We propose a method to produce, in a pulsed or continuous way, cold samples of highly polar molecules. Using a pulsed or continuous standard (supersonic) beam of these molecules, our idea consists of transforming the molecules into their anionic counterparts, which are decelerated to a standstill by a well-controlled external electric field and ultimately neutralized. The neutral-to-anion transformation occurs through collisions with Rydberg atoms coming from an additional atomic beam. This Rydberg electron transfer process is possible provided that the molecular species has a sufficiently strong electric dipole ( D, i.e., cm). Whatever the mass of the species, the deceleration stage is realized by a temporally and spatially controlled electric field within a range of less than one centimeter, which is much shorter than in current deceleration experiments of neutral molecules. Once stopped, the molecular anions are neutralized by laser photodetachment or a pulsed electric field process. The resulting molecules might be held and accumulated, for instance, in a magnetic trap.
We propose a method to produce, in a pulsed or continuous way, cold samples of highly polar molecules. Using a pulsed or continuous standard (supersonic) beam of these molecules, our idea consists of transforming the molecules into their anionic counterparts, which are decelerated to a standstill by a well-controlled external electric field and ultimately neutralized. The neutral-to-anion transformation occurs through collisions with Rydberg atoms coming from an additional atomic beam. This Rydberg electron transfer process is possible provided that the molecular species has a sufficiently strong electric dipole ( D, i.e., cm). Whatever the mass of the species, the deceleration stage is realized by a temporally and spatially controlled electric field within a range of less than one centimeter, which is much shorter than in current deceleration experiments of neutral molecules. Once stopped, the molecular anions are neutralized by laser photodetachment or a pulsed electric field process. The resulting molecules might be held and accumulated, for instance, in a magnetic trap.
Slowing down atoms using laser cooling, together with techniques like magnetic trapping and evaporative cooling, has led to numerous exciting results over the last decade [1], with the realization of Bose-Einstein condensation as the most spectacular achievement [2]. Laser-cooling schemes are applicable to atoms since closed multilevel systems can be realized and many consecutive absorptionemission cycles can be induced. This leads to a significant momentum transfer from the photons of the laser to the atom, resulting in a change of the velocity of the atom. There currently is a great interest in producing cold molecules for the study of cold molecule-molecule collisions, molecular quantum collective effects, Doppler-free spectroscopy, frequency standards, as well as many other applications already realized for atoms [3]. Slowing down of neutral molecules, a prerequisite for being able to trap them, has proven to be considerably more difficult to be achieved, however. The above-mentioned laser-cooling scheme cannot be applied to slow down molecules as no simple closed-level systems can be found; the unavoidable off-resonant radiative decay of molecules from the excited state to other vibrational levels in the electronic ground state hampers efficient momentum transfer [4]. Once molecules are present at sufficiently low kinetic energies, below a fraction of a cm21, they can be trapped in various ways. Trapping of neutral molecules in inhomogeneous magnetic [3] and electric fields [5] and trapping based on the use of evanescent fields close to the dielectricvacuum interface have been proposed [6]. It has also been suggested that extremely high laser powers might be used to induce a dipole moment in polarizable molecules, leading to trapping of these molecules in the laser beam [7]. Other methods to produce slow molecules have been put forward and have recently been successfully applied to produce the first samples of trapped molecules. By injecting molecules in a cold buffer gas, sufficiently low kinetic energies of the injected molecules can be obtained after thermalization that they can subsequently be trapped in an inhomogeneous magnetic field. This has recently been demonstrated for CaH injected in 3He buffer gas at temperatures of around 0.3 K [8]. Associative collisions between ultracold trapped atoms [9] have proven to be
Inspired by the spectacular successes in the field of cold atoms, there is currently great interest in cold molecules. Cooling molecules is useful for various fundamental physics studies and gives access to an exotic regime in chemistry where the wave property of the molecules becomes important. Although cooling molecules has turned out to be considerably more difficult than cooling atoms, a number of methods to produce samples of cold molecules have been demonstrated over the last few years. This paper aims to review the application of cold molecules and the methods to produce them. Emphasis is put on the deceleration of polar molecules using time-varying electric fields. The operation principle of the array of electrodes that is used to decelerate polar molecules is described in analogy with, and using terminology from, charged-particle accelerators. It is shown that, by applying an appropriately timed high voltage burst, molecules can be decelerated while the phase-space density, i.e. the number of molecules per position-velocity interval, remains constant. In this way the high density and low temperature in the moving frame of a pulsed molecular beam can be transferred to the laboratory frame. Experiments on metastable CO in states that are either repelled by or attracted to high electric fields are presented. Loading of slow molecules into traps and storage rings is discussed.
This thesis describes contributions to the development of a new method to control the translational motion of atoms and molecules in supersonic beams.This method, Rydberg-Stark deceleration, is in principle applicable to all atoms and molecules in the gas phase.It relies on the Stark effect exhibited by Rydberg states and enables the production of samples of translationally and internally cold atoms and molecules which have possible applications in high-resolution spectroscopic experiments, in the studies of collisions at low temperatures and in quantum information science.This method has been developed and tested in deceleration and trapping experiments on hydrogen and deuterium atoms, and hydrogen molecules initially moving in supersonic beams.Its power originates from the large dipole moments, easily exceeding 1000 Debye, induced in Rydberg states by electric fields.Large forces are exerted on Rydberg atoms and molecules
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.
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.