Magnetic trapping of bromine atoms at temperatures in the millikelvin regime is demonstrated for the first time. The atoms are produced by photodissociation of Br2 molecules in a molecular beam. The lab-frame velocity of Br atoms is controlled by the wavelength and polarization of the photodissociation laser. Careful selection of the wavelength results in one of the pair of atoms having sufficient velocity to exactly cancel that of the parent molecule, and it remains stationary in the lab frame. A trap is formed at the null point between two opposing neodymium permanent magnets. Dissociation of molecules at the field minimum results in the slowest fraction of photofragments remaining trapped. After the ballistic escape of the fastest atoms, the trapped slow atoms are lost only by elastic collisions with the chamber background gas. The measured loss rate is consistent with estimates of the total cross section for only those collisions transferring sufficient kinetic energy to overcome the trapping potential.
Magnetic trapping of bromine atoms at temperatures in the millikelvin regime is demonstrated for the first time. The atoms are produced by photodissociation of Br2 molecules in a molecular beam. The lab-frame velocity of Br atoms is controlled by the wavelength and polarization of the photodissociation laser. Careful selection of the wavelength results in one of the pair of atoms having sufficient velocity to exactly cancel that of the parent molecule, and it remains stationary in the lab frame. A trap is formed at the null point between two opposing neodymium permanent magnets. Dissociation of molecules at the field minimum results in the slowest fraction of photofragments remaining trapped. After the ballistic escape of the fastest atoms, the trapped slow atoms are lost only by elastic collisions with the chamber background gas. The measured loss rate is consistent with estimates of the total cross section for only those collisions transferring sufficient kinetic energy to overcome the trapping potential.
Near-threshold photodissociation of Br2 from a supersonic beam produces slow bromine atoms that are trapped in the magnetic-field minimum formed between two opposing permanent magnets. Here we quantify the dominant trap-loss rate due to collisions with two sources of residual gas: the background limited by the vacuum chamber base pressure and the carrier gas during the supersonic gas pulse. The loss rate due to collisions with residual Ar in the background follows pseudo-first-order kinetics and the bimolecular rate coefficient for collisional loss from the trap is determined by measurement of this rate as a function of the background Ar pressure. This rate coefficient is smaller than the total elastic collision rate coefficient, as it only samples those collisions that lead to trap loss, and is determined to be $\ensuremath{\langle}\ensuremath{\nu}\ensuremath{\sigma}\ensuremath{\rangle}=(1.12\ifmmode\pm\else\textpm\fi{}0.09)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}\phantom{\rule{0.28em}{0ex}}{\mathrm{cm}}^{3}\phantom{\rule{0.16em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$. The calculated differential cross section can be used with this value to estimate a trap depth of $293\ifmmode\pm\else\textpm\fi{}24\phantom{\rule{0.28em}{0ex}}\mathrm{mK}$. Carrier-gas collisions occur only during the tail of the supersonic beam pulse. Using the differential cross section verified by the background-gas collision measurements provides an estimate of the peak molecular-beam density of $(3.0\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}{10}^{13}\phantom{\rule{0.28em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$, in good agreement with the prediction of a simple supersonic expansion model. Finally, we estimate the trap-loss rate due to Majorana transitions to be negligible, owing to the relatively large trapped-atom phase-space volume.
This thesis demonstrates the feasibility of producing the first cold source of halogen atoms, using Br atoms as the focus. Br atoms are produced by photodissociation of Br2, and detected by (2+1) REMPI and time-of-flight measurements. Ground- and excited-state Br fragments are formed with a recoil velocity directed along the molecular beam axis. The excess energy from the dissociation laser provides the backscattered Br fragments with sufficient recoil velocity to match and cancel out the average velocity of the molecular beam. The Br fragments which undergo sufficient velocity cancellation remain in the laser detection volume for up to 5 ms. A magnetic trap, composed of two permanent bar magnets with their North poles facing each other, is placed around the detection volume and with an axis perpendicular to the molecular beam and laser axes. The centres of the trap and of the laser interaction volume are overlapped. The magnetic field is linear near the centre of the trap and forms a 3-dimensional well with a depth of 0.22 T, equivalent to a trap depth of U0/kB = 255 mK, with the upper and lower standard error [215,325] mK, for ground-state Br. With this configuration, Br atoms have been detected up to delays of 99 ms, to the next laser pulse, suggesting the possibility of accumulating density over successive molecular beam cycles. The decay of Br atoms from the trap is measured, and a Monte Carlo Markov Chain method is implemented to extract the intensity of the Br signal, which decreases to be on the order of the background noise at delays close to 99 ms. Monte-Carlo simulations demonstrate that the trap loss mechanisms are primarily due to collisions with the molecular beam and background gas, inhibiting the ability to accumulate trap density. These simulations also show that Majorana transitions to higher quantum states are minimal and can be ignored. Experimental measurements confirm that near the peak of the molecular beam, when the strongest signal of Br is observed at long delays, around 60% of initially trapped Br atoms are lost due to molecular beam collisions, and (34 ±3)% due to collisions with the background gas. To minimise molecular beam collisions, a chopper construct is designed to reduce the beam pulse width and is placed between the molecular beam valve and detection volume. The chopper runs from 3,000 rpm to 80,000 rpm, during which the duration of the molecular beam at the detection volume is shortened from 130 μs (measured at the full width at half maximum) to between 80 μs and 13 μs, respectively. However, the chopper significantly reduces the initial Br2 density in the trapping region, and the influence of the chopper construct in reducing molecular beam collisions requires further experimental work. Further work is also necessary to improve the operational components, such as reducing the base pressure in the detection chamber to lower background gas collisions, or using a heavier carrier gas to increase density of initially trapped Br atoms. These improvements can lead us closer toward building density of cold Br atoms in the trap over successive molecular beam cycles, with which a source of cold, dense halogen atoms can be realised.
The production of a translationally cold (T < 1 K) sample of bromine atoms with estimated densities of up to 10(8) cm(-3) using photodissociation is presented. A molecular beam of Br(2) seeded in Kr is photodissociated into Br + Br* fragments, and the velocity distribution of the atomic fragments is determined using (2 + 1) REMPI and velocity map ion imaging. By recording images with varying delay times between the dissociation and probe lasers, we investigate the length of time after dissociation for which atoms remain in the laser focus, and determine the velocity spread of those atoms. By careful selection of the photolysis energy, it is found that a fraction of the atoms can be detected for delay times in excess of 100 μs. These are atoms for which the fragment recoil velocity vector is directly opposed and equal in magnitude to the parent beam velocity leading to a resultant lab frame velocity of approximately zero. The FWHM velocity spreads of detected atoms along the beam axis after 100 μs are less than 5 ms(-1), corresponding to temperatures in the milliKelvin range, opening the possibility that this technique could be utilized as a slow Br atom source.
The use of photodissociation to produce cold, slow molecules from a molecular beam of cold, fast molecules is dubbed “photostop”. The essence of the scheme is thus: a pulsed molecular beam of a precursor molecule AB seeded in a noble carrier gas is crossed by a laser beam. The laser light dissociates AB, producing fragments A and B. These recoil from the dissociation site. The speed of the molecular beam and the wavelength of the laser beam are tuned so that the recoil velocity of those A molecules recoiling opposite to the molecular beam direction cancels out their initial velocity. This leaves a certain amount of A close to stationary in the laboratory frame. The photostop technique was first demonstrated with the production of cold, slow NO radicals by the photodissociation of nitrogen dioxide, both at Durham and in South Korea. The work described in this thesis began as a development of the NO photostop experiment, with an attempt made to magnetically trap NO. Latterly, the photostop project became part of the Millikelvin Molecules in a Quantum Array (MMQA) collaboration, the aim of which is the trapping of ten million cold, polar molecules. To this end, the photostop of SH radicals by the photodissociation of hydrogen disulphide was demonstrated.
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
This thesis describes the development of a relatively novel technique for the gen- eration and subsequent trapping of cold species. Molecules in a pulsed supersonic expansion are photolysed, such that the centre-of-mass velocity vector of one of the fragments is equal in magnitude but opposed in orientation to the lab-frame velocity of the precursor molecule. This technique, known as ‘Photostop’, leaves a fraction of the fragments with a narrow velocity distribution, centered around zero velocity in the lab-frame. They can be shown to have zero velocity by changing the time between photodissociation and ionisation; fragments with a high kinetic energy will leave the ionisation volume prior to interrogation. The underlying velocity distribu- tion is uncovered by using the velocity-map imaging technique, and the temperature of the fragments can be determined.The method was originally optimised for the molecular case. Cold NO has been produced from the dissociation of NO₂ molecules, and a single rotational state has been shown to remain in the ionisation volume 10 μs after dissociation, implying a sample temperature of 1.17 K. Using the optimised experimental conditions de- rived from the velocity cancellation of NO, the atomic case is demonstrated for the dissociation of Br₂ to give zero-velocity Br fragments. The Br atoms are seen for delay times in excess of 100 μs, showing the greater applicability of the method to the atomic case. The temperature of the residual atoms is shown to be in the milliKelvin regime, as determined through detailed Monte Carlo simulation of the motion of the stopped atoms. The possibility of trapping the ultracold Br atoms in a magnetic field is explored, and a quadrupolar trap created between two per- manent bar magnets is demonstrated to confine the atoms spatially, within the ion extraction optics, for delays in excess of 1 ms.The Photostop technique is intended to be a stepping stone on the way to widening the number of chemical species available for study in the ultracold regime. The possibility of improvements to the experiment is considered, in order to increase the efficiency of the experiment such that the number density becomes high enough to be viable as a source of atoms for use in cold chemical reactive studies. The possibility of extending the method so as to be used as a tunable velocity source of atoms is also discussed.