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arXiv:1108.4871 · Physical Review A

Microwave state transfer and adiabatic dynamics of magnetically trapped polar molecules

Benjamin Stuhl, Mark Yeo, Brian C. Sawyer, Matthew T. Hummon, Jun Ye

Published Mar 30, 2012• 20 citations
arXivHTMLPDF

Abstract

Cold and ultracold polar molecules with nonzero electronic angular momenta are of great interest for studies in quantum chemistry and control, investigations of novel quantum systems, and precision measurement. However, in mixed electric and magnetic fields, these molecules are generically subject to a large set of avoided crossings among their Zeeman sublevels; in magnetic traps, these crossings lead to distorted potentials and trap loss from electric bias fields. We have characterized these crossings in OH by microwave-transferring trapped OH molecules from the upper $|f;\phantom{\rule{0.16em}{0ex}}M=+\frac{3}{2}\ensuremath{\rangle}$ parity state to the lower $|e;\phantom{\rule{0.16em}{0ex}}+\frac{3}{2}\ensuremath{\rangle}$ state and observing their trap dynamics under an applied electric bias field. Our observations are very well fit by a simple Landau-Zener model, yielding insight to the rich spectra and dynamics of polar radicals in mixed external fields.

DOI
10.1103/physreva.85.033427

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Cold and ultracold polar molecules with nonzero electronic angular momenta are of great interest for studies in quantum chemistry and control, investigations of novel quantum systems, and precision measurement. However, in mixed electric and magnetic fields, these molecules are generically subject to a large set of avoided crossings among their Zeeman sublevels; in magnetic traps, these crossings lead to distorted potentials and trap loss from electric bias fields. We have characterized these crossings in OH by microwave-transferring trapped OH molecules from the upper ∣f;M=+32\ensuremath⟩|f;\phantom{\rule{0.16em}{0ex}}M=+\frac{3}{2}\ensuremath{\rangle}∣f;M=+23​\ensuremath⟩ parity state to the lower ∣e;+32\ensuremath⟩|e;\phantom{\rule{0.16em}{0ex}}+\frac{3}{2}\ensuremath{\rangle}∣e;+23​\ensuremath⟩ state and observing their trap dynamics under an applied electric bias field. Our observations are very well fit by a simple Landau-Zener model, yielding insight to the rich spectra and dynamics of polar radicals in mixed external fields.
We report magnetic confinement of neutral, ground state OH at a density of approximately 3 x 10(3) cm(-3) and temperature of approximately 30 mK. An adjustable electric field sufficiently large to polarize the OH is superimposed on the trap in various geometries, making an overall potential arising from both Zeeman and Stark effects. An effective molecular Hamiltonian is constructed, with Monte Carlo simulations accurately modeling the observed single-molecule dynamics in various trap configurations. Magnetic trapping of cold polar molecules under adjustable electric fields may enable study of low energy dipolar interactions.
Confining atoms with a combination of optical and magnetic fields has led to the formation of new states of matter and provided a tunable test bed to explore many-body atomic and electronic interactions; however, its extension to molecules has been slow. Ultracold molecules (milikelvin temperatures and below) are of interest for a number of additional applications, including studies of quantum phase transitions and precision spectroscopy. One approach to confining polar molecules has relied on inhomogeneous electric fields. Sawyer et al. present an alternative method that traps molecules magnetically. They demonstrate the technique on hydroxyl (OH) radicals, which have appreciable magnetic as well as electric dipole moments. Lifetimes in the magnetoelectrostatic trap ranged from 20 to 500 ms, depending on the background pressure. The technique allows the additional degree of freedom of an electrical field to be superimposed onto the trapped molecules and should facilitate further studies in the direction of controlled molecular collisions and chemical reactions. — ISO
Polar molecules are desirable systems for quantum simulations and cold chemistry. Molecular ions are easily trapped, but a bias electric field applied to polarize them tends to accelerate them out of the trap. We present a general solution to this issue by rotating the bias field slowly enough for the molecular polarization axis to follow but rapidly enough for the ions to stay trapped. We demonstrate Ramsey spectroscopy between Stark-Zeeman sublevels in (180)Hf(19)F(+) with a coherence time of 100 milliseconds. Frequency shifts arising from well-controlled topological (Berry) phases are used to determine magnetic g factors. The rotating-bias-field technique may enable using trapped polar molecules for precision measurement and quantum information science, including the search for an electron electric dipole moment.
Theoretical investigation of the dynamics of adiabatic quantum mechanics in two different, highly polar systems has been made. The systems were chosen for their fundamental scientific interest, as they represent atoms and molecules with exagger-ated properties, as well as ease of experimental study as such highly polar systems are easier to manipulate using readily-available electric fields. A model two-level system is used to derive one approach for maximizing the probability of adiabatic passage through an avoided crossing and this is compared with the classic Landau-Zener re-sult, and the commonly encountered spin-flip problem of a particle with spin located in a rotating magnetic field. This approach is applied to the avoided crossing between the n = 13, n1 − n2 = 11 (dipole moment of 532 D) and the n = 14, n1 − n2 = −12 (dipole moment of-657 D) highly polar Stark states of the lithium atom at 447 kV/m. Ion-pair formation from two neutral lithium atoms, one in the 2s ground state and the other in an excited state, is also investigated. The cross section σ(v) for free ion-pairs is calculated for the initial colliding pairs of atomic states located below
Research in the field of cold polar molecules is progressing rapidly. An array of interesting\ntopics is being developed including precision measurement and fundamental tests, quantum phase transitions, and ultracold chemistry. In particular, dipolar molecules in well-defined quantum states enable exquisite control of their interactions via applied electric fields. The long-range, anisotropic interaction between dipolar molecules leads to new collision dynamics that could be used for novel collective effects, quantum state engineering, and information processing. The focus of this Thesis is the production of cold samples of neutral OH molecules via Stark deceleration and magnetic trapping for novel collision experiments. This novelty results from our combination of cold external beams and trapped target molecules which facilitates observation of dipolar effects as well as low temperature collision resonances. The large permanent electric dipole moment of OH allows us to precisely tune the lab-frame velocity of the molecular packets from ∼ 500 m/s to rest. We have magnetically trapped OH packets at the terminus of our Stark decelerator at a temperature of 70 mK and density of 106 cm−3. With improved understanding of Stark deceleration, we optimize the decelerator efficiency and its coupling to the magnetic trap. Our latest trap design uses permanent ring magnets to create a three-dimensional magnetic quadrupole field. Use of magnetically trapped OH molecules for collision experiments with external beams allow us the unique opportunity of observing both elastic and inelastic collisions. In addition, the trap confinement yields sensitivity to differential elastic cross sections at low collision energies. This open magnetic trap has allowed measurement of collision cross sections between trapped OH and external supersonic beams of He and D2, the latter of which is of astrophysical interest due to the role of H2-OH collisions in pumping interstellar OH megamasers. The combination of trapped OH molecules and temperature tuned beams of He and D2 has facilitated measurement of the lowest-energy D2-OH collision cross sections yet reported. More recently, we report the first observation of electric-field dependent cross sections between two different species of cold polar molecules - OH and ND3 - thereby demonstrating control over molecular scattering in the cold regime. By combining for the first time the production techniques of Stark deceleration and buffer gas cooling, we increase the molecular interaction time by∼ 105 over traditional crossed-beam experiments to gain enhanced sensitivity at the characteristic densities of cold molecule production.
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.