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
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
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.
Abstract Trapped cold molecules represent attractive systems for precision-spectroscopic studies and for investigations of cold collisions and chemical reactions. However, achieving their confinement for sufficiently long timescales remains a challenge. Here, we report the long-term trapping of Stark-decelerated OH radicals in their X2Π3/2 (ν = 0, J = 3/2, MJ = 3/2, f) state in a permanent magnetic trap. The trap environment is cryogenically cooled to a temperature of 17 K to suppress black-body-radiation-induced pumping of the molecules out of trappable quantum states and collisions with residual background gas molecules which usually limit the trap lifetime. The cold molecules are thus confined on timescales approaching minutes, an improvement of up to two orders of magnitude compared with room temperature experiments, at translational temperatures of ∼25 mK. The present results pave the way for new experiments using trapped cold molecules in precision spectroscopy, in studies of slow chemical processes at low energies and in the quantum technologies.
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.
While cold molecule experiments are rapidly moving towards their promised benefits of precision spectroscopy, controllable chemistry, and novel condensed phases, heretofore the field has been greatly limited by a lack of methods to cool and compress chemically diverse species to temperatures below ten millikelvin. While in atomic physics these needs are fulfilled by laser cooling, magneto-optical trapping, and evaporative cooling, until now none of these techniques have been applicable to molecules. In this thesis, two major breakthroughs are reported. The first is the observation of evaporative cooling in magnetically trapped hydroxyl (OH) radicals, which potentially opens a path all the way to Bose-Einstein condensation of dipolar radicals, as well as allowing cold- and ultracold-chemistry studies of fundamental reaction mechanisms. Through the combination of an extremely high gradient magnetic quadrupole trap and the use of the OH Λ-doublet transition to enable highly selective forced evaporation, cooling by an order of magnitude in temperature was achieved and yielded a final temperature no higher than 5mK. The second breakthrough is the successful application of laser cooling and magneto-optical trapping to molecules. Motivated by a proposal in this thesis, laser cooling of molecules is now known to be technically feasible in a select but substantial pool of diatomic molecules. The demonstration of not only Doppler cooling but also two-dimensional magneto-optical trapping in yttrium (II) oxide, YO, is expected to enable rapid growth in the availability of ultracold molecules--just as the invention of the atomic magneto-optical trap stimulated atomic physics twenty-five years ago.
The realization of rovibrationally stable dense samples of ultracold diatomic molecules remains one of the main stepping stones to achieve the next slate of major goals in the field of atomic and molecular physics. Though obtaining diatomic alkali molecules was seen as a logical next step following the optical cooling of atoms, many of the possible applications currently under investigation extend beyond atomic and molecular physics. For example, spectroscopy of ultracold molecules can help in testing extensions of the Standard Model via the search for a permanent electric dipole moment of the electron (1; 2), or the energy difference between enantiomers of chiral molecules (3). Various molecular transitions can be utilized to track the time dependence of fundamental constants, including the fine structure constant and the proton to electron mass ratio (4). They also open the way for cold and ultracold chemistry, where the interacting species and products are in a coherent quantum superposition state (5) and reactions can happen via quantum tunneling. Dipolar ultracold quantum gases promise to show a plethora of new phenomena due to anisotropic long-range dipole-dipole interactions (6). Dipolar molecules in optical lattices can be employed as a quantum simulator of condensed matter systems, and they are predicted to demonstrate new quantum phases such as a dipolar crystal, supersolid, checkerboard and collapse phases (7; 8). Ultracold polar molecules also represent an attractive platform for quantum computation (9). They offer a variety of long-lived states for qubit encoding, including rotational, spin and hyperfine (if electronic and nuclear spins are non-zero), Λ and Ω-doublet states (10) and scalability to a large number of qubits. Polar molecules can be easily controlled by DC electric and magnetic fields, as well as bymicrowave and optical fields, allowing the design of various traps (11; 12). The main appeal of polar molecules for quantum information processing, however, comes from their permanent electric dipole moment, permitting them to interact via a long-range dipole-dipole interaction. The dipole-dipole interaction offers a tool to construct two-qubit gates, required for universal quantum computation (9; 13). Ultracold molecules in their ground vibrational state v = 0 (and even in specific rotational, hyperfine or Zeeman states) are required formany of these applications since they have a large permanent electric dipole moment and are stable with respect to collisions and spontaneous emission. Currently translationally ultracold (100 nK 1 mK) molecules are produced by magneto(14) and photo-association (15) techniques. In a typical photoassociation scheme, 3
A hybrid trap was developed to confine neutral molecules and molecular ions. We demonstrated the long-term trapping of Stark-decelerated OH radicals in the X 2Pi3/2 (v = 0, J = 3/2, MJ = 3/2, f) state in a permanent magnetic trap. The trap environment was cryogenically cooled to a temperature of 17 K in order to efficiently suppress black-body-radiation-induced pumping of the molecules out of trappable quantum states and collisions with residual background gas molecules which usually limit the trap lifetimes. The cold molecules were kept confined on timescales approaching minutes, an improvement of up to two orders of magnitude compared to room-temperature experiments, at translational temperatures on the order of 25 mK. A cryogenic ion trap was built and laser cooled Ca+ ions were confined. This ion trap can be used to confine sympathetically cooled molecular ions such as N+2or H2O+. Furthermore, a mechanism to superimpose both trap centers by moving the permanent magnets from the magnetic trap over the ion trap was developed. Both traps were characterized and their functionality was proven. The challenges of lasercooling in the strong magnetic field gradients were discussed. The present results pave the way for investigations of cold collisions and reactions with very small reaction rates between molecular ions and neutral molecules, for new avenues for the production of ultracold molecules via sympathetic cooling and for the realization of new forms of hybrid matter with co-trapped atoms or ions.