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Laser cooling of BaH molecules, and new ideas for the detection of dark matter

Rees L. McNally

Published Jan 1, 2021• 1 citation
Publisher

Abstract

The advent of laser cooling and optical manipulation for atomic samples revolutionized atomic physics in 1990’s, allowing the creation of new phases of matter, more accurate atomic clocks, and enabling leading candidates for the first functional quantum computer. This could not have been predicted at the time, and is a testament to the value of fundamental research for its own sake. These same laser cooling techniques are now being applied to simple molecular systems with the same revolutionary potential. In this thesis, I will present a range of experiments exploring these schemes in a new class of molecules, the diatomic alkaline earth hydrides. We present the creation and characterization of a bright beam of cold barium hydride molecules, high precision spectroscopy of these samples, as well as optical deflection and transverse cooling. This represents the first laser cooling of a Hydride molecule. This is a crucial step towards the creation of new cold molecular samples for a variety of scientific applications. In the final chapter, I will change gears, and introduce new ideas for the detection of scalar field dark matter. While this variety of dark matter is typically searched for using atomic clocks, I will show that the same coupling also leads to anomalous acceleration of test masses. This acceleration would be detectable using both a network of precision acceleration sensors known as the IGETS network, and by the LIGO observatory. This new technique will compliment existing search strategies, and has higher sensitivity for a wide region of parameter space.

DOI
10.7916/d8-bbr3-zv47

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The advent of laser cooling and optical manipulation for atomic samples revolutionized atomic physics in 1990’s, allowing the creation of new phases of matter, more accurate atomic clocks, and enabling leading candidates for the first functional quantum computer. This could not have been predicted at the time, and is a testament to the value of fundamental research for its own sake. These same laser cooling techniques are now being applied to simple molecular systems with the same revolutionary potential. In this thesis, I will present a range of experiments exploring these schemes in a new class of molecules, the diatomic alkaline earth hydrides. We present the creation and characterization of a bright beam of cold barium hydride molecules, high precision spectroscopy of these samples, as well as optical deflection and transverse cooling. This represents the first laser cooling of a Hydride molecule. This is a crucial step towards the creation of new cold molecular samples for a variety of scientific applications. In the final chapter, I will change gears, and introduce new ideas for the detection of scalar field dark matter. While this variety of dark matter is typically searched for using atomic clocks, I will show that the same coupling also leads to anomalous acceleration of test masses. This acceleration would be detectable using both a network of precision acceleration sensors known as the IGETS network, and by the LIGO observatory. This new technique will compliment existing search strategies, and has higher sensitivity for a wide region of parameter space.
Ultracold molecules promise a revolutionary test bed for quantum science with applications ranging from experiments that probe the nature of our universe, to hosting new platforms for quantum computing. Cooling and trapping molecules in the ultracold regime is the first step to unlocking the wide array of proposed applications, and developing these techniques to control molecules is a key but challenging research field. In this thesis, we describe progress towards a new apparatus designed to cool and trap barium monohydride (BaH), a molecule that is amenable to laser cooling and has prospects as a precursor for ultracold atomic hydrogen. The same complexity that makes molecules interesting objects of study creates challenges for optical control. To mitigate some of these challenges, we first cool the molecules using cryogenic techniques and technologies. Our apparatus uses a cryogenic buffer gas to thermalize BaH within a contained cell. The molecules are extracted into a beam with millikelvin transverse temperature, and forward velocities <100 m/s. The BaH beam in this work is the brightest hydride beam to date, with molecule density and kinetic characteristics well suited for laser cooling and trapping.
Bright beams of cold molecules provide valuable quantum sensors for measuring permanent electric dipole moments that violate fundamental symmetries, which enables these tabletop experiments to probe energy scales exceeding those available with current or near-future particle colliders. The precision of such experiments generally scales with the number of molecules that are detected per unit time, typically a few meters downstream of the place where the molecular beam is created. So, improving the precision -and thereby probing new physics at higher and higher energy scales- requires increasing the downstream flux of molecules. This can be achieved by collimating the molecular beam to maintain a high number density. These molecular experiments can borrow techniques for control and manipulation from the extremely well-developed field of atomic physics. One such technique is laser cooling, which is a powerful method to achieve this boost in brightness, whose implementation however remains challenging due to the complex energy level structure of molecules. In this work, we demonstrate and analyze laser cooling of a focused cryogenic beam of BaF molecules. We conclude that with some follow-up steps this method will increase the beam brightness by a factor 100, a crucial milestone towards a high precision measurement of the electron electric dipole moment (eEDM).
Potential wide-ranging scientific applications, spanning fundamental physics to quantum engineering, has led to significant efforts in controlling molecules at the quantum level. The rich internal structure of molecules, that gives rise to these desirable properties also complicates the task of controlling such species. Over the past decade, our ability to produce, control, and detect molecules has advanced tremendously with direct laser-cooling and magneto-optical trapping of diatomic molecules realized by several groups around the world. In this thesis, we describe the creation of the first RF MOT of CaF, which at the time of the writing of this thesis, remains the largest and densest molecular MOT. New laser cooling techniques for molecules are demonstrated, allowing laser cooling of molecules to 4 uK, 50 times colder than the Doppler limit. Optical trapping of these molecules is also achieved, which, in combination with in-trap laser cooling increased the density of trapped molecules by five orders of magnitude compared to the density in the MOT. We developed methods to cool and detect single molecules with high fidelity, which aided us in the creation of an optical tweezer array of single, ultracold CaF molecules. The densities of molecules (10^12 cm^-3) attained inside the tweezer traps also enabled us to observe both light-assisted and ground state collisions of laser cooled molecules, for the first time. The phase space density within the merged tweezers reached 5x10^-4, 10 orders of magnitude larger than the initial MOT. We implemented internal quantum state control of the molecules and dynamical control of the tweezers to build a platform for exploring state-selective ultracold quantum chemistry.
Cold molecules are an invaluable tool for modern physics. Cold atoms have already revolutionized precision metrology, allowed for spectacular findings in quantum physics and opened the door for the creation and observation of novel states of matter. Cold molecules bring with them additional degrees of freedom which give rise to unique properties that enable new kinds of experiments. For these experiments it is of vital importance to start with a sufficiently large number of cold molecules. There are multiple paths for the slowing and cooling of atoms and most of the slowing techniques utilizing lasers for direct cooling have been transferred to the molecular case with its specific requirements. The Zeeman slowing technique is advantageous for loading a trap with cold particles but had not yet been transferred from atoms to the molecular case. In this thesis I will show the first realization of the Zeeman slowing technique for diatomic molecules. This thesis will discuss several preparatory steps: Our group has had some ideas to collimate the molecular beam with a conical nozzle outlet at the buffer gas cell which I investigated on potassium atoms generated by the ablation of 39K35Cl inside the buffer gas cell. I also realized a fluorescence spectroscopy of the |XΣ1/2, N = 1, v = 0⟩ → |AΠ1/2, N = 0, v = 0⟩ transition in magnetic fields up to 300 G and confirmed simulations regarding our two laser cycling scheme in the Paschen-Back regime by measuring the scattering rate of light on one molecule. Finally, I created pre-cooled 40Ca19F with a forward velocity of around 150 m s−1 from a 40Ca19F2 target with laser ablation inside a cryogenic buffer gas cell. With the Zeeman slowing technique I slowed the molecules down to 25 m s−1, a velocity where trapping can be possible. I have also shown the characteristic compression into specific velocity classes for not yet trappable velocities. Together these two findings demonstrate that molecular Zeeman slowing is possible and a real promising tool for future experiments.
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.
Abstract Direct laser cooling of molecules has made significant progress in recent years. However, the selective cooling and manipulation of generic molecular samples based on their isotopic composition, which is ubiquitous in atomic laser cooling, has not yet been achieved. Here, we demonstrate such isotopologue-selective laser cooling and near-arbitrary control over the isotopic composition of a molecular beam, using barium monofluoride (BaF) as an example. The manipulation of the rare and previously uncooled 136 BaF is achieved in the presence of several isotopologues of significantly higher natural abundance. Our results enable intense molecular beams, high fidelity detection and manipulation of select low-abundance isotopologues or isotopic mixtures. Such beams are a first step towards isotopologue-selective molecular trapping and will be useful for applications in trace gas analysis, cold collisions and precision tests of fundamental symmetries.