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arXiv:0905.4489 · Physical Review A

Manipulating ultracold polar molecules with microwave radiation: The influence of hyperfine structure

J. Aldegunde, Hong Ran, Jeremy M. Hutson

Published Oct 15, 2009• 47 citations
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Abstract

We calculate the microwave spectra of ultracold $^{40}\text{K}^{87}\text{R}\text{b}$ alkali-metal dimers, including hyperfine interactions and in the presence of electric and magnetic fields. We show that microwave transitions may be used to transfer molecules between different hyperfine states, but only because of the presence of nuclear quadrupole interactions. Hyperfine splittings may also complicate the use of ultracold molecules for quantum computing. The spectrum of molecules oriented in electric fields may be simplified dramatically by applying a simultaneous magnetic field.

DOI
10.1103/physreva.80.043410

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We calculate the microwave spectra of ultracold 40K87Rb^{40}\text{K}^{87}\text{R}\text{b}40K87Rb alkali-metal dimers, including hyperfine interactions and in the presence of electric and magnetic fields. We show that microwave transitions may be used to transfer molecules between different hyperfine states, but only because of the presence of nuclear quadrupole interactions. Hyperfine splittings may also complicate the use of ultracold molecules for quantum computing. The spectrum of molecules oriented in electric fields may be simplified dramatically by applying a simultaneous magnetic field.
We investigate the microwave spectra of ultracold alkali metal dimers in magnetic, electric and combined fields taking into account the hyperfine structure due to nuclear spins. We consider the molecules 41 K 87 Rb and 7 Li 133 Cs, which are the targets of current experiments, and demonstrate two extremes of large and small nuclear quadrupole couplings. We calculate the frequencies and intensities of transitions that may be used to transfer ultracold molecules between hyperfine states in a magnetic field, employing different polarizations of microwave radiation. In an electric field, the hyperfine levels display narrow avoided crossings at specific fields that we explain in terms of molecular alignment. The hyperfine splittings that arise in electric fields may hinder individual addressing in schemes that use ultracold molecules in quantum computation, but the structure of the spectra is suppressed in combined fields.
We investigate the energy levels of heteronuclear alkali-metal dimers in levels correlating with the lowest rotational level of the ground electronic state, which are important in efforts to produce ground-state ultracold molecules. We use density-functional theory to calculate nuclear quadrupole and magnetic coupling constants for KRb and RbCs and explore the hyperfine structure in the presence of electric and magnetic fields. For nonrotating states, the zero-field splittings are dominated by the electron-mediated part of the nuclear spin-spin coupling. They are a few kilohertz for KRb isotopologs and a few tens of kilohertz for RbCs isotopologs.
Ultracold molecules are expected to find applications in cold chemistry, quantum phases, precision measurements and quantum information. In this thesis three novel applications of cold molecules are studied. First the thesis presents a general method for coherent control of collisions between non-identical particles. It is shown that by preparing two alkali-metal atoms in a superposition of hyperfine states, the elastic-to-inelastic cross section ratio can be manipulated at ultracold temperatures by tuning laser parameters in the presence of a magnetic field. The static field is needed to induce quantum interference between scattering states. Extensions of this scheme for ultracold molecular reactive scattering are discussed. Second, the thesis describes rotational excitons and polarons in molecular ensembles trapped in optical lattices. Rotational excitons can be manipulated using static electric and magnetic fields. For a one-dimensional molecular array with substitutional impurities any localized exciton state can be delocalized by applying a suitable electric field. The electric field induces correlations between diagonal and off-diagonal disorder. It is also shown that the translational motion of polar molecules in an optical lattice can lead to phonons. The lattice dynamics and the phonon spectrum depend on the strength and orientation of a static electric field. An array of polar molecules in an optical lattice can be described by generalized polaron model with tunable parameters including diagonal and off-diagonal exciton-phonon interactions. It is shown that in a strong electric field the system is described by a generalized Holstein model, and at weak electric fields by the Su-Schrieffer-Heeger (SSH) model. The possibility of observing a sharp polaron transition in the SSH model using polar alkali-metal dimers is discussed. Finally, the thesis presents a method to generate entanglement of polar molecules using strong off-resonant laser pulses. Bipartite entanglement between alkali-metal dimers separated by hundreds of nanometers can be generated. Maximally entangled states can be prepared by tuning the pulse intensity and duration. A scheme is proposed to observe the violation of Bell’s inequality based on molecular orientation correlation measurements. It is shown that using a combination of microwave and off-resonant optical pulses, arbitrary tripartite and many-particle states can be prepared.
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 lifetimes of more than 3 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.
By leveraging the hyperfine interaction between the rotational and nuclear spin degrees of freedom, we demonstrate extensive magnetic control over the electric dipole moments, electric dipolar interactions, and ac Stark shifts of ground-state alkali-dimer molecules such as KRb(X^{1}Σ^{+}). The control is enabled by narrow avoided crossings and the highly ergodic character of molecular eigenstates at low magnetic fields, offering a general and robust way of continuously tuning the intermolecular electric dipolar interaction for applications in quantum simulation, quantum sensing, and dipolar spinor physics.
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 ¼ 1, we observe lifetimes of more than 3 s, comparable to those in the rovibrational ground state, J ¼ 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.