This thesis presents numerical optimization of geometries of axially symmetric ion trap mass analyzers. The motivation for this thesis is two fold. First is to demonstrate how the automated scheme can be applied to achieve geometry parameters of axially symmetric ion traps for a desired field configuration. Second is, through the Geometries investigated in this thesis, to present practically achievable geometries for mass spectroscopists to use. Here the underlying thought has been to keep the design simple for ease of fabrication (with the possibility of miniaturization) and still ensure that the performance of these analyzers is similar to the stretched geometry Paul traps. Five geometries have been taken up for investigation: one is the well known Cylindrical ion trap (CIT), three are new geometries and the last is the Paul trap under development in our laboratory. Two of these newer geometries have a step in the region of the midline of the cylindrical ring electrode (SRIT) and the third geometry has a step in its endcap electrodes (SEIT). The optimization has been carried out around deferent objective functions composed of the desired weights of higher order multiples. The Nelder-Mead simplex method has been used to optimize trap geometries. The multipoles included in the computations are quadrupole, octopole, dodecapole, hexadecapole,ikosipole and tetraikosipole having weights A2, A4, A6, A8, A10 and A12, respectively.Poincare sections have been used to understand dynamics of ions in the traps investigated. For the CIT, it has been shown that by changing the aspect ratio of the trap the harmful ejects of negative dodecapole superposition can be eliminated, although this results in a large positive A4=A2 ratio. Improved performance of the optimized CIT is suggested by the ion dynamics as seen in Poincare sections close to the stability boundary. With respect to the SRIT, two variants have been investigated. In the first geometry, A4=A2 and A6=A2 have been optimized and in the second A4=A2, A6=A2 and A8=A2 have been optimized; in both cases, these ratios have been kept close to their values reported for stretched hyperboloid geometry Paul traps. In doing this, however, it was seen that the weights of still higher order multipole not included in the objective function, A10=A2 and A12=A2, are high; additionally, A10=A2 has a negative sign. In spite of this, for both these configurations, the Poincare sections predict good performance. In the case of the SEIT, a geometry was obtained for which A4=A2 and A6=A2 are close to their values in the stretched geometry Paul trap and the higher even multipole (A8=A2, A10=A2 and A12=A2) are all positive and small in magnitude. The Poincare sections predict good performance for this con¯guration too. Direct numerical simulations of coupled nonlinear axial/radial dynamics also predict good performance for the SEIT, which seems to be the most promising among the geometries proposed here. Finally, for the Paul trap under development in our laboratory, Poincare sections and numerical simulations of coupled ion dynamics suggest a stretch of 79:7% is the best choice.

Laser beams with precisely controlled intensity profiles are essential for many areas. We developed a beam shaping system based on the digital micromirror device (DMD) for ultra-cold atom experiments and other potential applications. The binary DMD pattern was first designed by the error diffusion algorithm based on an accurate measurement of the quasi-Gaussian incident beam from a real-world laser. The DMD pattern was projected to the image plane by a bandwidth-limited 4f telescope that converted this pattern to the grayscale image. The system bandwidth determined the theoretical limit of image precision by the digitization error. In addition, it controlled the spatial shape of the point spread function (PSF) that reflected the tradeoff between image precision and spatial resolution. PSF was used as a non-orthogonal basis set for iterative pattern refinement to seek the best possible system performance. This feedback process, along with stable performance of DMD, the blue-noise spectrum of the error diffusion algorithm, and low-pass filtering, guaranteed high-precision beam shaping performance. This system was used to produce various beam profiles for different spatial frequency spectra. First, we demonstrated high-precision slowly-varying intensity beam profiles with an unprecedented high intensity accuracy. For flattop and linearly-tilted flattop beams, we achieved 0.20-0.34% root-mean-square (RMS) error over the entire measurement region. Second, two-dimensional sinusoidal-flattop beams were used to evaluate image precision versus system bandwidth. System evaluation confirmed that this system was capable of producing any spatial pattern with <3% RMS error for the most system bandwidth. This experiment extended the beam shaping to any system bandwidth and provided a reference to estimate the output image quality based on its spatial spectrum. Later experiment using a Lena-flattop beam profile demonstrated the arbitrary beam profile generation. We implemented this system for applications on the homogenous optical lattice and dynamic optical trap generation. The DMD pattern was optimized by the iterative refinement process at the image feedback arm, and projected through a two-stage imaging system to form the desired beam profile at the working plane. Experiments demonstrated a high-precision beam shaping as well as a fast and dynamic control of the generated beam profile. / text

Solid phase extraction is one of the most widely used techniques to trap and release compounds in a solution. A hydrophobic substance will stick efficiently to a hydrophobic surface (the “like dissolves like” principle). With an introduced response (i.e. pH change), a responsive surface can change from hydrophobic to hydrophilic, weakening the hydrophobic substance’s attraction and thus facilitate in an easy removal. A surface has been prepared having a terminal anthranilic acid (AA) moiety on silica gel particles, microscope slides, and TLC plates in three steps. First, a vinyl group was attached to the surface. Then, this vinyl group was reacted to form a surface carboxylic acid group. Finally, the carboxylic acid group was converted to an amide group that linked to the silica surface. FT-IR, and elemental analysis were used to confirm each step of the synthesis. At low pHs the –COOH group on the AA moiety is neutral and intrahydrogen bonding keeps this moiety’s phenyl (hydrophobic) portion exposed to the surface. The effect has been investigated by measuring contact angles at various pH values. At higher pHs the AA’s carboxylic acid group becomes the charged carboxylate, rendering the surface hydrophilic. Substances can be trapped and released using this unique switching approach. 2-naphthol, for example, is hydrophobic and thus was trapped at lower pHs (pH 4) (hydrophobic surface) and released at higher pHs (pH 10) (hydrophilic surface) on this responsive surface

<p>The trapped atomic ion qubits feature desirable properties for use in a quantum computer such as long coherence times, high qubit readout fidelity, and universal logic gates. While these essential properties have been demonstrated, the ability to scale a trapped ion quantum system has not yet been shown. The challenge of scaling the system calls for methods to realize high-fidelity logic gates in scalable trap structures. Surface electrode ion traps, that are microfabricated from a silicon substrate, provide a scalable platform for trapping ion qubits only if high-fidelity operations are achievable in these structures. Here, we present a system for trapping and manipulating ions in a scalable surface trap. Trapping times exceeding 20 minutes without laser cooling, and heating rates as low as 0.8 quanta/ms indicate stable trapping conditions in these microtraps. Coherence times of more than one second verify adequate qubit and control field stability. We demonstrate low-error single-qubit gates performed using stimulated Raman transitions driven by lasers that are tightly focused on the ion qubit. Digital feedback loops are implemented to control the driving field's amplitude and frequency. Gate errors are measured using a randomized benchmarking protocol for single qubit gates, where residual amplitude error in the control beam is compensated using various pulse sequence techniques. Using pulse compensation, we demonstrate single qubit gates with an average error per randomized Clifford group gate of $3.6(3)\times10^{-4}$, which is below the fault-tolerant threshold for some error-correction schemes.</p> / Dissertation

No description available.

No description available.

Introduction Recently in our laboratory we needed a reliable and relatively simple source of aqueous solutions of [11C]CO2. We examined various methods of trapping [11C]CO2 gas both in solution and on ion exchange resins, followed by elution into aqueous phase. We favor simple methods that have high trapping and elution efficiencies and produce a highly concentrated solution. Furthermore, we desired methods that would minimize the use of hazardous reagents and materials with respect to both handling and disposal. We also considered the formulation of the final solution in terms of chemical compatibility with contacted materials, working with the assumption that dilute bicarbonate or carbonate solutions will have little reactivity with many materials. In a phantom, compatibility with materials (i.e. plastics, glues, metals, etc.) is important (1-4), while in (bio)geochemical studies – where transport of carbon is important – the chemical form of the radiolabelled molecule is important, but compatibility must be determined on a case-by-case basis (5-7). Small medical cyclotrons can easily produce carbon-11 as gaseous [11C]CO2, and various methods are utilized to incorporate carbon-11 into solution, often with unfavorable resource requirements, costs, or chemical properties. Commonly [11C]CO2 gas is bubbled through a strong base, forming the carbonate anion; but neutralizing a strong base (as to avoid special handling or disposal requirements) requires a large volume of diluent or buffer; or a very precise addition of acid – which if done improperly – may lead to an acidic pH and subsequent loss of [11C]CO2 from solution (8,9). Alternatively, [11C]CO2 (or [11C]CH4) can be converted to [11C]CH3I at high-yield, but requires specialized, expensive radio-synthesis equipment (10-12). [11C]CH3I can then be trapped in DMSO (albeit providing a volatile and hazardous solution) or used as a synthon en route to water soluble compounds such as [11C]choline (13). Finally, leftover radiolabelled radiopharmaceuticals from a carbon-11 imaging experiment could be used, but chemical compatibility (i.e. lipophilicity) of the radiolabelled compound may be of concern. Carbon dioxide gas will dissolve with a solubility of 1.5 g/L at STP (9) and slowly react with water to generate carbonic acid (H2CO3), a weak acid. Passing [11C]CO2 through a base-activated ion exchange cartridge, the [11C]CO2 reacts with hydroxide ions to form [11C]carbonate which is bound to the resin due to its higher selectivity for carbonate than hydroxide (14). Elution with excess bicarbonate displaces [11C]carbonate and neutralizes any remaining hydroxide, providing a 11C aqueous solution that is mildly basic, chemically non-hazardous, and very concentrated. Material and Methods [11C]CO2 gas trapping efficiency was evaluated for solutions and base-activated ion exchange resins. The gas was delivered either rapidly in a high-flow bolus directly from the cyclotron target or slowly in a low-flow helium stream during heating of a carbosieves column. Elution efficiency of ion exchange cartridges were evaluated for both fraction of trapped activity eluted and volume of solution needed for elution. [11C]CO2 was produced via the 14N(p,α)11C reaction on a CTI RDS111 – 11 MeV cyclotron at the Lawrence Berkeley National Laboratory’s Bio-medical Isotope Facility. The 7 mL target is pressurized to 315 psi with 1% O2/N2 gas, equating to 150 mL gas at STP. For direct-from-target trapping experiments, the target was decompressed and routed to the cartridge via 50 feet of 0.020” I.D. tubing until the target falls to atmospheric pressure (~55 seconds) providing an inhomogeneous flow – a short rapid burst of flow followed by a longer low-flow bleed. For helium-eluted experiments, the [11C]CO2 was unloaded from the cyclotron target and trapped on a room-temperature carbosieves column (15). Target gases were subsequently flushed from the column for 30 seconds with helium at 50 mL/min. After heating the column to 125 °C without gas flow, [11C]CO2 was eluted off the column in helium at 15 mL/min. [11C]CO2/He was bubbled through 9 aqueous and 2 organic solutions to test for trapping efficiency in a slow, steady helium stream at 15 mL/min (sodium hydroxide (0.96M, 0.096M, 0.0096M), sodium bicarbonate (1.14M, 0.57M, 0.057M), sodium carbonate (2.0M, 1.0M, 0.10M), ethanol, and DMSO (2mL ea.). An Ascarite-filled cartridge was attached to trap any untrapped [11C]CO2. Measures of radioactivity were made using a Capintec CRC-15R dose calibrator. Trapping efficiency for solutions is calculated as the fraction of radioactivity captured in solution relative to the sum of the solution and the Ascarite trap. Three different commercially available, ion ex-change cartridges were evaluated for trapping and elution efficiencies. FIGURE 1 shows a photo-graphic comparison of the physical size and shapes of the cartridges as well as a X-ray computed tomography (CT) cross sectional view of the internal ion exchange resin volume and dead volume of the cartridges. All cartridges were activated with 1 mL of 1 N aqueous NaOH followed by passing 10 mL deionized water then 10 mL of air through the cartridge. In both direct-from-target (n = 4) and helium-stream experiments (n = 3 or 4), cartridges were connected to [11C]CO2 delivery lines via Luer connections. The gas exiting the cartridge passed through an empty 3 mL crimp-top vial as a liquid trap en route to an Ascarite trap on the vent needle as described above. Trapping efficiency for cartridges is calculated as the fraction of radioactivity captured on the cartridge relative to the sum of the cartridge, the empty vial, and the Ascarite trap. Cartridges were eluted with 0.5 mL of saturated sodium bicarbonate solution (1.14 M @ 20°C) followed by 9.5 mL water and 10 mL air. Elution efficiency is calculated as the fraction of radioactivity eluted in 10 mL relative to the sum of the spent cartridge following elution and the 10 mL eluate (Equation 5). The pH of the eluate was measured using 0-14 pH test strips. Results and Conclusion The trapping of [11C]CO2 in all solutions was less than 70% of the total radioactivity with the exception of the 0.96 M and 0.096 M NaOH. With a higher concentration of base driving equilibrium towards carbonate stability, it could be expected that the most basic solution had the best trapping efficiency, but this attribute also means it is least desirable solution to work with from a hazardous material or chemical compatibility perspective. When [11C]CO2 was delivered in a helium stream, all three cartridges performed at near 100% efficiency, as shown in FIGURE 4. With higher flow, direct-from-target delivery, the cartridges trapped [11C]CO2 with a wider range of efficiencies: ICOH (99 ± 1 %), ORTG (90 ± 2 %), and QMA (79 ± 4 %). Elution resulted in > 99 % release of carbon-11 activity for both QMA and ORTG cartridges, but only 39 ± 3 % release from the ICOH cartridge. Elution efficiency of the trapped radioactivity (Equation 5) was independent of the method of [11C]CO2 delivery. Across all cartridges and delivery methods, the eluate was at about pH = 10. We recommend that the ORTG cartridge be used for trapping of [11C]CO2 gas with elution by > 300 µL of saturated bicarbonate solution. This recommendation is based on the better trapping for ORTG cartridges compared to the QMA cartridges in the direct-from-target [11C]CO2 delivery method and the smaller volume needed for elution of all trapped carbon. This method excels based on its simplicity, adaptability to automation, low-cost ($5/cartridge), and observations that a single ORTG cartridge suffers no loss of performance after multiple uses. A potential disadvantage to this method is that it involves using a carbon-containing eluent, which means that this method cannot be used for imaging experiments that require high specific activity. However, considering the eluate is a mildly basic aqueous solution, we expect that it will be compatible with a wide variety of materials and experimental applications.

The Canadian Penning Trap (CPT) mass spectrometer at the Argonne National Laboratory makes precise mass measurements of both stable and unstable nuclides. To date, more than 60 radioactive isotopes having half-lives as short as one second have been measured with the CPT with a mass precision approaching 10 ppb. This thesis will present measurements made of nuclides along the rp-process path, which describes a process resulting from a series of rapid proton-capture reactions in an astrophysical environment. One possible site for the rp-process mechanism is an x-ray burst which results from the rapid accretion of hydrogen and helium from one star onto the surface of its neutron star binary companion. Mass measurements are required as key inputs to network calculations used to describe the rp-process in terms of the abundances of the nuclides produced, the light-curve profile of the x-ray bursts, and the energy produced. This thesis will describe the CPT apparatus, explain the method used to make precise mass measurements, and present the masses of the "waiting-point" nuclides ⁶⁸Se and ⁶⁴Ge. The mass measurement results, when used in x-ray burst models, confirm both ⁶⁸Se and ⁶⁴Ge as waiting-point nuclides which delay the rp-process by approximately 30 s and 7 s respectively.

Needle trap device (NTD) is a technique that is useful for a wide variety of applications involving the sample preparation of compounds with a wide range of chemico-physico properties, and varying volatilities. A newly designed NTD that improves the performance relative to previous NTD designs is simple to produce is developed. The NTD utilizes a side-hole needle with a modified tip to improve the sealing between the NTD and narrow neck liner of the GC injector, thereby increasing the desorption efficiency. The slurry packing method was applied, evaluated, and NTDs prepared by this method were compared to NTDs prepared using the vacuum aspiration method. NTD geometries including blunt tip with a side-hole needle, tapered tip with side-hole needle, dome tapered tip with side-hole, sliding tip with side-hole and blunt tip with no side-hole needle (expanded desorptive flow) were prepared and evaluated. Sampling performance and desorption efficiency were investigated using automated headspace extraction of benzene, toluene, ethylbenzene, p¬-xylene (BTEX), anthracene and pyrene. The tapered tip and sliding tip NTDs were found to have increased desorption efficiency. SPME and NTDs are valuable sample preparation tools for on-site analysis. Combining both extraction techniques allows for the differentiation of free and particle-bound compounds in a sample matrix. Portable GC/MS instrumentation can achieve fast separation, identification, and quantitation of samples prepared by the above techniques on-site without the need for transport to the laboratory. This minimizes the effects of volatiles lost and sample degradation during storage time. Here, SPME and tapered tip NTDs combined with portable GC/MS are used to investigate free and total emissions of BTEX and select PAHs from gasoline and diesel exhaust. Using the above optimized technologies, cigarette smoke in a smoking area where people were actively smoking and inside a smoker’s car were also investigated. Target contaminants were found in the investigated matrices at ng/mL levels.

The Canadian Penning Trap (CPT) mass spectrometer at the Argonne National Laboratory makes precise mass measurements of both stable and unstable nuclides. To date, more than 60 radioactive isotopes having half-lives as short as one second have been measured with the CPT with a mass precision approaching 10 ppb. This thesis will present measurements made of nuclides along the rp-process path, which describes a process resulting from a series of rapid proton-capture reactions in an astrophysical environment. One possible site for the rp-process mechanism is an x-ray burst which results from the rapid accretion of hydrogen and helium from one star onto the surface of its neutron star binary companion. Mass measurements are required as key inputs to network calculations used to describe the rp-process in terms of the abundances of the nuclides produced, the light-curve profile of the x-ray bursts, and the energy produced. This thesis will describe the CPT apparatus, explain the method used to make precise mass measurements, and present the masses of the "waiting-point" nuclides ⁶⁸Se and ⁶⁴Ge. The mass measurement results, when used in x-ray burst models, confirm both ⁶⁸Se and ⁶⁴Ge as waiting-point nuclides which delay the rp-process by approximately 30 s and 7 s respectively.