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Experiments on Cold Molecules Produced via Stark Deceleration

Eric R. Hudson

Published Jan 1, 2006• 3 citations
OpenAlex

Abstract

The final copy of this thesis has been examined by the signatories, and we find that both the content and the form meet acceptable presentation standards of scholarly work in the above mentioned discipline. iii Hudson, Eric R. (Ph.D., Physics) Experiments on Cold Molecules Produced via Stark Deceleration Thesis directed by Prof. Jun Ye The work described in this thesis is the construction and operation of a Stark deceleration apparatus. Specifically, this work represents only the second successful im-plementation of the method1 and the first deceleration of the hydroxyl radical (OH) and the formaldehyde molecule (H2CO). Experimentally, much of the work in the beginning of our experiments was the construction of a suitable molecular beam. Though molecular beams have been used for decades in physical chemistry, the design goals of the typical physical chemistry experiment are very different than ours, and as such, much work was required to adapt these sources for Stark deceleration. Since the maximum-attainable,

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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.

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The motion of polar molecules can be controlled by time-varying inhomogeneous electric fields. In a Stark decelerator, this is exploited to accelerate, transport, or decelerate a fraction of a molecular beam. When combined with a trap, the decelerator provides a means to store the molecules for times up to seconds. Here, we review our efforts to produce cold molecules via this technique. In particular, we present a new generation Stark decelerator and electrostatic trap that selects a significant part of a molecular beam pulse that can be loaded into the trap. Deceleration and trapping experiments using a beam of OH radicals are discussed.

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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.

•Jan 1, 2018•1 citation
The final copy of this thesis has been examined by the signatories, and we find that both the content and the form meet acceptable presentation standards of scholarly work in the above mentioned discipline. iii Hudson, Eric R. (Ph.D., Physics) Experiments on Cold Molecules Produced via Stark Deceleration Thesis directed by Prof. Jun Ye The work described in this thesis is the construction and operation of a Stark deceleration apparatus. Specifically, this work represents only the second successful im-plementation of the method1 and the first deceleration of the hydroxyl radical (OH) and the formaldehyde molecule (H2CO). Experimentally, much of the work in the beginning of our experiments was the construction of a suitable molecular beam. Though molecular beams have been used for decades in physical chemistry, the design goals of the typical physical chemistry experiment are very different than ours, and as such, much work was required to adapt these sources for Stark deceleration. Since the maximum-attainable,
We propose a method for controlling a class of low temperature chemical reactions. Specifically, we show the hydrogen abstraction channel in the reaction of formaldehyde (H{sub 2}CO) and the hydroxyl radical (OH) can be controlled through either the molecular state or an external electric field. We also outline experiments for investigating and demonstrating control over this important reaction. To this end, we report the first Stark deceleration of H{sub 2}CO. We have decelerated a molecular beam of H{sub 2}CO essentially to rest, producing molecules at 100 mK with a density of {approx} 10{sup 6} cm{sup -3}.
We propose a method for controlling a class of low temperature chemical reactions. Specifically, we show the hydrogen abstraction channel in the reaction of formaldehyde (H2CO)({\mathrm{H}}_{2}\mathrm{CO})(H2​CO) and the hydroxyl radical (OH)(\mathrm{OH})(OH) can be controlled through either the molecular state or an external electric field. We also outline experiments for investigating and demonstrating control over this important reaction. To this end, we report the first Stark deceleration of H2CO{\mathrm{H}}_{2}\mathrm{CO}H2​CO. We have decelerated a molecular beam of H2CO{\mathrm{H}}_{2}\mathrm{CO}H2​CO essentially to rest, producing molecules at 100mK100\phantom{\rule{0.3em}{0ex}}\mathrm{mK}100mK with a density of $\ensuremath{\sim}{10}^{6}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$.
Samples of cold and ultracold polar molecules have the potential to revolutionize physical chemistry, precision measurement, and few-body quantum physics. This thesis describes experimental results for the production of cold samples of OH radicals by Stark deceleration of a supersonic beam. Since Stark deceleration cannot increase the phase space density of the sample, the initial production stage of the OH molecule is critical. The first set of experiments describes a general methodology for the production of OH beams with maximal phase space density, as well as the subsequent coupling to a Stark decelerator. Additionally, we describe the redesign of our electrostatic trap, optimized for future collision experiments of OH with co-trapped ultracold Rb atoms. The new design resulted in a 15-fold increase in total number of trapped molecules over the previous design when tested with ND3 molecules. The second set of experiments focuses on laser-based detection of OH molecules at the exit of the decelerator based on laser induced fluorescence (LIF) and resonance enhanced multiphoton ionizaton (REMPI). The latter method uses vacuum-ultraviolet light at 118nm produced by third-harmonic generation in Xe/Ar gas mixtures as the ionizing step. The sensitivity of this latter technique is limited by the attainable photon flux of the ionizing radiation at 118nm. We present detailed measurements of the conversion efficiencies as well as absolute photon fluxes. Strategies to overcome these limitations as well as prospects for detection of OH molecules in a trap are discussed.
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.
The motion of polar molecules can be controlled by time-varying inhomogeneous electric fields. In a Stark decelerator, this is exploited to accelerate, transport, or decelerate a fraction of a molecular beam. When combined with a trap, the decelerator provides a means to store the molecules for times up to seconds. Here, we review our efforts to produce cold molecules via this technique. In particular, we present a new generation Stark decelerator and electrostatic trap that selects a significant part of a molecular beam pulse that can be loaded into the trap. Deceleration and trapping experiments using a beam of OH radicals 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.