of μ = 10 μ(B). We show that the dispersion coefficients of the ground state adiabatic potentials lie between 1865 a.u. and 1890 a.u., creating a non-negligible anisotropy with a spread of 25 a.u. and that the electric quadrupole-quadrupole interaction is weak compared to the other interactions. We also find that for interatomic separations R < 50a(0) both the anisotropic dispersion and magnetic dipole-dipole potential are larger than the atomic Zeeman splittings for external magnetic fields of order 10 G to 100 G. At these separations the atomic angular momentum can be reoriented. We finish by describing two scattering models for these inelastic m-changing collisions. A universal scattering theory is used to model loss due to the anisotropy in the dispersion and a Born approximation is used to model losses from the magnetic dipole-dipole interaction for the (164)Dy isotope. These models find loss rates that are of the same order of magnitude as the experimental value.
Obtaining an accurate value of the electric dipole moment μ is essential in the fields of laser application technologies. A direct way of measuring the electric dipole moment μ is to observe the Rabi-oscillation which manifests itself in the coherent photo-excitation behavior of atoms. In the case of the elements which have large angular momenta, identifying the Rabi-oscillation in their excitation behavior becomes rather difficult. We proposed an accurate and straightforward method of determining the electric-dipole moment μ between multifold degenerate levels. The point is to remove the degeneracy by applying an external magnetic field with the aid of the Zeeman effect and, then, to realize a degeneration free coherent excitation. As a result, we can observe the Rabi-oscillations explicitly in the excitation vs. laser-fluence curves. The present method provides a reliable basis of experimental determination of μ. As an example, we applied the present method to a transition to 0–17,362 cm−1 level in uranium and obtained the value μ=0.86±0.06 (Debye).