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A Three-Dimensional MOT of YO Towards Narrow-Line Cooling

Alejandra Collopy

Published Jan 1, 2018• 0 citations

Abstract

Laser cooling and magneto-optical trapping of neutral atoms has been a driving force in physics over the last few decades by providing an efficient method to produce cold and dense samples of cold atoms. Polar molecules which can have strong, long-range dipolar interactions and possess more rich internal structure promise a wide range of new physics and chemistry studies if they can be controlled efficiently. Until recently, the only way to achieve sub-milliKelvin level temperatures in molecules was to associate two precooled atomic species, which while very effective, has a firm bound on the chemical diversity accessible. While laser cooling of molecules relies on fortuitous molecular properties, it will significantly increase the choices of species available for molecular cooling.In this thesis I present the improved optical deceleration of the molecule yttrium monoxide (YO) and the loading of molecules into a 3-D magneto-optical trap (MOT). By making an improved choice of repumping scheme from our groups’ previous work, our photon scattering rate has been increased. By also improving our buffer gas cell source, we produce a much larger flux (2000 times higher) of slowed molecules at 5 m/s to reach the trapping region. I have designed and implemented 3-D MOT field coils operating at 5 MHz, and demonstrated a successful operation of a 3-D MOT. This is the first 3-D laser trapping of an oxide and the first of a molecule with an electronic state intermediate to the main cycling transition states.I have also performed a study of the transition from the ground state to the intermediate electronic state, which has a narrower linewidth of 150 kHz, in contrast to the main cycling transition’s linewidth of 5 MHz. This transition is well suited to second-stage narrow line cooling after loading molecules with the main MOT transition, which will allow direct laser cooling of a molecule to the 10 uK regime.

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Complex molecular structure demands customized solutions to laser cooling by extending its general set of principles and practices.Compared with other laser-cooled molecules, yttrium monoxide (YO) exhibits a large electron-nucleus interaction, resulting in a dominant hyperfine interaction over the electron spinrotation coupling.The YO ground state is thus comprised of two manifolds of closely spaced states, with one of them possessing a negligible Landé g factor.This unique energy level structure favors dual-frequency dc magneto-optical trapping (MOT) and gray molasses cooling (GMC).We report exceptionally robust cooling of YO at 4 μK over a wide range of laser intensity, detunings (one-and two-photon), and magnetic field.The magnetic insensitivity enables the spatial compression of the molecular cloud by alternating GMC and MOT under the continuous operation of the quadrupole magnetic field.A combination of these techniques produces a laser-cooled molecular sample with the highest phase space density in free space.

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Laser cooling and magneto-optical trapping of neutral atoms has been a driving force in physics over the last few decades by providing an efficient method to produce cold and dense samples of cold atoms. Polar molecules which can have strong, long-range dipolar interactions and possess more rich internal structure promise a wide range of new physics and chemistry studies if they can be controlled efficiently. Until recently, the only way to achieve sub-milliKelvin level temperatures in molecules was to associate two precooled atomic species, which while very effective, has a firm bound on the chemical diversity accessible. While laser cooling of molecules relies on fortuitous molecular properties, it will significantly increase the choices of species available for molecular cooling.In this thesis I present the improved optical deceleration of the molecule yttrium monoxide (YO) and the loading of molecules into a 3-D magneto-optical trap (MOT). By making an improved choice of repumping scheme from our groups’ previous work, our photon scattering rate has been increased. By also improving our buffer gas cell source, we produce a much larger flux (2000 times higher) of slowed molecules at 5 m/s to reach the trapping region. I have designed and implemented 3-D MOT field coils operating at 5 MHz, and demonstrated a successful operation of a 3-D MOT. This is the first 3-D laser trapping of an oxide and the first of a molecule with an electronic state intermediate to the main cycling transition states.I have also performed a study of the transition from the ground state to the intermediate electronic state, which has a narrower linewidth of 150 kHz, in contrast to the main cycling transition’s linewidth of 5 MHz. This transition is well suited to second-stage narrow line cooling after loading molecules with the main MOT transition, which will allow direct laser cooling of a molecule to the 10 uK regime.

Laser cooling and trapping are central to modern atomic physics. It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields and a number of Nobel prizes. Prior to the work presented in this thesis, laser cooling had not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for a wide range of applications. The first direct laser cooling of a molecule and further results we present here provide a new route to ultracold temperatures for molecules. In particular, these methods bridge the gap between ultracold temperatures and the approximately 1 kelvin temperatures attainable with directly cooled molecules (e.g. with cryogenic buffer gas cooling or decelerated supersonic beams). Using the carefully chosen molecule strontium monofluoride (SrF), decays to unwanted vibrational states are suppressed. Driving a transition with rotational quantum number R=1 to an excited state with R'=0 eliminates decays to unwanted rotational states. The dark ground-state Zeeman sublevels present in this specific scheme are remixed via a static magnetic field. Using three lasers for this scheme, a given molecule should undergo an average of approximately 100,000 photon absorption/emission cycles before being lost via unwanted decays. This number of cycles should be sufficient to load a magneto-optical trap (MOT) of molecules. In this thesis, we demonstrate transverse cooling of an SrF beam, in both Doppler and a Sisyphus-type cooling regimes. We also realize longitudinal slowing of an SrF beam. Finally, we detail current progress towards trapping SrF in a MOT. Ultimately, this technique should enable the production of large samples of molecules at ultracold temperatures for molecules chemically distinct from competing methods.

In addition to being suitable for laser cooling and trapping in a magneto-optical trap (MOT) using a relatively broad transition, the molecule YO possesses a narrow-line transition. This forbidden transition between the and states has linewidth kHz. After cooling in a MOT on the 614 nm to (orange) transition, the narrow 690 nm (red) transition can be used to further cool the sample, requiring only minimal additions to the first stage system. We estimate that the narrow line cooling stage will bring the temperature from ∼1 mK to ∼10 μ K, significantly advancing the frontier on direct cooling achievable for molecules.

We report three-dimensional trapping of an oxide molecule (YO), using a radio-frequency magneto-optical trap (MOT). The total number of molecules trapped is ∼1.5×10^{4}, with a temperature of 4.1(5) mK. This diversifies the frontier of molecules that are laser coolable and paves the way for the second-stage narrow-line cooling in this molecule to the microkelvin regime. Futhermore, the new challenges of creating a 3D MOT of YO resolved here indicate that MOTs of more complex nonlinear molecules should be feasible as well.

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.

Laser cooling and trapping in a magneto-optical trap (MOT) have been essential to the success of cold atom physics in the last decades. Recently, the application of the same techniques to molecules has begun. The complexity of even a simple diatomic molecule makes laser cooling difficult, but promises new applications in many areas of research. In this thesis I describe the development of the first three-dimensional MOT of calcium fluoride (CaF) molecules. First, a cryogenic buffer gas source was set up, producing a pulsed beam of 9.3*10^10 molecules per steradian per pulse with forward velocities around 170 m/s. A similar source for very large molecules was set up during a 5 month internship at the University of Vienna. Next, the molecular pulse was slowed down to the capture velocity of a MOT using chirped laser slowing, resulting in about 7*10^5 CaF molecules passing through the typical MOT volume of 1 cm^3 at velocities of 15+-5 m/s. A new deceleration method, called Zeeman-Sisyphus deceleration, was also investigated. In this method molecules move through a spatially varying magnetic field and are optically pumped between low- and high-field seeking states in such as a way that they are always losing kinetic energy. The method promises to deliver more slow molecules because the molecules are guided transversely as they are decelerated. A small prototype was built and the optical pumping step was tested successfully. Finally, 7.6*10^3 CaF molecules were trapped in a MOT and cooled to a temperature of 8.5 mK. The radial trap frequency is 2 pi*130 Hz and the damping constant is beta=9.5*10^2 s^-1. The lifetime is about 100 ms and depends strongly on the scattering rate. This MOT is an an ideal starting point for a wide range of new experiments with ultracold molecules.

Complex molecular structure demands customized solutions to laser cooling by extending its general set of principles and practices.Compared with other laser-cooled molecules, yttrium monoxide (YO) exhibits a large electron-nucleus interaction, resulting in a dominant hyperfine interaction over the electron spinrotation coupling.The YO ground state is thus comprised of two manifolds of closely spaced states, with one of them possessing a negligible Landé g factor.This unique energy level structure favors dual-frequency dc magneto-optical trapping (MOT) and gray molasses cooling (GMC).We report exceptionally robust cooling of YO at 4 μK over a wide range of laser intensity, detunings (one-and two-photon), and magnetic field.The magnetic insensitivity enables the spatial compression of the molecular cloud by alternating GMC and MOT under the continuous operation of the quadrupole magnetic field.A combination of these techniques produces a laser-cooled molecular sample with the highest phase space density in free space.