The growing field of cold molecule physics has demonstrated many methods of quantum control for precision measurement and molecular interaction studies. One particular method is Stark deceleration, which uses electric field gradients to produce packets of slow polar molecules. Since Stark deceleration does not increase phase-space density, the efficiency of the deceleration process is critical in determining the final cold molecule density. This dissertation describes three different Stark deceleration techniques. The first type of deceleration is pulsed-pin deceleration. We use this technique to produce slow OH molecules that can be trapped for cold collision studies. A two photon state-selective detection system, which includes a 118 nm photon, is used to determine the density distribution of OH in the trap. We explore the advantages and limitations to creating 118 nm light. The second and third types of Stark deceleration are pulsed-ring and traveling-wave methods of running a ring-geometry decelerator. Ring-geometry decelerators present improved deceleration efficiencies due to the cylindrical symmetry of the electrodes and true three-dimensional confinement. The pulsed-ring mode of the ring decelerator uses commercial high-voltage switches to apply discrete pulses to the ring electrodes. The continuous operation mode of the ring decelerator uses varying sine-wave voltages to create a traveling Stark potential well and has proven to be incredibly challenging due to the analog high voltage requirements of the system. In order to bring ND3 seeded in krypton (∼415 m/s) down to rest in the laboratory, sine wave voltages with amplitudes up to ±10 kV, currents up to 500 mA, and a bandwidth of 30 kHz down to DC are required. We describe a high-voltage amplifier that can be used for traveling-wave deceleration. The traveling-wave Stark deceleration mode is then compared to the pulsed-ring Stark deceleration mode and cases where one mode is superior to another are discussed.
The growing field of cold molecule physics has demonstrated many methods of quantum control for precision measurement and molecular interaction studies. One particular method is Stark deceleration, which uses electric field gradients to produce packets of slow polar molecules. Since Stark deceleration does not increase phase-space density, the efficiency of the deceleration process is critical in determining the final cold molecule density. This dissertation describes three different Stark deceleration techniques. The first type of deceleration is pulsed-pin deceleration. We use this technique to produce slow OH molecules that can be trapped for cold collision studies. A two photon state-selective detection system, which includes a 118 nm photon, is used to determine the density distribution of OH in the trap. We explore the advantages and limitations to creating 118 nm light. The second and third types of Stark deceleration are pulsed-ring and traveling-wave methods of running a ring-geometry decelerator. Ring-geometry decelerators present improved deceleration efficiencies due to the cylindrical symmetry of the electrodes and true three-dimensional confinement. The pulsed-ring mode of the ring decelerator uses commercial high-voltage switches to apply discrete pulses to the ring electrodes. The continuous operation mode of the ring decelerator uses varying sine-wave voltages to create a traveling Stark potential well and has proven to be incredibly challenging due to the analog high voltage requirements of the system. In order to bring ND3 seeded in krypton (∼415 m/s) down to rest in the laboratory, sine wave voltages with amplitudes up to ±10 kV, currents up to 500 mA, and a bandwidth of 30 kHz down to DC are required. We describe a high-voltage amplifier that can be used for traveling-wave deceleration. The traveling-wave Stark deceleration mode is then compared to the pulsed-ring Stark deceleration mode and cases where one mode is superior to another are discussed.
Abstract Stark deceleration is a technique that uses time-varying inhomogeneous electric fields to decelerate polar molecules for various molecular beam and trapping experiments. New ring-geometry Stark decelerators with continuously varying voltages offer a method to produce a more intense source of molecules than in the more typically used crossed-pin geometry Stark decelerators. However, this new technique, traveling-wave Stark deceleration, is more experimentally challenging due to the electronic requirements. A third method, pulsed-ring Stark deceleration, uses ring-geometry electrodes with high-voltage pulses to decelerate molecules. The discrete voltages make it easier to implement, and it is more efficient in certain situations due to an increased longitudinal potential gradient. Here, we present an experimental realization of a ring-geometry Stark decelerator using both continuously varying and discrete voltages. Using the pulsed-ring method, we demonstrate a newly accessible low-velocity regime for moderate peak voltages on ring electrodes. This opens up the opportunity to efficiently decelerate various molecular species using a medium length decelerator. A comparison of experimental and simulated results between traveling-wave and pulsed-ring Stark deceleration is presented along with a simple model for determining when each mode is more efficient.
Stark deceleration is a technique that uses time-varying inhomogeneous electric fields to decelerate polar molecules for various molecular beam and trapping experiments. New ring-geometry Stark decelerators with continuously varying voltages offer a method to produce a more intense source of molecules in a technique called traveling-wave Stark deceleration. However, this type of deceleration is more experimentally challenging than the more typically used crossed-pin geometry decelerators with pulsed voltages. Here, we present an experimental realization of a ring-geometry Stark decelerator using either continuously varying or discrete voltages. Pulsed-ring Stark deceleration using discrete voltages is easier to implement and, under certain circumstances, is more efficient than traveling-wave Stark deceleration. A comparison of experimental and simulated results between traveling-wave and pulsed-ring Stark deceleration is presented along with a simple model for determining when each mode is more efficient.
Cryogenic buffer-gas beams are a promising method for producing bright sources of cold molecular radicals for cold-collision and chemical-reaction experiments. In order to use these beams in studies of reactions with controlled collision energies or in trapping experiments, one needs a method of controlling the forward velocity of the beam. A Stark decelerator can be an effective tool for controlling the mean speed of molecules produced by supersonic jets, but efficient deceleration of buffer-gas beams presents new challenges due to longer pulse lengths. Traveling-wave decelerators are uniquely suited to meet these challenges because of their ability to confine molecules in three dimensions during deceleration and their versatility afforded by the analog control of the electrodes. We have created ground-state $\mathrm{CH}(X{\phantom{\rule{0.16em}{0ex}}}^{2}\ensuremath{\Pi})$ radicals in a cryogenic buffer-gas cell with the potential to produce a cold molecular beam of 1011 molecules/pulse. We present a general protocol for Stark deceleration of beams with a large position and velocity spread for use with a traveling-wave decelerator. Our method involves confining molecules transversely with a hexapole for an optimized distance before deceleration. This rotates the phase-space distribution of the molecular packet so that the packet is matched to the time-varying phase-space acceptance of the decelerator. We demonstrate with simulations and an analytic one-dimensional model that this method can decelerate a significant fraction of the molecules in successive wells of a traveling-wave decelerator to produce energy-tuned beams for cold and controlled-molecule experiments.
Research of cold and ultracold molecules is currently a burgeoning field in experimental and theoretical physics. New experimental techniques, involving an increasingly large set of molecule types under high levels of control, are currently opening up new avenues of research with a vast array of potential applications. From understanding the role of quantum mechanics in molecular scattering and cold chemistry, to testing the fundamental symmetries of nature and realizing quantum computing with dipolar molecular qubits, experiments are accessing regimes not dreamed of even a few years ago. Theoretical interest and computing capabilities are also at an all time high, spurred on by the possibility of creating ultracold dipolar gases as tunable realizations of strongly interacting quantum Hamiltonians, creating exotic phases of matter, and the investigation of controlling molecular interactions with applied electromagnetic fields.\nLess than a decade ago, cold molecule experiments had seemingly reached a technological plateau, being capable of creating moderate densities of 106-107 molecules/cm3 at temperatures of 10-100 mK. With many applications requiring colder temperatures and higher densities, the field was ripe for new advances. Today, via a plethora of methods such as direct molecular laser cooling, electro-optical cooling, magneto- and photo-association, and new molecular beam deceleration techniques, the field is just beginning to have the tools capable of producing truly interesting systems for study.\nThis work will discuss a couple of major steps taken in the direction of achieving scientific goals using cold molecules. The first experimental advancement discussed will be the development of a co-trap environment for studying interactions and collisions between ultracold atoms and Stark decelerated cold polar molecules. In this experiment, rubidium atoms are trapped using magnetic fields, and ammonia atoms are decelerated and trapped using electric fields. The two traps are spatially overlapped in order to investigate inter-species interactions. The co-trap environment provides exceedingly long interaction times, many orders of magnitude longer than typical beam-based interaction studies. As a result, it provides extremely high sensitivity to weak interaction mechanisms. The second experimental advancement discussed will be the development and construction of a new style of Stark decelerator, capable of producing much larger densities of cold molecules. This apparatus has the potential to expand the realm of possible experiments with chemically interesting species, and provide an unprecedented amount of control over molecular beams and traps. The gains haven't come easily though, as a new class of custom high-voltage amplifiers have needed to be developed. This part of the experiment alone took approximately two years of consistent effort to bring to fruition. After many years of development, this experiment is poised to come online, finally fulfilling its potential.
We present experiments on decelerating and trapping ammonia molecules using a combination of a Stark decelerator and a traveling wave decelerator. In the traveling wave decelerator, a moving potential is created by a series of ring-shaped electrodes to which oscillating high voltages (HV) are applied. By lowering the frequency of the applied voltages, the molecules confined in the moving trap are decelerated and brought to a standstill. As the molecules are confined in a true 3D well, this kind of deceleration has practically no losses, resulting in a great improvement on the usual Stark deceleration techniques. The necessary voltages are generated by amplifying the output of an arbitrary wave generator using fast HV amplifiers, giving us great control over the trapped molecules. We illustrate this by experiments in which we adiabatically cool trapped NH3 and ND3 molecules and resonantly excite their motion.
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.