1,576 research outputs found
Interaction of molecular Rydberg states with metal surfaces
No full textThe interaction between high-n Rydberg states of molecular hydrogen and metal surfaces has been investigated for the first time. Rydberg states of hydrogen possessing either 0 or 2 units of rotational angular momentum, defined by the quantum number N+ , and principal quantum numbers in the range n= 17 22 (for the N+= 2 states) and n=41-45 (for the N+= 0 states) are directed at a grazing angle onto a metal surface (gold or aluminium). At a sufficiently close distance ionisation may occur via tunnelling of the Rydberg electron into the vacant metal conduction band. Any ions formed in the vicinity of the metal are extracted by the application of an electric field and information about the distance at which the ions are formed can be inferred from the magnitude of the applied field required for detection. Two novel effects are observed. Firstly, it appears that the rotation of the H2+ core has a significant effect on the ionisation properties of the Rydberg states in a manner akin to rotational autoionisation, such that the rotational energy of the core is given up to the Rydberg electron. Secondly, the surface ionisation profiles do not vary smoothly with applied field suggesting that at certain fields the feasibility of ionisation is either enhanced or reduced. A preliminary discussion of the origin of the structure is presented in terms of the crossings in the Stark map between the N+= 0 and N+= 2 Stark manifolds. The development of a theoretical model, and an associated Fortran program, involving the technique of complex scaling is also reported. The hydrogen molecules are modeled using an atomic hydrogen system which provides a good first approximation to the behaviour of the Rydberg electron for states with n > 5. Energies and linewidths, for states with principal quantum number n= 6 9 interacting with a model surface, are explicitly calculated at a range of surface separations. From this information, predictions of the ionisation behaviour expected for states of higher principal quantum number are presented
Digital ion trap mass spectrometry for cold ion-molecule chemistry
No full textA promising new approach for studying cold ion-molecule chemical reactions is the combination of laser- or sympathetically-cooled trapped ions and slow-moving molecules from a cold molecule source, such as a quadrupole velocity selector or a Stark decelerator. Previous reaction studies using trapped atomic ions and slow molecules from a quadrupole velocity selector were able to reach average collision energies as low as 1 K. However, the guided molecules had an approximately room temperature rotational energy distribution, so the reactions studied were not truly cold. Thus, a new molecular source for producing translationally and rotationally cold molecules utilizing buffer gas cooling and quadrupole velocity selection was constructed by K. Twyman and characterized for use in cold reaction studies. This new source of cold molecules is referred to as the buffer gas guide. A new ion trap has been designed and built for use with the existing buffer gas guide. The new ion trap apparatus is compact and mechanically compatible with this new guide. It uses a linear Paul ion trap with cylindrical electrodes to trap ions. Two optical axes (one axial and one radial) enable efficient cooling of small ion crystals. A field-free time-of-flight tube and ion detection assembly are also incorporated into the apparatus. A new technique for determining the mass and quantity of trapped ions has also been developed, termed digital ion trap mass spectrometry. The new technique uses a digital RF waveform to trap ions before ejecting the ions radially from the trap using an ejection pulse applied to the trap electrodes. The ions are then detected after free flight along a time-of-flight tube. This technique was characterized by ejecting crystals of various sizes and compositions: Ca+ only, Ca+/CaF +, Ca+/CaOH +/CaOD+, and Ca+/NH +3 /NH +4 /H3O+. A linear relationship between the number of ions ejected (determined by comparing experimental and simulated crystal images) and the integral of the time-of-flight peak was observed for Ca+ and Ca+/CaF +. All mass peaks were resolved. Simulations of the trapped ions and their trajectories through the time-of-flight tube were also performed, and excellent agreement between the simulated and experimental mass resolution was observed. Progress towards combining the buffer gas guide with the previously independent ion trap is also presented. It is anticipated that the combined buffer gas guide ion trap apparatus will enable the study of ion-molecule reactions at low temperatures with translationally and rotationally cold molecules. It is anticipated that the new digital ion trap mass spectrometry technique will simplify the study of reactions when multiple product ions whose masses are separated by only 1 AMU are formed. A new ion trap has been designed and built for use with the existing buffer gas guide. The new ion trap apparatus is compact and mechanically compatible with this new guide. It uses a linear Paul ion trap with cylindrical electrodes to trap ions. Two optical axes (one axial and one radial) enable efficient cooling of small ion crystals. A field-free time-of-flight tube and ion detection assembly are also incorporated into the apparatus. A new technique for determining the mass and quantity of trapped ions has also been developed, termed digital ion trap mass spectrometry. The new technique uses a digital RF waveform to trap ions before ejecting the ions radially from the trap using an ejection pulse applied to the trap electrodes. The ions are then detected after free flight along a time-of-flight tube. This technique was characterized by ejecting crystals of various sizes and compositions: Ca+ only, Ca+/CaF+, Ca+/CaOH+/CaOD+, and Ca+/NH+3/NH+4/H3O+. A linear relationship between the number of ions ejected (determined by comparing experimental and simulated crystal images) and the integral of the time-of-flight peak was observed for Ca+ and Ca+/CaF+. All mass peaks were resolved. Simulations of the trapped ions and their trajectories through the time-of-flight tube were also performed, and excellent agreement between the simulated and experimental mass resolution was observed. Progress towards combining the buffer gas guide with the previously independent ion trap is also presented. It is anticipated that the combined buffer gas guide ion trap apparatus will enable the study of ion-molecule reactions at low temperatures with translationally and rotationally cold molecules. It is anticipated that the new digital ion trap mass spectrometry technique will simplify the study of reactions when multiple product ions whose masses are separated by only 1 AMU are formed
Electrostatic extraction of buffer-gas-cooled beams for studying ion-molecule chemistry at low temperatures
No full textThis thesis describes the design, construction, operation, and characterisation of an experimental apparatus that produces a source of internally cold, slow molecules that can be used for studying ion-molecule reactions at low temperatures. The apparatus combines buffer-gas cooling with a bent quadrupole velocity selector to cool both the translational and rotational degrees of freedom of the molecules. A cold cell (6 K) is filled with a buffer gas, such as helium, that exhibits sufficiently high vapour pressure for cryogenic applications. Hot molecules (150 to 300 K) enter the cell and thermalise with the buffer gas through collisions. Molecules are subsequently loaded into an electrostatic quadrupole guide, which acts as a velocity filter; only translationally cold polar molecules are guided around the bend. Using a buffer-gas-cooled source of molecules for electrostatic velocity selection, rather than a 300 K effusive source, yields a rotationally cold sample, with J ≤ 3. This rotational selectivity will enable the dependence of reaction cross sections on the reactant rotational state to be examined. Mass spectrometry is used to characterise cold molecular beams of ND3 and CH3F, while (2+1) REMPI spectra are recorded for the ammonia isotopologues. The peak velocity of guided ND3 is 75.86(0.70) ms-1 for standard conditions in a 6 K helium buffer gas cell (1.0 sccm ND3 flow rate, 0.6 mbar helium inlet pressure, ± 5 kV voltage). This corresponds to a peak kinetic energy of 6.92(0.13) K. (2+1) REMPI spectroscopy of the B1E''(v2'=5) ← X(1) transition enabled the rotational state distribution of guided ammonia molecules to be established. PGOPHER simulations of the experimental spectra suggest a rotational temperature of 10 K for ND3 molecules (from a 6 K helium buffer gas cell). The extent of translational and rotational cooling can be controlled by varying the molecular and buffer gas densities within the cell, by changing the temperature of the buffer gas cell (we can operate at 6 K or 17 K), or by changing the buffer gas. The translational temperature of guided ND3 is similar in a 6 K helium and 17 K neon buffer gas cell (peak kinetic energies of 6.92(0.13) K and 5.90(0.01) K, respectively) because the heavier neon gas has a slightly lower thermal velocity at 17 K than helium does at 6 K. Despite similar translational temperatures, the rotational temperature of guided ND3 is lower for molecules exiting the 6 K helium cell compared to the 17 K neon buffer gas cell (10 K and 15 K, respectively). The 6 K helium and 17 K neon buffer gas cells provide an excellent opportunity to investigate the effect of rotational cooling on branching ratios and reaction rates in low temperature ion-molecule reactions. The buffer gas cell and velocity guide described in this work will be combined with a linear Paul ion trap, to facilitate the study of cold ion-molecule reactions
Evaluating Citebase, an open access Web-based citation-ranked search and impact discovery service
No full textCitebase is a new citation-ranked search and impact discovery service that measures citations of scholarly research papers which are openly accessible on the Web, i.e. papers that are assessable continuously online. Other services, such as ResearchIndex, have emerged in recent years to offer citation indexing of Web research papers. In the first detailed user evaluation of an open access Web citation indexing service, Citebase has been evaluated by nearly 200 users from different backgrounds. The paper details the procedures used in the evaluation, and analyses the results of this study, which took place between June and October 2002. It was found that within the scope of its primary components, the search interface and services available from its rich bibliographic records, Citebase can be used simply and reliably for the purpose intended, and that it compares favourably with other bibliographic services. It is shown tasks can be accomplished efficiently with Citebase regardless of the background of the user. More data need to be collected and the process refined before it is as reliable for measuring citation impact of indexed papers. Better explanations and guidance are required for first-time users. Coverage is seen as a limiting factor, even though Citebase indexes over 200,000 papers from arXiv. Non-physicists were frustrated at the lack of papers from other sciences. The principle of citation searching of open access archives has thus been demonstrated and need not be restricted to current users. Since the evaluation, Citebase has become a featured service of the ArXiv physics eprint archives
Cold reactive collisions between neutral molecules and trapped ions
No full textThis thesis describes the development and demonstration of techniques for the study of
ion-neutral reactive collisions at low temperatures conducted using two unique experimental
apparatuses comprising radio-frequency Paul traps. One apparatus combines
a Stark decelerator with a Paul trap; the other apparatus features a buffer gas cell
interfaced with a Paul trap through an electrostatic quadrupole guide.
A novel ion trap time-of-flight mass spectrometer has been introduced and characterised.
This apparatus is designed to detect the ion products of reactive collisions
at low temperatures (< 10 K). This detection approach affords excellent detection
efficiency and is broadly applicable to all ion-molecule reactions that one could study
within a linear Paul ion trap. A proof-of-principle reaction between xenon ions and
neutral ammonia isotopologues is examined to test the performance of the new detection
set-up.
With the goal of achieving full control over the reaction parameters, the amount of
alignment retained by rotationally and translationally cold ammonia molecules exiting
the electrostatic guide has been examined using (2 + 1) REMPI detection of the
molecules with varying linear polarisation. Simulations suggests how modifications
to the current setup will enable full orientation of the cooled molecules reaching the
detection region to be achieved.
Experiments on cold charge exchange reactions between sympathetically-cooled Xe+
and room temperature ammonia (NH3 and ND3) have been conducted within lasercooled
Ca+ Coulomb crystals in a linear Paul ion trap. There is ongoing work to
ascertain any difference in reactivity between NH3 and ND3 as the neutral reactant
species. Preliminary data are discussed at a qualitative level, with the prospect of
observing any isotope effect in this charge transfer process. Charge exchange reaction
experiments using cold state-selected ammonia are discussed with the goal of
establishing reaction rate constants at different collision energies.</p
Author Talk
No full textUniversity president, Jim Schmotter, introduces Tim O'Brien at the author talk in Ives Auditorium, October 26, 2010.</p
Who Belongs? Immigrants, Refugees, Migrants, and Actions Towards Justice: A Conversation With Tim Wise
No full textTim Wise is an antiracist activist, essayist and author of seven books on racism, inequality and white privilege. He is among the most prominent anti-racist writers and educators in the United States. Over the past 25 years he has engaged audiences in all 50 states, at over 1000 college and high school campuses, at hundreds of professional and academic conferences, and to community groups across the country. While visiting Iowa State University Tim Wise interviewed with us to discuss Who Belongs? by providing a brief historical perspective of immigration, the current political climate, and the role of activism.</p
Ejection of Coulomb crystals from a linear Paul ion trap for ion-molecule reaction studies - metadata
No full textMetadata to accompany the JPC A publication
Accepting Optimally in Automated Negotiation with Incomplete Information (abstract)
No full textIntelligent SystemsElectrical Engineering, Mathematics and Computer Scienc
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