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Creating a source for cold, magnetically-trapped bromine atoms

Jessica Lam

Published Jan 1, 2015• 0 citations
Publisher

Abstract

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.

DOI
10.5287/ora-mvqpekvep

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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.
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.
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.
Near-threshold photodissociation of Br2{\mathrm{Br}}_{2}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.
Successful magnetic trapping of both SH at a density of 2.4 x 10^5 cm^-3 and atomic oxygen at a density of 3000 +/- 900 cm^-3 has been demonstrated with respective trapping lifetimes of 40 +/- 10 ms and 82 +/- 3 ms inside a 0.41 T deep, anti-Helmholtz configuration magnetic trap. To achieve trapping of these species, a stable precursor was cooled by supersonic expansion in a molecular beam and photodissociated in such a way as to match and oppose a photofragments recoil speed to the precursors molecular beam speed. This process is called photostop. Velocity-map images have been taken of photostop of atomic oxygen from photodissociation of NO2 in a molecular beam. They show that atomic oxygen can be photostopped from a variety of NO photodissociation co-fragments with a suitably broad molecular-beam velocity-distribution. Although photostop is simple and cheap to use, the trapping lifetimes and densities that have been achieved in this thesis are not competitive compared to other methods of trapping similar molecular species. The main problem that presents universally in photostop experiments is due to the large number of fast molecules from the supersonic expansion that pass through the trap after the photostop event. Only a small fraction of the molecules in the molecular beam are stopped and the remaining ones cause significant trap loss through high energy elastic collisions with trapped species. Work has been carried out to develop the cavity-enhanced laser-induced-fluorescence (CELIF) technique to be used more widely in the cold molecules field. The technique was employed unsuccessfully to measure photostopped SH radicals but was used elsewhere to measure cold SD radicals after Stark deceleration. In addition, the technique has been initially developed for use inside magnetic traps. Clusters of NO.Ar(n) have been studied using [1+1'] REMPI to assess the viability of a new soft-ionisation technique for molecular clusters of atmospheric interest. This work did not show conclusive evidence that [1+1'] REMPI would reduce cluster fragmentation and displayed some interesting but poorly understood data.
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