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Physics

Taming Ultracold Molecules

Susanne F. Yelin

Published Jun 3, 2016• 0 citations
Publisher

Abstract

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.

DOI
10.1103/physics.9.60

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Physical Review Letters•May 1, 2015•1 citation
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.
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.
This thesis presents the development of a toolbox for the coherent control of ultracold polar molecules. Such systems of molecules promise the creation of long-lived, highly dipolar quantum gases with applications spanning the fields of quantum state controlled chemistry, quantum information, quantum simulation, and precision measurement. However, the addition of vibrational and rotational degrees of freedom leads to molecular systems being significantly more complex than their widely used atomic counterparts. In this work we demonstrate full control of the quantum state down to the hyperfine level of an optically trapped sample of ultracold bosonic 87Rb133 Cs molecules, and exploit that control to begin an investigation into the collision processes which take place in an ultracold molecular gas. We create a sample of up to ∼ 4000 optically trapped molecules in their rovibronic and hyperfine ground state. We characterise the molecules by measuring their temperature, binding energy, and molecule-frame electric dipole moment. We perform spectroscopy of the first rotationally excited state with hyperfine state resolution using microwaves to determine accurate values of rotational and hyperfine coupling constants. We use coherent π pulses to perform complete transfer population between selected hyperfine levels of the ground, first-excited, and second-excited rotational states. We investigate the effect of the off-resonant light of our optical dipole trap on the rotational and hyperfine structure of the molecules. Through a combination of high-resolution microwave spectroscopy and parametric heating measurements, we characterise the polarisability of the 87Rb133Cs molecule. We demonstrate that coupling between neighbouring hyperfine states manifests in rich structure with many avoided crossings in any rotational state other than the ground state. This coupling may be tuned by rotating the polarisation of the linearly polarised trapping light. Finally, we study the lifetime of polar bosonic 87Rb133Cs molecules in our 3D optical dipole trap. We examine the lifetime of the molecules as a function of dipole trap intensity, magnetic field, and hyperfine and rotational state. Despite the chemical stability of the 87Rb133 Cs molecule, we observe lifetimes of ∼1 s corresponding to 2-body decay rates close to the universal limit.
Ultracold polar molecules possess a manifold of long-lived molecular rotational states, which can be coherently controlled using microwave fields and entangled by the long-range dipole-dipole interactions between molecules. The ability to control these features at the individual molecule level provides a rich toolbox with which to engineer quantum simulations of exotic materials or build a molecular quantum computer. Until recently, this level of single molecule control has eluded researchers due to the challenges inherent in taming the complex internal structure of molecules. In this thesis, we demonstrate full control over the internal quantum states and coherent interactions of individual NaCs molecules in optical tweezers. This platform is based on coherent assembly of ultracold Na and Cs atoms trapped and cooled in separate arrays, before being magnetoassociated at a Feshbach resonance to form weakly-bound molecules. Using high-resolution spectroscopy of electronically excited molecular states, we identify an efficient two-photon pathway to the rovibrational ground state of NaCs that we use to prepare an array of ground state molecules in tweezers. We demonstrate a "magic ellipticity'' technique to eliminate differential light shifts between two molecular rotational states and achieve coherence times of up to 250(40) ms for a superposition of those states. We then show that we can rearrange molecules in an array to eliminate defects and perform single-shot readout of multiple rotational states using controlled molecule dissociation and imaging of constituent atoms at high magnetic field. Finally, we coherently control the dipole-dipole interactions between two molecules, producing a Bell state with a fidelity of 94(3) % and demonstrating a universal entangling iSWAP gate for qubits encoded in molecular hyperfine states.
We demonstrate coherent control of the rotational and hyperfine state of ultracold, chemically stable 87Rb133Cs^{87}\mathrm{Rb}^{133}\mathrm{Cs}87Rb133Cs molecules with external microwave fields. We create a sample of $\ensuremath{\sim}2000$ molecules in the lowest hyperfine level of the rovibronic ground state N=0N=0N=0. We measure the transition frequencies to eight different hyperfine levels of the N=1N=1N=1 state at two magnetic fields $\ensuremath{\sim}23$ G apart. We determine accurate values of rotational and hyperfine coupling constants that agree well with previous calculations. We observe Rabi oscillations on each transition, allowing complete population transfer to a selected hyperfine level of N=1N=1N=1. Subsequent application of a second microwave pulse allows the transfer of molecules back to a different hyperfine level of N=0N=0N=0.
We report on the creation of an ultracold dipolar gas of fermionic 23Na40 K molecules in their absolute rovibrational and hyperfine ground state. Starting from weakly bound Feshbach molecules, we demonstrate hyperfine resolved two-photon transfer into the singlet X 1Σ+|v=0,J=0⟩ ground state, coherently bridging a binding energy difference of 0.65 eV via stimulated rapid adiabatic passage. The spin-polarized, nearly quantum degenerate molecular gas displays a lifetime longer than 2.5 s, highlighting NaK's stability against two-body chemical reactions. A homogeneous electric field is applied to induce a dipole moment of up to 0.8 D. With these advances, the exploration of many-body physics with strongly dipolar Fermi gases of 23Na40K molecules is within experimental reach.
We report on the creation of an ultracold dipolar gas of fermionic [superscript 23]Na[superscript 40]Kmolecules in their absolute rovibrational and hyperfine ground state. Starting from weakly bound Feshbach molecules, we demonstrate hyperfine resolved two-photon transfer into the singlet X[superscript 1]Σ[superscript +]|v = 0,J = 0⟩ ground state, coherently bridging a binding energy difference of 0.65 eV via stimulated rapid adiabatic passage. The spin-polarized, nearly quantum degenerate molecular gas displays a lifetime longer than 2.5 s, highlighting NaK’s stability against two-body chemical reactions. A homogeneous electric field is applied to induce a dipole moment of up to 0.8 D. With these advances, the exploration of many-body physics with strongly dipolar Fermi gases of [superscript 23]Na[superscript 40]K molecules is within experimental reach.